Strong and Transparent Deacetylated Chitin Nanofibril Films using Bees’ Honey and Carrageenan as Potential Plasticizers in Packaging

Strong and Transparent Deacetylated Chitin Nanofibril Films using Bees’ Honey and Carrageenan as Potential Plasticizers in Packaging | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Strong and Transparent Deacetylated Chitin Nanofibril Films using Bees’ Honey and Carrageenan as Potential Plasticizers in Packaging Ngesa Ezekiel Mushi, Cosmas Fednand Kindole, Neema Msuya This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6343422/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Honey from bees and carrageenan from red seaweeds may act as alternative plasticizers to commercial glycerol in improving the mechanical flexibility of deacetylated chitin nanofibril (DeChNF) films. Free-standing films with plasticizer content up to 65% were produced using a casting technique. Transparency, thermal relaxation, tensile properties, water absorption capacity, and water vapor permeability of the films were evaluated as essential properties in packaging. Firstly, the deacetylated ChNF film had a transmittance of 84.9% at 800 nm, with films containing 20 wt% plasticizers displaying transmittance values of 87.8% (glycerol), 83.6% (honey), and 85.4% (carrageenan). Secondly, Differential Scanning Calorimetry (DSC) indicated relaxation temperatures between 40–80ºC and 300–370ºC towards lower values with the plasticizer content. A more profound plasticization effect appears to be associated with honey, followed by glycerol, and finally, carrageenan. Thirdly, mechanical testing revealed a decrease in tensile strength from 41.3 MPa for pure DeChNF to 6.3 MPa (glycerol), 4.3 MPa (honey), and 9.4 MPa (carrageenan). Tensile strain increased from 8.5% for DeChNF to 24.74% (glycerol), 31.5% (honey), and 21.65% (carrageenan). Fourthly, water absorption capacity and water vapor permeability performance are compared to commercial packaging films. Thus, the data from DeChNF plasticized films with honey and carrageenan are novel and promising for innovative chitin nanofibril applications in packaging. Deacetylated chitin nanofibrils bees' honey carrageenan glycerol films mechanical properties Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Introduction As interest in biopolymers grows, shifting from petroleum-based plastics to renewable and biodegradable polymer materials becomes essential. In 2014, global plastic production was estimated at 311 million tons [ 1 – 2 ], and projections indicate that this figure could quadruple by 2050 [ 2 ], showing the need for sustainable alternatives. Biopolymers offer versatile properties that rival traditional plastics, including excellent mechanical and barrier characteristics [ 3 – 5 ]. In addition, they are abundant and non-toxic, making them an appealing choice for eco-friendly materials [ 1 , 2 ]. Biopolymer films for packaging have been developed from chitosan [ 6 ] gelatin [ 7 ], carboxymethyl cellulose [ 8 ], hydroxypropyl methylcellulose [ 9 ], cellulose acetate [ 10 ], ethyl cellulose [ 11 ], starch [ 12 ], xyloglucan [ 13 , 14 ], and cellulose nanofibrils [ 15 , 16 ]. Unlike cellulose, chitin nanofibril-based films demonstrate novel properties that have not been extensively investigated. Being the second most abundant polysaccharide after cellulose [ 17 ], chitin is a promising resource for sustainable packaging. It is primarily obtained as waste from marine industries and is biosynthesized through the action of chitinase enzymes, with monomers of N-acetyl-D-glucosamine linked by β-1-4 bonds. Individual chitin nanofibrils (ChNFs) can be extracted from invertebrates such as crabs, shrimp, squid pens, lobster shells, insect cuticles, and fungi [ 18 , 19 ]. Approximately 47 million tons of chitin from seafood waste are discarded yearly, with 6–8 million tons either dumped or buried in landfills [ 20 – 22 ]. To fully harness the potential of chitin from waste, it is crucial to control its mechanical properties. Biological ChNFs form strong and tough nanostructured materials with exceptional properties that make them suitable for various applications, including composites, textiles, tissue engineering, biomedicine, and pharmaceuticals [ 23 ]. The unique mechanical characteristics of ChNFs stem from their α-type extended polymer conformation and long-range crystallinity with a swirled morphology, making them remarkably strong and stiff [ 24 ]. Research indicates that ChNFs with a degree of acetylation (DA) of around 70–74% are classified as deacetylated chitin nanofibrils (DeChNF) [ 25 ]. These DeChNFs, considered partially deacetylated, retain their extended chitin crystal core at higher DA levels [ 24 , 25 ]. Films made from DeChNFs are highly transparent and can form stable hydrocolloid networks, enhancing film formation compared to native ChNFs [ 27 ]. The DA significantly correlates to mechanical properties, and lower DA contributes to good tensile strain to failure and antibacterial properties through increased amino-active sites on the surface [ 27 , 28 ]. However, pure DeChNF films can be brittle, fragile, and challenging [ 29 ]. These films may crack easily when dried or folded under ambient conditions due to strong intermolecular hydrogen bonding from capillary condensation, which creates permanent nanofibril bonds during drying. This brittleness limits the broader applicability of DeChNF films, particularly in packaging. Plasticization has been employed to improve the properties of deacetylated ChNF-based films and create flexible, strong, and transparent films [ 29 , 30 ]. The addition of plasticizers disrupts intermolecular forces by sitting in between the polymer chains [ 29 , 30 ]. As a result, it softens the film structure and enhances the mobility of the polymer chains. Glycerol has proven to be an effective plasticizer, increasing the flexibility of chitosan films while being biocompatible [ 29 , 30 ]. It also improves the mechanical properties and reduces the brittleness of native DeChNF films [ 30 ]. In contrast, incorporating chitosan into the ChNF films enhances their toughness and strength, for example, chitosan with a 10 wt. % ChNF loading fraction boosted the tensile strength to 98 MPa, with a tensile strain at failure of 46% and work of fracture at 35 MJ/m³ [ 31 ]. These mechanical data are excellent because of the unique interactions between the small-diameter nanofibrils and chitosan. Chitosan, a deacetylated chitin derivative and cationic polyelectrolyte, stabilizes the hydrocolloid suspension, which is essential for good mechanical properties. On the other hand, glycerol-plasticized ChNF films demonstrate lower mechanical properties, achieving tensile strength of 40 MPa and tensile strain to failure of 18% at a higher ChNF loading fraction of 50 wt. % [ 29 ]. In another study, chitosan enhanced ChNF quality, taking advantage of the compatibility and electrostatic interactions between the chitosan polymer and ChNF [ 32 ]. For example, the combination of ChNFs with a 4 wt.% residual chitosan matrix resulted in an ultimate strength of 187.2 MPa and work of fracture measured at 12.1 MJ/m³, owing to the more favorable failure mechanisms compared to neat ChNF films [ 32 ]. Based on existing literature regarding chitosan and glycerol, controlling the mechanical properties of DeChNF films through plasticization appears promising and could enhance their practical applications. However, limited information is available about DeChNF plasticized wrapping films that utilize food-grade resources for packaging. Moreover, the preparation of chitosan or glycerol utilizes many chemicals that are not environmentally friendly and may be expensive. Honey, known for its unique properties and high biocompatibility, is a promising plasticizer for DeChNF films. It is highly hydrophilic, with a 17–18% moisture content due to its natural composition of sugars, proteins, minerals, and antioxidants [ 33 ]. Honey exhibits anti-inflammatory, antioxidant, and antimicrobial properties, making it an excellent candidate for packaging [ 34 ]. Previous studies reported that DeChNF-honey films prepared through casting demonstrated a tensile strength of 21.32 MPa and a strain failure of 6.5% with 35 wt. % honey [ 30 ]. Though these films exhibited good flexibility for wrapping and tomatoes coated with DeChNF-honey maintained quality for up to 20 days, there is no detailed understanding of the effect of honey on the properties, including mechanical, of the DeChNF films. Carrageenan, a natural polysaccharide extracted from edible red seaweed, also shows potential as a plasticizer for DeChNF films. It comprises a sulfated galactan backbone alternating 3-linked and 4-linked D-galactopyranose units [ 35 , 36 ]. Carrageenan is an abundant and renewable biopolymer with excellent gelling, stabilizing, plasticizing, antimicrobial, and film-forming properties [ 37 – 40 ]. Despite its unique characteristics, little is known about its effectiveness as a plasticizer for DeChNF films. While the literature on using natural honey or carrageenan as plasticizing agents to modify the mechanical properties of DeChNF films is sparse, previous research suggests that honey-plasticized DeChNF films can extend the postharvest shelf life of tomatoes more effectively than unmodified DeChNF films, which is attractive in packaging [ 30 ]. The flexibility of films containing 35% honey allowed for multiple wrapping and unwrapping of tomatoes over a 20-day storage period. Furthermore, prior studies have indicated that the toughness and strength of DeChNF films could be enhanced by incorporating glycerol as a plasticizer [ 29 ] or by blending with chitosan [ 32 ]. However, the effects of plasticization using these food-sourced materials have not been thoroughly investigated. The current study explores using carrageenan and honey from food-grade resources as plasticizers. In addition to reviewing published literature, the study compares their effectiveness with glycerol in reducing the mechanical brittleness of DeChNF films. The primary objective is to improve our understanding of the mechanical potential of DeChNF films as novel nanomaterials. Ultimately, this research aims to contribute to developing fully biodegradable and eco-friendly films, offering alternatives to petroleum-based polymer materials for postharvest food technologies. Experimental Materials DeChNF was prepared from crab shell wastes ( Portunus Pelagius ) purchased from the Kigamboni fish market in Dar es Salaam, Tanzania. The edible red seaweed for carrageenan extraction was purchased from local producers in Zanzibar. The DA of DeChNF was 68.2%. Glycerol was purchased from Loba Chemie Ltd in India and used as received. Matured bees (non-stingless) honey harvested from Apis Mellifera Scutellata in the Kigosi-Moyowosi game reserve was purchased from local vendors in Dar es Salaam. The chemicals, such as hydrochloric acid, sodium hydroxide, ethanol, and acetic acid, were purchased from Loba Chemie PVT LTD in India. DeChNF and carrageenan preparation Following the method described by Mushi et al. [ 41 ], the raw crushed crab shells were treated with 2 M of HCl for demineralization at room temperature. Then, the shells were washed with deionized water to a neutral pH. The sample was decolorized by treating it with ethanol under constant stirring overnight. Next, the deproteinization was done based on the method developed by Fan et al. [ 25 ], with a few modifications. First, the samples were deproteinized and deacetylated by treatment with 33% NaOH at 100 ℃ for 4 h. Then, the sample was washed several times with deionized water until it reached a neutral pH. The deacetylated chitin was dispersed in aqueous acetic acid (pH 3–4) and stirred overnight for mechanical disintegration. The sample was then passed through a kitchen blender (Vitamix, USA) at 1500 rpm and repeated thrice. The degree of deacetylation of the thus obtained DeChNFs was 32.8%. Carrageenan extraction was performed as previously described by Dong et al. [ 42 ] with slight modifications. Essentially, 100 g of wet red seaweed sample was weighed and soaked in distilled water (2L) for 1 hr. at 80°C using a hot plate magnetic stirrer to remove the skin pigment on the surface. Then, seaweed biomass was washed with distilled water and collected. The obtained samples were refluxed in 8% NaOH solution (27 mL of NaOH per gram of seaweed biomass) and shaken (500 rpm) at 80°C for 2 h using a magnetic stirrer. After cooling, the solution was stored in a non-dried state for further use. Preparation of DeChNF plasticized films The plasticized DeChNF film was prepared from the DeChNF, carrageenan gel, and bee honey shown in Fig. 1 a. The preparation procedures are described in Fig. 1 b. Initially, 1 wt. % aqueous dispersion of DeChNF was prepared. Next, different plasticizers were added into the dispersions at 0, 5, 20, 35, and 65 wt—%, as described in Table 1 , based on the dry weight of DeChNF. The film-forming solutions were blended in the kitchen blender (Vitamix 5200, USA) for 2 min and treated with a super stirrer (MX-S401 S, China) to mix homogeneously for 1 hour at room temperature. After one hour, the mixtures were degassed to remove air from bubbles for 30 minutes before casting in glass Petri dishes. The mixtures were poured into glass Petri dishes coated with a release agent and dried in ambient conditions (50°C, 24 hours) to allow evaporation. All films were prepared in triplicate, including films without plasticizers used as controls. After 24 h of drying, films were peeled from the casting surfaces and stored in desiccators with 53 ± 1% relative humidity (RH). Table 1 Formulation of plasticizer in the preparation of plasticized DeChNF film Sample Plasticizer type Plasticizer concentration (%) DeChNF - 0 G5 Glycerol 5 G20 Glycerol 20 G35 Glycerol 35 G65 Glycerol 65 H5 Honey 5 H20 Honey 20 H35 Honey 35 H65 Honey 65 C5 Carrageenan 5 C20 Carrageenan 20 C35 Carrageenan 35 C65 Carrageenan 65 Characterization of the DeChNF plasticized films Determination of DeChNF plasticized film thickness The thickness of the produced samples was measured using a digital micrometer (Mitutoyo Co., Kawasaki, Japan) with 0.001 mm accuracy. The thickness measurement of each film sample was replicated five times at different areas of the film, and the mean value of the film’s thickness was calculated. The density of ChNF films was determined by measuring their dimensions and air-dried weight. Fourier Transform Infra-Red (FTIR) Spectroscopy and DA conductometric titration The surface functional groups of the control and the DeChNF plasticized films were studied through IR spectra recorded using a Spectrum 2000 FTIR spectrophotometer (Perkin-Elmer Inc., USA) equipped with an attenuated total reflectance crystal accessory (Golden Gate). All samples were scanned in the range of 400–4000 cm − 1 . A total of 64 scans with a wavelength resolution of 4 cm − 1 were performed on each sample. The spectra were interpreted using the frequency assignment approach. As reported in previous work, the DA of the ChNFs was measured using the conductometric titration method [ 43 ]. X-ray Powder Diffraction (XRD) The X-ray Powder Diffraction (XRD) patterns were employed to analyze the α-chitin crystalline structure. The data were collected in the 2θ range of 5 − 40° using an X-ray diffractometer (Rigaku Co., Ltd., South Africa) with Cu Kα radiation (λ = 1.5418 Å) at 40 kV and 40 mA. The diffractograms were curve-fitted in Origin software to obtain the crystallinity index. Regular Light Transmittance Spectrophotometry The films' light transmittance was measured using an Analytikjena SPECORD 210 PLUS UV-Vis spectrophotometer (UV-2550, Shimadzu, Japan). The wavelengths from 200 to 900 nm were scanned. The transmittance spectra were recorded at room temperature, with air as a reference. Differential Scanning Calorimetry (DSC) The film samples were conditioned (65% ± 1% for 24 h) before analyses using the DSC model Universal V3-9A TA Instrument, made in New Castle, USA. The calibration of the equipment was conducted using indium as a standard. For DSC analyses, 5 mg of film samples were weighed, placed in an aluminum sample pan, and immediately sealed. An empty sample pan was used as a reference. Film samples were heated from 0 to 400°C at 10°C/min. Nitrogen gas was used to flush the DSC cell at a 20 mL/min flow rate to maintain an inert environment. The transition temperatures were determined from the thermogram results. Tensile Properties Measurement The tensile test was conducted using the method previously used by Mushi et al. [ 41 ] with a few modifications. The tensile properties of the control and the plasticized films were studied from 5 specimens. The specimens were cut into a width = 5 mm and a length = 20 mm, then conditioned at 20℃ overnight. The uniaxial deformation test was performed using a Universal tensile testing machine (Instron, UK) with a crosshead speed of 2 mm/min and a load cell of 10 kN to obtain tensile modulus, tensile strength, and tensile strain to failure. Determination of the Moisture Content and Water Absorptive Capacity The film samples' moisture content (MC) was determined by weighing each sample (Wi) using a digital scale. The samples were then dried in an oven at 105°C for 24h and reweighed (W f ), and the MC was calculated using Eq. (1) [ 44 ]. The test was carried out in triplicate, and the final MC for each film was recorded as the mean of the results. MC = \(\:\:\frac{Wi-Wf}{Wi}\times\:100\) (1) The film's water absorption capacity (WAC) was determined according to Pereda and Norma [ 45 ] with minor modifications. The water sorption capacity of each film was studied by immersing a known mass (Wd) of the film sample into distilled water at room temperature (23 ± 2°C). The Film was periodically removed from the distilled water and reweighed until a constant film mass (Ww) was attained. The test was performed in triplicate. The water uptake was determined using Eq. (2). WAC = \(\:\:\frac{Ww-Wd}{Wd}\times\:100\) (2) Determination of Water Vapor Permeability Before the water vapor permeability (WVP) test, the film samples were conditioned in a desiccator with a relative humidity of 50% at 25°C. The WVP test was conducted using the method described by Pereda et al. [ 45 ] with minor modifications. The films were cut into rectangular shapes (7.5 cm x 7.5 cm) and then mounted and sealed on the open mouth of cylindrical cups containing 20 g of calcium chloride. The test cups were measured before being kept in a relative humidity chamber (25°C, relative humidity 75%). The weight of the test cups was determined by periodic measurement till the equilibrium state was reached. Weight increments of the test cups were recorded, and WVP was calculated using Eq. (3). WVP= \(\:\:\frac{m\:\times\:\:d}{A\:\times\:t\:\times\:\:P}\times\:100\) (3) Where m (g) is the weight increment of the test cup, d (mm) is the film thickness, A (m 2 ) is the area of film exposed, t (s) is the duration for permeation, and P (Pa) is the water vapor partial pressure across the films. The results were expressed in g·mm·s − 1 ·m − 2 ·Pa − 1 . Results and Discussion Physical properties of the plasticized DeChNF films Figure 2 a shows the thickness of the plasticized DeChNF films. It was observed that the film thickness increased from 0.041 to 0.074 mm, 0.054 to 0.105 mm, and 0.052 to 0.097 mm with concentrations of G, H, and C, respectively. The film thickness increased as the plasticizer concentration increased from 5 to 65%, regardless of plasticizer type. Films with H were thicker than those plasticized with C and G. Moreover, the type of plasticizer significantly influences film thickness, indicating a sign of interfacial interactions between the plasticizers and DeChNFs. Figure 2 b shows the effect of plasticizer type and concentration on the density of DeChNF films plasticized with different ratios of plasticizers. The addition of plasticizers reduced the density of native DeChNF (1.24 g/cm 3 ). All the plasticized films exhibit lower density than the control DeChNF film. Increasing the concentration of plasticizers from 5 to 65 % causes a slight decrease in the density of G-(1.173 − 1.112 g/cm 3 ), H- (1.193 − 1.154g/cm 3 ), and C-plasticized films (1.153 − 1.127 g/cm 3 ). According to Jouki et al. [ 47 ], an increase in glycerol content from 25–50% for cress seed gum (CSG) edible films led to a notabe increase in film thickness, from 0.067 mm to 0.079 mm. Likewise, the density values decreased from 1.26 g/cm 3 at 25% to 1.22 g/cm 3 at 50% glycerol [ 47 ]. Tarique et al. [ 46 ] observed a decrease in film density for arrowroot ( Maranta arundinacea) starch films with 15, 30, and 45% glycerol, as observed in DeChNF plasticized films. The higher thickness of H-plasticized film may be related to honey's unique complex molecular composition, which includes a mixture of sugars. In contrast, glycerol is a small, simple molecule of trihydroxy alcohol that penetrates the network of chitin easily. While forming a strong gel-like network, carrageenan does not create a denser network than honey. Increasing film thickness can be attributed to the role of plasticizers in disrupting and restructuring intermolecular polymer chain networks [ 46 ]. Percent-wise, the current data demonstrate a much more significant change in thickness. The FTIR spectra of both unplasticized and plasticized DeChNF films are presented in Fig. 2 c-e. The spectral peak conforms to intra- and intermolecular O-H stretching at 3444 cm − 1 , while the peaks at 3245 and 3100 cm − 1 are associated with the N-H stretching band [ 28 , 48 , 49 ]. The doublets observed at 1654 cm⁻¹ and 1621 cm⁻¹ correspond to amide I (C = O stretching). The amide II band (N–H bending) is present at 1554 cm⁻¹, along with the amide III band (C–N stretching) at 1310 cm⁻¹ [ 50 , 51 ]. These spectral peaks characterize the α-chitin in the DeChNFs material. The frequency shift of the broad bands of hydroxyl functional groups in DeChNF indicates the presence of hydrogen bonding between DeChNF and the plasticizers. The peaks around 2950 cm − 1 are attributed to C-H aliphatic absorption peaks, and the characteristic peaks at 1004 cm − 1 are assigned to the C-O bond stretching of C-O-C groups in the anhydrous-glucose ring of DeChNF. These results from the FTIR analysis provide valuable insights into the molecular interactions in the films, highlighting the complex interplay between chitin and plasticizers. In essence, the interactions are primarily dominated by physical bonding between the nanofibrils and the plasticizers. Figure 2 f presents XRD patterns of DeChNF films plasticized with 20 wt. % of glycerol, honey, and carrageenan. All the plasticized nanofilms retained the α-chitin structure, as indicated by the four sharp crystalline reflections at 2ϴ = 9.3, 12.6, 19.3, and 26.4, corresponding to the (020), (021), (110), and (013) lattice planes [ 52 , 53 ]. The X-ray diffraction patterns of unplasticized DeChNF films are similar to those of G-plasticized, H-plasticized, and C-plasticized films, indicating that plasticization did not affect the chitin crystal structure, in support of the FTIR mentioned above. Regular light transmittance of the plasticized DeChNF films Figure 3 a presents photographic images of free-standing films prepared from deacetylated chitin nanofibers (DeChNF) with varying ratios of plasticizers, while Table 2 outlines their visual characteristics. Notably, free-standing DeChNF plasticized films were successfully obtained even at higher concentrations of plasticizers. In contrast, DeChNF films without plasticizers appeared wavy, brittle, semi-rigid, and fragile. This phenomenon can be attributed to the strong inter- and intramolecular hydrogen bonds within DeChNF due to the capillary condensation, common during the drying process, which restricts the mobility of the macromolecular chains and leads to brittle and semi-rigid films. The addition of plasticizers to the DeChNF films enhanced their flexibility and smoothness. Among the tested films, those with 65% plasticizer content exhibited the greatest flexibility, while flexibility decreased as the amount of plasticizer was reduced, regardless of its type. Among all plasticized DeChNF films, those with honey (H65) were particularly flexible but weak and highly sticky, making them difficult to peel off the petri dish (data not shown here). This stickiness is attributed to honey's complex, sugary constituents, which become more pronounced at higher concentrations. In contrast, films with glycerol and carrageenan were easier to peel off due to the more effective incorporation of these plasticizers within the intermolecular spaces of the DeChNF. This integration strengthens the cohesive nature of the chitin molecules, contributing to the easier peeling of the glycerol- and carrageenan-plasticized films. Figure 3 b displays the regular light transmittance spectra for a series of plasticized DeChNF films. The transmittance of the deacetylated ChNF film without plasticizer was found to be 84.9% at 800 nm. In comparison, films with 20 wt% plasticizers — G20, H20, and C20 — showed approximate transparency values of 87.8%, 83.6%, and 85.4%, respectively. Light transmittance measured using a UV-Vis spectrophotometer allows for comparing the transparency of different films over a wide spectrum. The plasticizers' smaller molecular size, i.e., glycerol, likely enhances molecular interactions, reducing voids within the DeChNF matrix and creating a more homogeneous structure that minimizes light scattering. While the refractive index values are essential to increase understanding, this data was inferred rather than directly measured. Research on transparent wood showed that transparency depends on the similarity in refractive indices among constituents such as cellulose nanofibrils, methyl methacrylate, and styrene monomers [ 54 ]. According to the literature, the refractive index of glycerol is approximately 1.472 [ 55 ], DeChNF ranges from 1.56 to 1.58 [ 56 ], carrageenan varies between 1.33 and 1.45 [ 57 ], and honey ranges from 1.488 to 1.504 [ 58 ]. These values can change based on moisture content, crystallinity, polymer conformation, nanofibril size, processing methods, and composition. Therefore, combining glycerol, honey, or carrageenan with DeChNF likely facilitates effective matching, leading to minimized light scattering at interfaces. As such, all films exhibited high transmittance regardless of plasticizer content. The low transparency of honey-plasticized films remains to be investigated. Table 2 Appearance of unplasticized and plasticized DeChNF films Sample Plasticizer type Appearance of the films DeChNF - Transparent, brittle, and fragile, rigid surface cracks G5 Glycerol Transparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable G20 Glycerol Transparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable G35 Glycerol Transparent, not brittle and fragile, no surface cracks, flexible, slightly sticky/tacky, slightly difficult to peel G65 Glycerol Transparent, not brittle and fragile, no surface cracks, flexible, sticky/tacky, slightly difficult to peel H5 Honey Transparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable H20 Honey Transparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable H35 Honey Transparent, not brittle and fragile, no surface cracks, flexible, slightly sticky/tacky, slightly difficult to peel H65 Honey Transparent, not brittle and fragile, no surface cracks, flexible, highly sticky/tacky, difficult to peel C5 Carrageenan Transparent, not brittle and fragile, rigid, no surface cracks, flexible, not sticky/tacky, peelable C20 Carrageenan Transparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable C35 Carrageenan Transparent, not brittle and fragile, no surface cracks, flexible, slightly sticky/tacky, slightly difficult to peel C65 Carrageenan Transparent, not brittle and fragile, not rigid, no surface cracks, flexible, sticky/tacky, slightly difficult to peel DSC of the DeChNF-plasticized films The DSC curves are shown in Fig. 4 a-c, and a bar chart of the relaxation temperatures with plasticizer type and content is summarized in Fig. 4 d. An initial endothermic peak is observed between temperatures (T 1 ) 40–80°C (highlighted in yellow) for both the control DeChNF and the plasticized films. The endothermic peak for the glycerol-plasticized DeChNF films (G5) is less pronounced than those plasticized with honey and carrageenan. At elevated temperatures, a significant exothermic peak appears between temperatures (T 2 ) 300–370°C (also highlighted in yellow) for both the control and plasticized films. Notably, there is a shift in the relaxation temperature towards lower values as the plasticizer content increases. For the control DeChNF films, which have a transition temperature of around 365°C, the relaxation temperature shifts dramatically to 301°C for the honey-plasticized films. By comparison between the plasticized films, the trend in the relaxation behavior closely matches that observed in films at lower temperatures. Based on the relaxation trend, a more substantial plasticization effect appears to be associated with honey, followed by glycerol, and finally, carrageenan. This could be due to the disrupted film structure and thus plasticization, which is noteworthy. According to literature data [ 59 ], chitin has a relaxation temperature of around 60–100°C, which is sensitive to its moisture content and degree of crystallinity. The composition of honey is complex, and its relaxation temperature is not clearly defined. However, softening temperatures range between − 51°C and − 33°C, depending on its water content [ 60 ]. Carrageenan exhibits primary relaxation behavior in the 150–200°C range, with additional secondary relaxations occurring between 60°C and 90°C, depending on carrageenan sulfate content and properties, as well as moisture content [ 61 ]. Glycerol undergoes a transition around − 94°C [ 62 ], with secondary relaxation processes observable in the 10–30°C range [ 63 ], which is also influenced by moisture. When these components are combined, their relaxation behavior becomes more complex and may be affected by the relative ratios and interactions with ChNF at the interfaces. Both DeChNFs, glycerol, honey, and carrageenan can absorb moisture. Since moisture significantly impacts the relaxation temperature, the transition occurring at lower temperatures, around 40–80°C, may indicate the loss of freely bound water within the films. Additionally, the relaxation temperatures of carrageenan, glycerol, and honey may overlap with water evaporation. Water interaction can be classified based on different states. Water evaporates at lower temperatures, while bound water evaporates at slightly higher temperatures due to its stronger interaction with the materials. The DSC relaxation peak at 365°C in DeChNF can be attributed to molecular relaxation, breaking of hydrogen bonds, and amorphous phase transitions, as complete decomposition occurs at higher temperatures around 400–450°C [ 64 ]. Tarique et al. [ 46 ] used a dry processing technique (hot pressing) and observed a reduction in transition temperature from 294.6°C to 291.9°C for starch films plasticized with 15, 30, and 45% glycerol. Similarly, Hazrati et al. [ 65 ] observed decreased relaxation temperature in starch films plasticized with 30, 45, and 60% glycerol, sorbitol, and urea, respectively. Thus, the shift in the relaxation temperature of chitin towards lower values reflects increased molecular mobility, which signifies a crucial indication of plasticization. Mechanical properties of the DeChNF-plasticized films Figure 5 a-c show the stress-strain curves of the DeChNF films with varying plasticizer contents, as shown in Fig. 5 a-c, reveal two distinct deformation behaviors. In pure DeChNF, the elastic deformation is followed by the plastic deformation, resulting in a more developed curve than the films containing plasticizers. As plasticizer content increases, the tensile strain to failure in the plastic region increases. Initially, DeChNF networks dominated the elastic region, with the plasticization effect becoming more pronounced with higher plasticizer content. Consequently, the slope of the elastic region gradually decreases. Apart from other arguments, and by the assumption that the nanofibril dimensions are distributed homogeneously, the molar mass of the plasticizers plays an essential role in controlling strain-hardening behavior in the plastic region. Glycerol, a commercially available plasticizer, displayed the same trend as honey and carrageenan. As shown in Fig. 5 d-f, Young’s modulus, tensile strength, and strain of DeChNF film without plasticizer were comparatively high, measuring 3.1 GPa, 41.3 MPa, and 8.2%, respectively. The addition of plasticizers from 0–65% resulted in a significant reduction in the tensile strength of films, regardless of the type of plasticizer used. Nevertheless, for G-plasticized films, tensile strength notably decreased from 41.3 MPa to 6.3 MPa, while for H-plasticized films, it dropped from 41.3 MPa to 4.3 MPa. In the case of C-plasticized films, the tensile strength decreased from 41.3 MPa to 9.4 MPa over the same range of plasticizer concentrations. These reductions correspond to 85%, 90%, and 77%. H-plasticized films showed the highest reduction in tensile strength, at 90%, compared to G- and C-plasticized films. The data on elastic modulus, which indicates the stiffness of materials, is represented in Fig. 5 d. It is evident that the effect of plasticizer concentration (0–65%) on Young’s modulus of DeChNF-plasticized films closely resembles the behavior of their corresponding tensile strength, although different factors govern them. Increasing the plasticizer concentration from 0–65% led to a noticeable decrease in film stiffness, from 3.1 GPa to 0.7 GPa for G-plasticized films, 3.1 GPa to 0.5 GPa for H-plasticized films, and 3.1 GPa to 1.1 GPa for C-plasticized films. These reduction values corresponded to a 74%, 80%, and 65% decrease in stiffness for G-plasticized, H-plasticized, and C-plasticized, respectively. The effect of plasticizer concentration (0–65%) on the tensile strain of DeChNF plasticized films is also analyzed. As anticipated, increasing the plasticizer concentration resulted in a considerable increase in film tensile strain from 8.5–24.74% for G-plasticized films, 8.5–31.5% for H-plasticized films, and 8.5–21.65% for CG-plasticized films. The observed mechanical data suggest that the DeChNF matrix is indeed plasticized. The high mechanical properties of the plain DeChNF films can be attributed to the strong hydrogen bonding, which sometimes co-crystallizes, between strong nanofibrils caused by the ambient drying process. DeChNFs derived from crab shells possess an extended-type crystalline structure, contributing to increased stiffness and strength. Moreover, nanofibril-nanofibril interaction controls the strength in the plastic region. The plasticizer disrupts the hydrogen bonds between chitin-chitin nanofibril molecules. As a result, this led to an enhancement in flexibility by allowing greater chain mobility. Although dynamic thermomechanical data on molecular mobility could further support these findings, this study does not present them. Decreasing tensile modulus, strength, and increasing strain to failure have been reported in the literature [ 30 , 47 , 60 , 66 ]. The decrease in tensile strength of DeChNF-based films with plasticizer concentration is a significant observation. Mushi et al. [ 30 ] investigated DeChNF films plasticized with honey (35%) and compared them to films plasticized with glycerol (25%), both prepared through the casting technique. The much higher tensile strength for honey-plasticized DeChNF films (35% concentration, 21.32 MPa) was striking [ 30 ]. According to Muscat et al. [ 67 ], tensile strength in starch films decreased with increasing glycerol and xylitol concentrations above 15%. Hazrati et al. [ 60 ] focused on starch films with sorbitol and fructose, where 35% sorbitol yielded the highest elongation at break, and 35% fructose yielded the highest tensile strength. Suppakul et al. [ 66 ] found that tensile strength vastly decreased with increasing sorbitol concentration while the elongation percentage increased significantly. Here, a low-weight fraction of honey achieves higher strain results. With honey (20 wt%) in DeChNF films, a higher tensile strain (31.5%) was reported compared to glycerol (24.74%), while glycerol (6.3 MPa) showed a higher tensile strength than honey (4.3 MPa) at the same concentration. For the Suppakul et al. [ 66 ] results on cassava flour starch films with sorbitol, the present data showed a decrease in tensile strength and an increase in tensile strain (elongation) in DeChNF films with increasing concentrations of glycerol, honey, and carrageenan. Both studies by Muscat et al. [ 67 ] and Suppakul et al. [ 66 ] focused on starch-based films whose commercial applicability is hindered by poor ductility. The higher strength data is intriguing with honey-plasticized DeChNF films (35% concentration, 21.32 MPa) in the literature, suggesting a promising potential for this material. In general, the presented DSC and mechanical data could suffice to demonstrate the effectiveness of the materials studied as plasticizers for controlling the mechanical properties of DeChNF films. Finally, the mechanical properties of the obtained films are comparable to those of significant packaging films, as shown in Table 3 . Although synthetic polymers such as PE, PP, Nylon, PET, and EVOH exhibit higher tensile strain to failure [ 6 – 15 , 68 ] than the biopolymeric films, molecular weight and polymer structure differences may account for this disparity. Table 3 Mechanical properties of the major packaging films Packaging films Tensile strength (MPa) Modulus (GPa) Elongation (%) References DeChNF/Glycerol 6.3 (0.2)-41.3 (0.4) 0.7–3.1 8.5–24.7 DeChNF/Honey 4.3 (0.2)-41.3 (0.4) 0.5–3.1 8.5–31.5 This work DeChNF/Carrageenan 9.4 (0.3)-41.3 (0.4) 1.1–3.1 8.5–21.7 Chitosan 20.8 * 12.7 [ 6 ] Gelatin 41 * 34 [ 7 ] Carboxymethyl cellulose 28–51 2–4 65–91 [ 8 ] Hydroxymethyl methylcellulose 38.35 1.6 9.40 [ 9 ] Cellulose acetate 46.56 5 6.8 [ 10 ] Ethylcellulose 14–29 0.5-1.0 * 11] Starch 4.48–8.14 0.12–0.29 35–100 [ 12 ] Xyloglucan 55–78 4.6–5.4 1.7–5.7 14] Cellulose nanofibers 42–175 1.5–15 15–50 [ 15 ] Polyethylene (PE) 10–40 0.2–1.5 100–700 [ 68 ] Polypropylene (PP) 20–50 1–2 200–600 [ 68 ] Polyvinyl chloride (PVC) 40–60 1–3 10–400 [ 68 ] Polyamide (Nylon) 70–80 2–3 100–200 [ 68 ] Ethylene vinyl alcohol (EVOH) 50–60 3–4 100–200 [ 68 ] Polyethylene Terephthalate (PET) 50–70 2–3 50–150 [ 68 ] * Data were not reported. The bracket for experimental data indicates the standard deviation Water interaction properties of the plasticized DeChNF films Figure 6 a presents the MC of the control and plasticized films. For all plasticized DeChNF films, the moisture content increased significantly as plasticizer concentration increased from 5 to 65%. Generally, DeChNF-based films absorbed more moisture with higher plasticizer concentrations. Several researchers have reported that adding more plasticizers increases the MC of the films [ 1 , 2 ]. Figure 6 b presents the WAC of unplasticized and plasticized films when immersed in water. As shown in Fig. 6 b, adding plasticizers significantly raised the WAC of the plasticized DeChNF films. At all concentrations, films with C were more water-resistant and less hygroscopic than those with G and H. The increase of plasticizer content had a notable effect on the WAC of the plasticized DeChNF films. The concentration of plasticizers has less influence on the C-plasticized films. This is attributed to the strong hydrogen bonding between the plasticizer and chitin. In addition, a limited solubility of water in carrageenan may contribute. The impact of different plasticizer types and their concentrations on the WVP of DeChNF films is summarized in Fig. 6 c. The WVP values of plasticized DeChNF films increased with higher plasticizer content. Specifically, the results indicate that increasing the plasticizer concentration from 5–65% led to WVP values rising from 3.82 × 10 − 10 to 8.41 × 10 − 10 g·s − 1 ·m − 1 ·Pa − 1 for G-plasticized films, from 4.24×10 − 10 to 9.17×10 − 10 g·s − 1 ·m − 1 Pa − 1 for H-plasticized films, and from 3.02×10 − 10 to 6.78×10 − 10 g·s − 1 ·m − 1 ·Pa − 1 for C and G-plasticized films. All plasticized films, regardless of the type of plasticizer, exhibited increased WVP values. Among the plasticizers tested in this study, DeChNF film with glycerol (G-plasticized) and honey (H-plasticized) demonstrated the highest WVP values. For MC, Jouki et al. [ 47 ] observed an increase with increasing glycerol concentration, from 16.37% at 25% glycerol to 18.78% at 50% glycerol. For WAC, Sanyang et al. [ 69 ] observed from the casted films of glycerol, sorbitol or their combination as plasticizers at the ratio of 15, 30, and 45 (wt%) with sugar palm starch (SPS) that the moisture content increased from 7.9–12.4% for glycerol, 6.6–8.1% for sorbitol and 11.4–18.6% for glycerol-sorbitol blend. Tarique et al. [ 46 ] demonstrated in arrowroot starch films plasticized with glycerol (15, 30, and 45 wt. %) that moisture content and solubility in water increased with the glycerol content. For WVP, Muscat et al. [ 67 ] have reported low WVP in films plasticized by combined plasticizers at a 20% concentration for low and high amylose starch-based films plasticized with glycerol and xylitol. WVP results showed an increased value from 0.55 to 1.34 g mm/m2 h, and the glycerol concentration ranged from 20, 30, and 40 (wt.%). In contrast, the current study observed an increased value of WVP with plasticizer content. An increase in WVP can be attributed to plasticizers modifying the structure of the DeChNF networks. The ability of materials to minimize moisture transfer in the surrounding environment is essential for adequate packaging [ 46 ]. As such, Table 4 was developed to compare the WVP of some selected, most common films [ 68 ] with those from the plasticized DeChNF films. The WVP of materials should be as low as possible, particularly for food packaging. More hydrophobic polymers, mainly derived from fossil-based resources, such as LDPE, HDPE, PVC, PP, and BOPP, exhibit lower WVP, which aligns with expectations. In contrast, because the unique character of biopolymeric materials has strength in the presence of moisture, the higher WVP, or MAC, in that regard, is not surprising but may be attributed to their superior characteristics in the presence of moisture. Table 4 WAC and WVP of plasticized DeChNF films and the reference films from the major packaging materials Packaging films Water absorption capacity (g) WVP (×10 − 10 g.s − 1 m − 1 Pa − 1 ) References DeChNF/0–65%Glycerol 0.9–3.5 2.84–8.41 DeChNF/0–65%Honey 1.8–4.7 2.84–9.17 This work DeChNF/0–65%Carrageenan 0.5–2.5 2.84–6.78 Chitosan 3 * [ 6 ] Gelatin 4.1 0.81–1.14 [ 7 ] Carboxymethyl cellulose * 2–4 [ 8 ] Hydroxymethyl methylcellulose * 4.41 [ 9 ] Cellulose acetate * 2.6 [ 10 ] Ethylcellulose * 8–14 [ 11 ] Starch 2 0.12–0.29 [ 65 ] xyloglucan * 0.5–1.9 [ 13 ] Low-density polyethylene (LDPE) * 0.003–0.005 [ 68 ] High-density polyethylene (HDPE) 0.00125 [ 68 ] Polypropylene (PP) * 0.001-0.00125 [ 68 ] Polyvinyl chloride 0.0075 [ 68 ] Biaxially oriented polypropylene (BOPP) * 0.001-0.00125 [ 68 ] * Data were not reported Conclusions The DeChNF films, which incorporated glycerol, honey, and carrageenan as plasticizers, were prepared through casting, and their effectiveness on the DeChNF films was examined. The DeChNF films that contained up to 65% w/w of plasticizer content demonstrated impressive properties as a packaging material and have been presented. The mechanical performance is good. Due to the plasticizing effect of glycerol, honey, and carrageenan, Young’s modulus and tensile strength were reduced, while the tensile strain increased, depending on the amount of plasticizer added. Concurrently, a shift in the relaxation temperature of the DeChNF film towards lower temperatures with plasticizer content observed around 40–90ºC and 300–370ºC, suggests a notable plasticization effect, with a more substantial plasticization appears to be associated with honey, followed by glycerol, and finally, carrageenan. Consequently, this shows that the mechanical properties of the deacetylated ChNF film can be optimized or tailored without compromising their essential attributes, including high transparency, thermal stability, WAC, and WVP. The mechanical performance of the film containing carrageenan is superior to that of the films plasticized with honey and glycerol. Furthermore, the tensile strengths of the DeChNF films with 5% w/w glycerol, honey, and carrageenan surpassed those of commercial polyethylene films, which have a tensile strength of only 10.9 MPa. Interestingly, this study is particularly significant since honey and carrageenan are high-quality, food-grade materials that are naturally occurring compared to glycerol. The implications of this study are substantial, as it enhances not only the potential applications of ChNFs in the development of high-performance films but also promotes the use of chitin as a natural, eco-friendly material, especially for edible films in packaging. Limitations and Future perspectives of the DeChNF plasticized films in Packaging In summary, this study successfully demonstrated that honey and carrageenan can serve as natural plasticizers to replace glycerol and potentially other conventional plasticizers such as sorbitol, xylitol, fructose, and urea, thereby enhancing the applicability of DeChNF films. The literature has extensively reported the impact of plasticizer concentration on the mechanical and barrier properties of biopolymer films, particularly those made from starch and chitosan, and recently, on cellulose and DeChNF. Summarizing the results from the previous studies presented in this work. Firstly, Jouki et al. [ 47 ] demonstrated that increasing glycerol concentration in cress seed gum films enhanced water vapor permeability, thickness, moisture content, water solubility, elongation at break, and surface smoothness, while decreasing density, tensile strength, and Young's modulus. Secondly, Sanyang et al. [ 69 ] observed increased moisture content, film thickness, and water solubility, while sugar palm starch films' density and water absorption decreased. Thirdly, Tarique et al. [ 46 ] demonstrated reduced moisture content and water solubility, along with increased tensile strain, but a decrease in tensile strength and modulus in arrowroot starch films plasticized with glycerol (at 15, 30, and 45 wt%). In contrast, Muscat et al. reported that combining glycerol and xylitol as plasticizers resulted in low WVP in low and high-amylose starches. Fourthly, Suppakul et al. [ 66 ] also observed a decrease in tensile strength and MVP, alongside an increase in the percentage of elongation to failure, with a rise in plasticizer content up to a certain level. These changes have been attributed to the molecular properties of the plasticizers. Consequently, the film structure may alter, affecting density and thickness. Despite the different focuses in the literature compared to the current study, particularly in preparation techniques and materials, the performance of glycerol and similar conventional plasticizers, alongside honey and carrageenan as alternatives, is apparent, highlighting the potential applicability of these natural plasticizers. However, several limitations exist. Firstly, while plasticization improved the flexibility of the films, it significantly reduced their tensile strength and Young's modulus of the DeChNF film. This reduction may limit the application of these films in packaging scenarios where high mechanical strength is critical. The optimization of the preparation technique and conditions can mitigate this issue. Nonetheless, our novel approach, using natural plasticizers to enhance the properties of DeChNF films, represents a unique contribution to the field. Future research should explore reinforcement strategies to balance flexibility and strength, such as cross-linking or blending with other biopolymers [ 69 ]. Secondly, issues related to higher water absorption and permeability were observed. The high WAC and WVP of the plasticized films indicate a concern about the susceptibility of the film properties to moisture. This could impact the films' structural integrity and effectiveness in protecting food in high-humidity environments. Further optimization, such as using hydrophobic coatings, nanocomposites, or lamination techniques, could enhance the moisture resistance of these films [ 48 , 67 ]. Chemical modification will improve compatibility for blending with the vast available polymers, such as LDPE, which are hydrophobic. Thirdly, the compatibility and long-term stability of the plasticizers need to be considered. The stickiness and adhesion issues noted in honey-plasticized films could affect handling and practical use in packaging. Over time, plasticizer migration and phase separation may alter the films' mechanical and barrier properties. Fourthly, imaging of the microstructure was not conducted in this study. However, we can infer the homogeneity and structural integrity of the films from their optical transparency, mechanical properties, and XRD data, which suggest a uniform dispersion of the plasticizers. Fifthly, scalability and economic viability are crucial. Although the study successfully developed DeChNF films, scaling production will require cost-effective and industrial-friendly methods. Exploring alternative processing techniques, such as vacuum filtration, melt-processing techniques, e.g., extrusion, or bio-composite layering, could enhance the feasibility of mass production. The potential of chitin-based films in packaging applications can be further enhanced through specific future studies. For instance, incorporating scanning electron microscopy (SEM) imaging could help investigate the film morphology and confirm the impact of plasticization at the nanoscale. Additionally, enhancing mechanical performance can be achieved by blending DeChNF with other biopolymers like starch, polylactic acid (PLA), or nanocellulose, or through nanocomposite reinforcement by incorporating clay nanoparticles, cellulose nanocrystals, carbon nanofibers, or graphene oxide [ 6 , 70 ]. Improving moisture barrier properties is another avenue for development. This can include layering DeChNF films with hydrophobic coatings such as wax, zein protein, or biodegradable polyesters. Cross-linking agents like tannins, citric acid, or enzymatic treatments can strengthen the intermolecular network, thereby reducing WVP [ 71 ]. Moreover, biodegradability can be tailored to meet specific applications. For example, controlled degradation profiles can be developed by modifying the degree of deacetylation of chitin to match different packaging needs, such as short-term food wrapping versus long-term storage. Lastly, utilizing chitin from the seafood industry promotes a circular economy and supports cost-effective production. Exploring innovative packaging applications, such as antimicrobial coatings, pH-sensitive food freshness indicators, and oxygen scavenging films, can help extend food shelf life. Declarations Funding: This project was supported by Knut och Alice Wallenbergs Data availability : No data sets were generated or analyzed during the current study. Competing interest : The authors declare no competing interest Author Contribution N.E Conceptualizations, Methodology, Analysis, and Writing. C.F.K. Experimentation, Writing, and Analysis. N.M Conceptualization, Writing, and Reviewing. All authors reviewed and approved the manuscript. Acknowledgement Prof LA Berglund at KTH Royal Institute of Technology is acknowledged for constructive discussions and provision of partial funding through his grant with the Knut and Alice Wallenberg Foundation. References Abotbina W, Sapuan SM, Sulaiman S, Ilyas RA (2020) Review of Corn Starch Biopolymer. In Proceedings of the 7th Postgraduate Seminar on Natural Fibre Reinforced Polymer Composites Serdang, Malaysia: Institute of Tropical Forest and Forest Products (INTROP), University Putra Malaysia. 37–40 Iram D, Riaz R, Iqbal RK (2019) Usage of Potential Micro-organisms for Degradation of Plastics. Open J Environ Biol 4:7–15. https://doi.org/10.17352/ojeb.000010 Abotbina W, Sapuan SM, Sultan MTH, Alkbir MFM, Ilyas RA (2021) Development and Characterization of Cornstarch-Based Bioplastics Packaging Film Using a Combination of Different Plasticizers. Polym 13:3487. https://doi.org/10.3390/polym13203487 Syafiq RMO, Sapuan SM, Zuhri MYM, Othman SH, Ilyas RA (2022) Effect of plasticizers on the properties of sugar palm nanocellulose/cinnamon essential oil reinforced starch bio-nanocomposite films. Nanotechnol Rev 11:423–437. https://doi.org/10.1515/ntrev-2022-0028 Ilyas M, Ahmad W, Khan H, Yousaf S, Khan K, Nazir SP (2018) Plastic Waste as A Significant threat to Environment-A Systematic Literature Review. Rev Environ Health 33:383–406. https://doi.org/10.1515/reveh-2017-0035 Qin YY, Zhang ZH, Li L, Yuan ML, Fan J, Zhao TR (2015) Physio-mechanical properties of an active chitosan film incorporated with montmorillonite and natural antioxidants extracted from pomegranate rind. J food Sci Techno 52:1471–1479. https://doi.org/10.1007/s13197-013-1137-1 Rawdkuen S, Sai-Ut S, Benjakul S (2010) Properties of gelatin films from giant catfish skin and bovine bone: a comparative study. Eur Food Res Technol 23:907–916. https://doi.org/10.1007/s00217-010-1340-5 Laith SA, Al-Hashimi AG (2019) Mechanical Properties of carboxymethyl cellulose edible films. Basrah J Agri Sci 32:68–78. https://doi.org/10.37077/25200860.2019.129 Shivakumara LR, Demappa T, Singh V (2017) Mechanical and barrier properties of hydroxy propyl methyl cellulose edible polymer films with plasticizer combinations. J Food Proc Pre 4:745–4549. https://doi.org/10.1111/jfpp.13020 Gonçalves SM, Dos Santos DC, Motta JFG, Dos Santos RR, Chávez DWH, de Melo NR (2019) Structure and functional properties of cellulose acetate films incorporated with glycerol. Carbohyr Polym 209:190–197. https://doi.org/10.1016/j.carbpol.2019.01.031 Horvat G, Žvab K, Knez Ž, Novak Z (2022) Simple, one-pot method for preparing transparent ethyl cellulose films with good mechanical properties. Polym 14:2399. https://doi.org/10.3390/polym14122399 Domene-López D, García-Quesada JC, Martin-Gullon I, Montalbán MG 2019 Influence of starch composition and molecular weight on physicochemical properties of biodegradable films. Polym 11: 1084. https://doi.org/10.3390/polym11071084 Santos NL, Braga RC, Bastos MS, Cunha PL, Mendes FR, Galvão AM, Passos AA (2019) Preparation and characterization of Xyloglucan films extracted from Tamarindus indica seeds for packaging cut-up ‘Sunrise Solo’papaya. Int J Biol Macromol 132:1163–1175. https://doi.org/10.1016/j.ijbiomac.2019.04.044 Kochumalayil JJ, Berglund LA (2014) Water-soluble hemicelluloses for high humidity applications–enzymatic modification of xyloglucan for mechanical and oxygen barrier properties. Green Chem 16:1904–1910. https://doi.org/10.1039/C3GC41823E Larsson PA, Berglund LA, Wagberg L 2014 Ductile all-cellulose nanocomposite films fabricated from core–shell structured cellulose nanofibrils. Biomacromol 15: 2218–2223. https://doi.org/10.1021/bm500360c Yang X, Jungstedt E, Reid MS, Berglund LA (2021) Polymer films from cellulose nanofibrils—effects from interfibrillar interphase on mechanical behavior. Macromol 9:4443–4452. https://doi.org/10.1021/acs.macromol.1c00305 Bai L, Liu L, Esquivel M, Tardy BL, Huan S, Niu X, Rojas OJ (2022) Nanochitin: chemistry, structure, assembly, and applications. Chem Rew 13:11604–11674. https://doi.org/10.1021/acs.chemrev.2c00125) Salaberria AM, Fernandes SCM, Diaz RH, Labidi J (2015) processing of α-chitin nanofibers by dynamic high pressure homogenization: Characterization and antifungal activity against A. niger. Carbohydr Polym 116:286–291. https://doi.org/10.1016/j.carbpol.2014.04.047 Ifuku S, Saimoto H (2012) Chitin nanofibers: preparations, modifications, and applications. Nanoscale 11:3308–3318. https://doi.org/10.1039/c2nr30383c FAO, The State of World Fisheries and Aquaculture (2020) Sustainability in Action. Rome: FAO, 2020. 10.4060/ca9229en . https://doi.org/10.4060/ca9229en Chen C, Wu Q, Wan Z, Yang Q, Xu Z, Li D, Rojas OJ (2022) Mildly processed chitin used in one-component drinking straws and single use materials: Strength, biodegradability and recyclability. Chem Eng J 442:136173. https://doi.org/10.1016/j.cej.2022.136173 Yan N, Chen X (2015) Sustainability: Don’t waste seafood waste 2015. Nature 524:155–157 Svensson SE, Oliveira AO, Adolfsson KH, Heinmaa I, Root A, Kondori N, Zamani A (2022) Turning food waste to antibacterial and biocompatible fungal chitin/chitosan monofilaments. Int J Biol Macromol. 209: 618–630. https://doi.10.1016/j.ijbiomac.2022.04.031 Mushi NE (2021) A review on native well-preserved chitin nanofibrils for materials of high mechanical performance. Int J Biol Macromol 178:591–606. https://doi.org/10.1016/j.ijbiomac.2021.02.149 Fan Y, Saito T, Isogai A (2010) Individual chitin nano-whiskers prepared from partially deacetylated α-chitin by fibril surface cationization. Carbohydr Polym 4:1046–1051. https://doi.org/10.1016/j.carbpol.2009.10.044 Chen C, Wang Y, Yang Y, Pan M, Ye T, Li D (2018) High strength gelatin-based nanocomposites reinforced by surface-deacetylated chitin nanofiber networks. Carbohydr Polym 195:387–392. https://doi.org/10.1016/j.carbpol.2018.04.095 Ifuku S, Ikuta A, Egusa M, Kaminaka HH, Izawa M, Saimoto M (2013) Preparation of high-strength transparent chitosan film reinforced with surface-deacetylated chitin nanofibers. Carbohydr Polym 98:1198–1202. https://doi.org/10.1016/j.carbpol.2013.07.033 Li M, Wu Q, Song K, Cheng HN, Suzuki S, Lei T (2016) Chitin Nanofibers as Reinforcing and Antimicrobial Agents in Carboxymethyl Cellulose Films: Influence of Partial Deacetylation. ACS Sustain Chem Eng 4:4385–4395. https://doi.org/10.1021/acssuschemeng.6b00981 Ifuku S, Ikuta A, Izawa H, Morimoto M, Saimoto H (2014) Control of mechanical properties of chitin nanofiber film using glycerol without losing its characteristics. Carbohydr Polym 101:714–717. https://doi.org/10.1016/j.carbpol.2013.09.076 Mushi NE, Meela E, Kaombe D (2023) Effective Enhancement of Post-Harvest Tomato Storage through Wrapping Using Deacetylated Chitin Nanofibril-Plasticized Honey Films. Tanz J Sci 14:711–724. https://doi.org/10.4314/tjs.v49i3.14 Mushi NE, Nishino T, Berglund LA, Zhou Q (2019) Strong and Tough Chitin Film from α-Chitin Nanofibers Prepared by High Pressure Homogenization and Chitosan Addition. ACS Sustain Chem Eng 7:1692–1697. https://doi.org/10.1021/acssuschemeng.8b05452 Mushi NE, Utsel S, Berglund LE (2014) Nanostructured biocomposite films of high toughness based on native chitin nanofibers and chitosan. Frontier Chem 2:99. https://doi.org/10.3389/fchem.2014.00099 Chen C (2019) Relationship between Water Activity and Moisture Content in Floral Honey, Foods (Basel, Switzerland) 1: 30. https://doi.org/10.3390/foods8010030 Kunat-Budzyńska M, Rysiak A, Wiater A, Grąz M, Andrejko M, Budzyński M, Bryś MS, Sudziński M, Tomczyk M, Gancarz M, Rusinek R, Ptaszyńska AA (2023) Chemical Composition and Antimicrobial Activity of New Honey Varietals. Int J Environ Res Public Health 3:2458. https://doi.org/10.3390/ijerph20032458 Fu M, Wu Y, Zhang Q, Xue Z, Geng C, Xia Y (2021) Study on the mechanical and flame retardant properties of a novel carrageenan fiber-CAF-K,Al. European. Polym J 150:110408. https://doi.org/10.1515/polyeng-2022-0237 Han J, Han X, Xue Z, Wang Q, Xia Y, Zhao Z (2021) An eco-friendly procedure for achieving high-yield carrageenan from Hypnea cervicornis suitable for wet spinning. J Appl Polym Sci 138:1–9. https://doi.org/10.1002/app.50833 Marangoni L, Garcia R, Maria R, Alves V (2021) Water vapor sorption and permeability of sustainable alginate/collagen/SiO 2 composite films. 152:112261. https://doi.org/10.1016/j.lwt.2021.112261 Zia KM, Tabasum S, Nasif M, Sultan N, Aslam A, Noreen, Zuber m (2019) A review on synthesis, properties, and applications of natural polymer-based carrageenan blends and composites. Int J Biol Macromol 96:282–301. https://doi.org/10.1016/j.ijbiomac.2016.11.095 Sormin RBD, Masela A, Idris A (2019) Physicochemical properties of carrageenan originated from Lermatang Village, Southwest Maluku District, and IOP Conference Series. Earth Environ Sci 339: 012053 Tasende MG, Manríquez-Hernández JA (2016) Carrageenan properties and applications: A review. Carrageenans Sources and Extraction. Methods, Molecular Structure Bioactive. Properties and Health Effects. Edition 1st Chap. Nova Sci Publisher 2:17–49 Mushi NE, Butchosa N, Salajkova M, Zhou Q, Berglund LA (2014) Nanostructured membranes based on native chitin nanofibers prepared by mild process. Carbohydr Polym 112:255–263. https://doi.org/10.1016/j.carbpol.2014.05.038 Dong M, Wu D, Han J, Wang Y, Xue Z, Xia Y (2020) Comparison of Two Different Preparation Methods of Wet-Spun Carrageenan Fibers Directly from Chondrus Extractions. ACS omega 5:6661–6665. https://doi.org/10.1021/acsomega.9b04435 Wang K, Kasuya H, Koga M, Nogi, Uetani K (2021) Thermal conductivity analysis of chitin and deacetylated-chitin nanofiber films under dry conditions. Nanomaterials 3:658. https://doi.org/10.3390/nano11030658 Jumaidin R, Sapuan SM, Jawaid M, Ishak MR, Sahari J (2017) Thermal, mechanical, and physical properties of seaweed/sugar and palm fibre reinforced thermoplastic sugar palm Starch/Agar hybrid composites. Int J Biol Macromol 97:606–615. https://doi.org/10.1016/j.ijbiomac.2017.01.079 Pereda M, Aranguren MI, Marcovich NE (2009) Water vapor absorption and permeability of films based on chitosan and sodium caseinate. J Appl Poly Sci 6:2777–2784. https://doi.org/10.1002/app.29347 Tarique J, Sapuan SM, Khalina A (2021) Effect of glycerol plasticizer loading on the physical, mechanical, thermal, and barrier properties of arrowroot (Maranta arundinacea) starch biopolymers. Sci Rep 1:13900. https://doi.org/10.1038/s41598-021-93094-y Jouki M, Khazaei N, Ghasemlou M, HadiNezhad M (2013) Effect of glycerol concentration on edible film production from cress seed carbohydrate gum. Carbohydr Polym 1:39–46. https://doi.org/10.1016/j.carbpol.2013.03.077 Tanpichai S, Srimarut Y, Woraprayote W, Malila Y (2022) Chitosan coating for the preparation of multilayer coated paper for food-contact packaging: Wettability, mechanical properties, and overall migration. Int J Biol Macromol 213:534–545. https://doi.org/10.1016/j.ijbiomac.2022.05.193 Tanpichai S, Pumpuang L, Srimarut Y, Woraprayote W, Malila Y (2023) Development of chitin nanofiber coatings for prolonging shelf life and inhibiting bacterial growth on fresh cucumbers. Sci Rep 1:13195. https://doi.org/10.1038/s41598-023-39739-6 Ifuku S, Nogi K, Abe M, Yoshioka M, Morimoto H, Saimoto H, Yano H (2009) Preparation of chitin nanofibers with a uniform width as alpha-chitin from crab shells. Biomacromol 6:1584–1588. https://doi.org/10.1021/bm900163d Boonmahitthisud A, Thongdonson K, Tanpichai S (2023) Preparation of Chitin Nanofibers from Shrimp Shell Waste by Partial Deacetylation and Mechanical Treatment Preparation of Chitin Nanofibers from Shrimp Shell Waste by Partial Deacetylation and Mechanical Treatment. J Natural Fibers 2: 2229515. https://doi.10.1080/15440478.2023.2229515 Ifuku S, Nogi M, Morimoto MY, Yano M, Saimoto H (2010) H Fibrillation of dried chitin into 10–20nm nanofibers by a simple grinding method under acidic conditions. Carbohydr Polym 1; 134–139. https://doi.10.1016/j.carbpol.2010.02.006 Aklog YK, Nagae T, Izawa H, Morimoto M, Saimoto H, Ifuku S (2016) Preparation of chitin nanofibers by surface esterification of chitin with maleic anhydride and mechanical treatment. Carbohydr Polym 153:55–59. https://doi.org/10.1016/j.carbpol.2016.07.060 Chen H, Montanari C, Yan M, Popov S, Li Y, Sychugov I, Berglund LA (2020) Refractive index of delignified wood for transparent biocomposites. RSC Adv 10:40719–40724. https://doi.org/10.1039/d0ra07409h Martini N, Jörg B, Hell SW (2002) A new high-aperture glycerol immersion objective lens and its application to 3D‐fluorescence microscopy. J Microscopy 206:146–151. https://doi.org/10.1046/j.1365-2818.2002.01016.x Zewude DA, Akamatsu M, Ifuku S (2024) Structural Color of Partially Deacetylated Chitin Nanowhisker Film Inspired by Jewel Beetle. Materials 21:5357. https://doi.org/10.3390/ma17215357 Chan SW, Mirhosseini H, Taip FS, Ling TC, Tan CP (2013) Comparative study on the physicochemical properties of κ-carrageenan extracted from Kappaphycus alvarezii (doty) doty ex Silva in Tawau, Sabah, Malaysia and commercial κ-carrageenans. Food Hydrocolloids 2: 581–588. https://doi.10.1016/j.foodhyd.2012.07.010) Albu, Frunză G, Zaharia R, Pop IM 2021 Estimation of some quality parameters of honey Kittur FS, Prashanth KV, Sankar KU, Tharanathan RN (2002) Characterization of chitin, chitosan and their carboxymethyl derivatives by differential scanning calorimetry. Carbohydr Polym 49:185–193 Kim MJ, Yoo BS (2010) Glass Transition Temperature of Honey Using Modulated Differential Scanning Calorimetry (MDSC): Effect of Moisture Content. Prev Nutr Food Sci 4:356–359. https://doi.org/10.3746/jfn.2010.15.4.356 Abdullah AHD, Firdiana B, Nissa RC, Satoto R, Karina M, Fransisk D (2021) Effect of κ-carrageenan on mechanical, thermal and biodegradable properties of starch–carboxymethyl cellulose (CMC) bioplastic. Cell Chem Technol 9–10:1109–1117. https://doi.org/10.35812 Angell C, Austen Sare EJ, Bressel RD (1967) Concentrated electrolyte solution transport theory: directly measured glass temperatures and vitreous ice. J Phy Chem 71:2759–2761 Patil SP, Mehrotra SC (1995) Dielectric Relaxation of Glycerol and Glycerol/Water Mixtures Nam YS, Park WH, Ihm D, Hudson SM (2010) Effect of the degree of deacetylation on the thermal decomposition of chitin and chitosan nanofibers. Carbohydr Polym 1:291–295. https://doi.org/10.1016/j.carbpol.2009.11.030 Hazrati KZ, Sapuan SM, Zuhri MYM, Jumaidin R (2021) Effect of plasticizers on physical, thermal, and tensile properties of thermoplastic films based on Dioscorea hispida starch. Int J Biol Macromol 185:219–228. https://doi.org/10.1016/j.ijbiomac.2021.06.099 Suppakul P, Chalernsook B, Ratisuthawat B, Prapasitthi S, Munchukangwan N (2013) Empirical modeling of moisture sorption characteristics and mechanical and barrier properties of cassava flour film and their relation to plasticizing–antiplasticizing effects. LWT - Food Sci Technol 1:290–297. https://doi.org/10.1016/j.lwt.2012.05.013 Muscat D, Adhikari B, Adhikari R, Chaudhary D (2010) Comparative study of film forming behavior of low and high amylose starches using glycerol and xylitol as plasticizers. J Food Eng 2:189–201. https://doi.org/10.1016/j.jfoodeng.2011.10.019 Mangaraj S, Goswami TK, Mahajan PV (2009) Applications of plastic films for modified atmosphere packaging of fruits and vegetables: a review. Food Eng Rev 1:133–158. https://doi.org/10.1007/s12393-009-9007-3 Sanyang ML, Sapuan SM, Jawaid M, Ishak MR, Sahari J (2016) Effect of plasticizer type and concentration on physical properties of biodegradable films based on sugar palm (arenga pinnata) starch for food packaging. J Food Sci Technol 1:326–336. https://doi.org/10.1007/s13197-015-2009-7) Liu X, Zhang T, Pang K, Duan Y, Zhang J (2016) Graphene oxide/cellulose composite films with enhanced UV-shielding and mechanical properties prepared in NaOH/urea aqueous solution. RSC Adv 77:73358–73364. https://doi.org/10.1039/C6RA16535D Wu H, Lei Y, Lu J, Zhu R, Xiao D, Jiao C, Li M (2019) Effect of citric acid induced crosslinking on the structure and properties of potato starch/chitosan composite films. Food Hydrocolloids 97:105208. https://doi.org/10.1016/j.foodhyd.2019.105208 Additional Declarations No competing interests reported. Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6343422","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":471712674,"identity":"a1da4971-a9b3-4faf-8a66-36cd12b56a56","order_by":0,"name":"Ngesa Ezekiel Mushi","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA8UlEQVRIiWNgGAWjYHACNoYECIPxAZBNmhZmA7iWA4S0wBgSRGnRnZH+7MEDhjt2/fyHn1XzlNVFM7AffsD84Q9uLWY3cswNEhieJc+ckWZ2m+fc4dwGnjQDhgM8eLWwSSQwHE42uMFgdpu37UBuA0MO0GES+LSkPwNrsT9//Fsxb1tdbgP/G6AWA3xaEsxAWuwMGHLMmHnbmHMbJEC2JODRcuYNUIvB4QSJGznFknOAfmmTeGZw4MwBPFqOpz+T/FFx2J6///jGD2/K6nL7+ZMfPqjAE2IQYMCQ2ABjg6IGjx0IYE+MolEwCkbBKBihAADBz1I8A5qrEAAAAABJRU5ErkJggg==","orcid":"","institution":"University of Dar es Salaam","correspondingAuthor":true,"prefix":"","firstName":"Ngesa","middleName":"Ezekiel","lastName":"Mushi","suffix":""},{"id":471712675,"identity":"f3125410-e708-42f0-a2e3-ceeda713b80f","order_by":1,"name":"Cosmas Fednand Kindole","email":"","orcid":"","institution":"University of Dar es Salaam","correspondingAuthor":false,"prefix":"","firstName":"Cosmas","middleName":"Fednand","lastName":"Kindole","suffix":""},{"id":471712676,"identity":"80c9302b-e532-4652-ac4f-62ec16915944","order_by":2,"name":"Neema Msuya","email":"","orcid":"","institution":"University of Dar es Salaam","correspondingAuthor":false,"prefix":"","firstName":"Neema","middleName":"","lastName":"Msuya","suffix":""}],"badges":[],"createdAt":"2025-03-31 09:23:22","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6343422/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6343422/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":84917651,"identity":"a6be21a3-c84a-49bc-834d-769930624090","added_by":"auto","created_at":"2025-06-18 19:02:35","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":465087,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Photographic images demonstrating the DeChNFs from crab shells, Carrageenan from edible seaweeds, \u0026nbsp;and honey from matured bees. (b) A flowchart of the plasticized DeChNF films preparation through casting.\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/110f0900c8e7ad4c8343ec9f.png"},{"id":84917652,"identity":"c7091f7c-644e-461c-be66-7d719d855c83","added_by":"auto","created_at":"2025-06-18 19:02:35","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":904358,"visible":true,"origin":"","legend":"\u003cp\u003eDeChNF plasticized film properties are (a) measured density and (b) film thickness. FTIR spectra for \u0026nbsp;DeChNF plasticized films (c), G-plasticized films (d), C-plasticized films (e), H-plasticized films, and (f) \u0026nbsp;XRD curve for G20, H20, and C20-plasticized films.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/71ad734da1aeaf5c783fdbd2.png"},{"id":84917655,"identity":"51e25179-b363-48e9-a473-3a258320fe12","added_by":"auto","created_at":"2025-06-18 19:02:36","extension":"jpeg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":1062958,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Digital images of the DeChNF plasticized films prepared using different plasticizer types and concentrations.\u003cstrong\u003e \u003c/strong\u003e(b\u003cstrong\u003e)\u003c/strong\u003e Regular light transmittance of the DeChNF plasticized films.\u003c/p\u003e","description":"","filename":"floatimage3.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/fcf2196c2cea6872df9383ca.jpeg"},{"id":84917654,"identity":"70cc0b03-4fad-4822-82e7-1f62ff14b499","added_by":"auto","created_at":"2025-06-18 19:02:35","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":805605,"visible":true,"origin":"","legend":"\u003cp\u003eDSC curve for DeChNF plasticized film (a), G-plasticized DeChNF film (b), H-plasticized DeChNF film \u0026nbsp;(c), and C-plasticized DeChNF film (d), and the bar chart of the relationship of the relaxation temperature \u0026nbsp;and plasticizer content and plasticizer type.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/9c9e52cb734c0d852241533c.png"},{"id":84917658,"identity":"a522b1c4-ea1a-4abe-810b-79cbc40b602b","added_by":"auto","created_at":"2025-06-18 19:02:36","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":4891518,"visible":true,"origin":"","legend":"\u003cp\u003eStress-strain curve for DeChNF-plasticized films; (a) G-plasticized, (b) C-plasticized, (c) H-plasticized, (d) \u0026nbsp;Bar charts of tensile modulus, (e) tensile strength, and (f) tensile strain to failure data for plasticized films.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/743ca937a4573e0e242a905c.png"},{"id":84918173,"identity":"79a9f5d7-20f2-40b2-8ff7-9f794b05410f","added_by":"auto","created_at":"2025-06-18 19:18:36","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":441818,"visible":true,"origin":"","legend":"\u003cp\u003eDeChNF plasticized film water interaction properties: (a) MC, (b) WAC, and (c) WVP.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/64adec9274a11ff1ffcc998f.png"},{"id":84918595,"identity":"6ecd8a8b-69e3-4051-99c2-937327db2c11","added_by":"auto","created_at":"2025-06-18 19:26:41","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":9022683,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6343422/v1/14e5f724-6c99-4549-a66c-19ddb3499adc.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Strong and Transparent Deacetylated Chitin Nanofibril Films using Bees’ Honey and Carrageenan as Potential Plasticizers in Packaging","fulltext":[{"header":"Introduction","content":"\u003cp\u003eAs interest in biopolymers grows, shifting from petroleum-based plastics to renewable and biodegradable polymer materials becomes essential. In 2014, global plastic production was estimated at 311\u0026nbsp;million tons [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e], and projections indicate that this figure could quadruple by 2050 [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e], showing the need for sustainable alternatives. Biopolymers offer versatile properties that rival traditional plastics, including excellent mechanical and barrier characteristics [\u003cspan additionalcitationids=\"CR4\" citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]. In addition, they are abundant and non-toxic, making them an appealing choice for eco-friendly materials [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e, \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e]. Biopolymer films for packaging have been developed from chitosan [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e] gelatin [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e], carboxymethyl cellulose [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e], hydroxypropyl methylcellulose [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e], cellulose acetate [\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e], ethyl cellulose [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e], starch [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e], xyloglucan [\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e, \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e], and cellulose nanofibrils [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e, \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]. Unlike cellulose, chitin nanofibril-based films demonstrate novel properties that have not been extensively investigated.\u003c/p\u003e \u003cp\u003eBeing the second most abundant polysaccharide after cellulose [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e], chitin is a promising resource for sustainable packaging. It is primarily obtained as waste from marine industries and is biosynthesized through the action of chitinase enzymes, with monomers of N-acetyl-D-glucosamine linked by β-1-4 bonds. Individual chitin nanofibrils (ChNFs) can be extracted from invertebrates such as crabs, shrimp, squid pens, lobster shells, insect cuticles, and fungi [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e, \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e]. Approximately 47\u0026nbsp;million tons of chitin from seafood waste are discarded yearly, with 6\u0026ndash;8\u0026nbsp;million tons either dumped or buried in landfills [\u003cspan additionalcitationids=\"CR21\" citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]. To fully harness the potential of chitin from waste, it is crucial to control its mechanical properties.\u003c/p\u003e \u003cp\u003eBiological ChNFs form strong and tough nanostructured materials with exceptional properties that make them suitable for various applications, including composites, textiles, tissue engineering, biomedicine, and pharmaceuticals [\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]. The unique mechanical characteristics of ChNFs stem from their α-type extended polymer conformation and long-range crystallinity with a swirled morphology, making them remarkably strong and stiff [\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. Research indicates that ChNFs with a degree of acetylation (DA) of around 70\u0026ndash;74% are classified as deacetylated chitin nanofibrils (DeChNF) [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. These DeChNFs, considered partially deacetylated, retain their extended chitin crystal core at higher DA levels [\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e, \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. Films made from DeChNFs are highly transparent and can form stable hydrocolloid networks, enhancing film formation compared to native ChNFs [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]. The DA significantly correlates to mechanical properties, and lower DA contributes to good tensile strain to failure and antibacterial properties through increased amino-active sites on the surface [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e, \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]. However, pure DeChNF films can be brittle, fragile, and challenging [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. These films may crack easily when dried or folded under ambient conditions due to strong intermolecular hydrogen bonding from capillary condensation, which creates permanent nanofibril bonds during drying. This brittleness limits the broader applicability of DeChNF films, particularly in packaging.\u003c/p\u003e \u003cp\u003ePlasticization has been employed to improve the properties of deacetylated ChNF-based films and create flexible, strong, and transparent films [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. The addition of plasticizers disrupts intermolecular forces by sitting in between the polymer chains [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. As a result, it softens the film structure and enhances the mobility of the polymer chains. Glycerol has proven to be an effective plasticizer, increasing the flexibility of chitosan films while being biocompatible [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. It also improves the mechanical properties and reduces the brittleness of native DeChNF films [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. In contrast, incorporating chitosan into the ChNF films enhances their toughness and strength, for example, chitosan with a 10 wt. % ChNF loading fraction boosted the tensile strength to 98 MPa, with a tensile strain at failure of 46% and work of fracture at 35 MJ/m\u0026sup3; [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. These mechanical data are excellent because of the unique interactions between the small-diameter nanofibrils and chitosan. Chitosan, a deacetylated chitin derivative and cationic polyelectrolyte, stabilizes the hydrocolloid suspension, which is essential for good mechanical properties. On the other hand, glycerol-plasticized ChNF films demonstrate lower mechanical properties, achieving tensile strength of 40 MPa and tensile strain to failure of 18% at a higher ChNF loading fraction of 50 wt. % [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. In another study, chitosan enhanced ChNF quality, taking advantage of the compatibility and electrostatic interactions between the chitosan polymer and ChNF [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]. For example, the combination of ChNFs with a 4 wt.% residual chitosan matrix resulted in an ultimate strength of 187.2 MPa and work of fracture measured at 12.1 MJ/m\u0026sup3;, owing to the more favorable failure mechanisms compared to neat ChNF films [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]. Based on existing literature regarding chitosan and glycerol, controlling the mechanical properties of DeChNF films through plasticization appears promising and could enhance their practical applications. However, limited information is available about DeChNF plasticized wrapping films that utilize food-grade resources for packaging. Moreover, the preparation of chitosan or glycerol utilizes many chemicals that are not environmentally friendly and may be expensive.\u003c/p\u003e \u003cp\u003eHoney, known for its unique properties and high biocompatibility, is a promising plasticizer for DeChNF films. It is highly hydrophilic, with a 17\u0026ndash;18% moisture content due to its natural composition of sugars, proteins, minerals, and antioxidants [\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e]. Honey exhibits anti-inflammatory, antioxidant, and antimicrobial properties, making it an excellent candidate for packaging [\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. Previous studies reported that DeChNF-honey films prepared through casting demonstrated a tensile strength of 21.32 MPa and a strain failure of 6.5% with 35 wt. % honey [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. Though these films exhibited good flexibility for wrapping and tomatoes coated with DeChNF-honey maintained quality for up to 20 days, there is no detailed understanding of the effect of honey on the properties, including mechanical, of the DeChNF films.\u003c/p\u003e \u003cp\u003eCarrageenan, a natural polysaccharide extracted from edible red seaweed, also shows potential as a plasticizer for DeChNF films. It comprises a sulfated galactan backbone alternating 3-linked and 4-linked D-galactopyranose units [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e, \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. Carrageenan is an abundant and renewable biopolymer with excellent gelling, stabilizing, plasticizing, antimicrobial, and film-forming properties [\u003cspan additionalcitationids=\"CR38 CR39\" citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]. Despite its unique characteristics, little is known about its effectiveness as a plasticizer for DeChNF films.\u003c/p\u003e \u003cp\u003eWhile the literature on using natural honey or carrageenan as plasticizing agents to modify the mechanical properties of DeChNF films is sparse, previous research suggests that honey-plasticized DeChNF films can extend the postharvest shelf life of tomatoes more effectively than unmodified DeChNF films, which is attractive in packaging [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. The flexibility of films containing 35% honey allowed for multiple wrapping and unwrapping of tomatoes over a 20-day storage period. Furthermore, prior studies have indicated that the toughness and strength of DeChNF films could be enhanced by incorporating glycerol as a plasticizer [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e] or by blending with chitosan [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]. However, the effects of plasticization using these food-sourced materials have not been thoroughly investigated. The current study explores using carrageenan and honey from food-grade resources as plasticizers. In addition to reviewing published literature, the study compares their effectiveness with glycerol in reducing the mechanical brittleness of DeChNF films. The primary objective is to improve our understanding of the mechanical potential of DeChNF films as novel nanomaterials. Ultimately, this research aims to contribute to developing fully biodegradable and eco-friendly films, offering alternatives to petroleum-based polymer materials for postharvest food technologies.\u003c/p\u003e"},{"header":"Experimental","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003eMaterials\u003c/h2\u003e \u003cp\u003eDeChNF was prepared from crab shell wastes (\u003cem\u003ePortunus Pelagius\u003c/em\u003e) purchased from the Kigamboni fish market in Dar es Salaam, Tanzania. The edible red seaweed for carrageenan extraction was purchased from local producers in Zanzibar. The DA of DeChNF was 68.2%. Glycerol was purchased from Loba Chemie Ltd in India and used as received. Matured bees (non-stingless) honey harvested from \u003cem\u003eApis Mellifera Scutellata\u003c/em\u003e in the Kigosi-Moyowosi game reserve was purchased from local vendors in Dar es Salaam. The chemicals, such as hydrochloric acid, sodium hydroxide, ethanol, and acetic acid, were purchased from Loba Chemie PVT LTD in India.\u003c/p\u003e \u003c/div\u003e\n\u003ch3\u003eDeChNF and carrageenan preparation\u003c/h3\u003e\n\u003cp\u003eFollowing the method described by Mushi et al. [\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e], the raw crushed crab shells were treated with 2 M of HCl for demineralization at room temperature. Then, the shells were washed with deionized water to a neutral pH. The sample was decolorized by treating it with ethanol under constant stirring overnight. Next, the deproteinization was done based on the method developed by Fan et al. [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e], with a few modifications. First, the samples were deproteinized and deacetylated by treatment with 33% NaOH at 100 ℃ for 4 h. Then, the sample was washed several times with deionized water until it reached a neutral pH. The deacetylated chitin was dispersed in aqueous acetic acid (pH 3\u0026ndash;4) and stirred overnight for mechanical disintegration. The sample was then passed through a kitchen blender (Vitamix, USA) at 1500 rpm and repeated thrice. The degree of deacetylation of the thus obtained DeChNFs was 32.8%. Carrageenan extraction was performed as previously described by Dong \u003cem\u003eet al.\u003c/em\u003e [\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e] with slight modifications. Essentially, 100 g of wet red seaweed sample was weighed and soaked in distilled water (2L) for 1 hr. at 80\u0026deg;C using a hot plate magnetic stirrer to remove the skin pigment on the surface. Then, seaweed biomass was washed with distilled water and collected. The obtained samples were refluxed in 8% NaOH solution (27 mL of NaOH per gram of seaweed biomass) and shaken (500 rpm) at 80\u0026deg;C for 2 h using a magnetic stirrer. After cooling, the solution was stored in a non-dried state for further use.\u003c/p\u003e\n\u003ch3\u003ePreparation of DeChNF plasticized films\u003c/h3\u003e\n\u003cp\u003eThe plasticized DeChNF film was prepared from the DeChNF, carrageenan gel, and bee honey shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea. The preparation procedures are described in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb. Initially, 1 wt. % aqueous dispersion of DeChNF was prepared. Next, different plasticizers were added into the dispersions at 0, 5, 20, 35, and 65 wt\u0026mdash;%, as described in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, based on the dry weight of DeChNF. The film-forming solutions were blended in the kitchen blender (Vitamix 5200, USA) for 2 min and treated with a super stirrer (MX-S401 S, China) to mix homogeneously for 1 hour at room temperature. After one hour, the mixtures were degassed to remove air from bubbles for 30 minutes before casting in glass Petri dishes. The mixtures were poured into glass Petri dishes coated with a release agent and dried in ambient conditions (50\u0026deg;C, 24 hours) to allow evaporation. All films were prepared in triplicate, including films without plasticizers used as controls. After 24 h of drying, films were peeled from the casting surfaces and stored in desiccators with 53\u0026thinsp;\u0026plusmn;\u0026thinsp;1% relative humidity (RH).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eFormulation of plasticizer in the preparation of plasticized DeChNF film\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"3\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eSample\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003ePlasticizer type\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003ePlasticizer concentration (%)\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e0\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e35\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG65\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e65\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e35\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH65\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e65\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e35\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC65\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e65\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e\n\u003ch3\u003eCharacterization of the DeChNF plasticized films\u003c/h3\u003e\n\u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003eDetermination of DeChNF plasticized film thickness\u003c/h2\u003e \u003cp\u003eThe thickness of the produced samples was measured using a digital micrometer (Mitutoyo Co., Kawasaki, Japan) with 0.001 mm accuracy. The thickness measurement of each film sample was replicated five times at different areas of the film, and the mean value of the film\u0026rsquo;s thickness was calculated. The density of ChNF films was determined by measuring their dimensions and air-dried weight.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003eFourier Transform Infra-Red (FTIR) Spectroscopy and DA conductometric titration\u003c/h2\u003e \u003cp\u003eThe surface functional groups of the control and the DeChNF plasticized films were studied through IR spectra recorded using a Spectrum 2000 FTIR spectrophotometer (Perkin-Elmer Inc., USA) equipped with an attenuated total reflectance crystal accessory (Golden Gate). All samples were scanned in the range of 400\u0026ndash;4000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. A total of 64 scans with a wavelength resolution of 4 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e were performed on each sample. The spectra were interpreted using the frequency assignment approach. As reported in previous work, the DA of the ChNFs was measured using the conductometric titration method [\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e].\u003c/p\u003e \u003c/div\u003e\n\u003ch3\u003eX-ray Powder Diffraction (XRD)\u003c/h3\u003e\n\u003cp\u003eThe X-ray Powder Diffraction (XRD) patterns were employed to analyze the α-chitin crystalline structure. The data were\u0026nbsp;collected in the 2θ range of 5\u0026thinsp;\u0026minus;\u0026thinsp;40\u0026deg; using an X-ray diffractometer (Rigaku Co., Ltd., South Africa) with Cu Kα radiation (λ\u0026thinsp;=\u0026thinsp;1.5418 \u0026Aring;) at 40 kV and 40 mA. The diffractograms were curve-fitted in Origin software to obtain the crystallinity index.\u003c/p\u003e\n\u003ch3\u003eRegular Light Transmittance Spectrophotometry\u003c/h3\u003e\n\u003cp\u003eThe films' light transmittance was measured using an Analytikjena SPECORD 210 PLUS UV-Vis spectrophotometer (UV-2550, Shimadzu, Japan). The wavelengths from 200 to 900 nm were scanned. The transmittance spectra were recorded at room temperature, with air as a reference.\u003c/p\u003e \u003cdiv id=\"Sec11\" class=\"Section2\"\u003e \u003ch2\u003eDifferential Scanning Calorimetry (DSC)\u003c/h2\u003e \u003cp\u003eThe film samples were conditioned (65% \u0026plusmn; 1% for 24 h) before analyses using the DSC model Universal V3-9A TA Instrument, made in New Castle, USA. The calibration of the equipment was conducted using indium as a standard. For DSC analyses, 5 mg of film samples were weighed, placed in an aluminum sample pan, and immediately sealed. An empty sample pan was used as a reference. Film samples were heated from 0 to 400\u0026deg;C at 10\u0026deg;C/min. Nitrogen gas was used to flush the DSC cell at a 20 mL/min flow rate to maintain an inert environment. The transition temperatures were determined from the thermogram results.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec12\" class=\"Section2\"\u003e \u003ch2\u003eTensile Properties Measurement\u003c/h2\u003e \u003cp\u003eThe tensile test was conducted using the method previously used by Mushi et al. [\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e] with a few modifications. The tensile properties of the control and the plasticized films were studied from 5 specimens. The specimens were cut into a width\u0026thinsp;=\u0026thinsp;5 mm and a length\u0026thinsp;=\u0026thinsp;20 mm, then conditioned at 20℃ overnight. The uniaxial deformation test was performed using a Universal tensile testing machine (Instron, UK) with a crosshead speed of 2 mm/min and a load cell of 10 kN to obtain tensile modulus, tensile strength, and tensile strain to failure.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec13\" class=\"Section2\"\u003e \u003ch2\u003eDetermination of the Moisture Content and Water Absorptive Capacity\u003c/h2\u003e \u003cp\u003eThe film samples' moisture content (MC) was determined by weighing each sample (Wi) using a digital scale. The samples were then dried in an oven at 105\u0026deg;C for 24h and reweighed (W\u003csub\u003ef\u003c/sub\u003e), and the MC was calculated using Eq.\u0026nbsp;(1) [\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e]. The test was carried out in triplicate, and the final MC for each film was recorded as the mean of the results.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec14\" class=\"Section2\"\u003e \u003ch2\u003eMC =\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\:\\:\\frac{Wi-Wf}{Wi}\\times\\:100\\)\u003c/span\u003e\u003c/span\u003e (1)\u003c/h2\u003e \u003cp\u003eThe film's water absorption capacity (WAC) was determined according to Pereda and Norma [\u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e] with minor modifications. The water sorption capacity of each film was studied by immersing a known mass (Wd) of the film sample into distilled water at room temperature (23\u0026thinsp;\u0026plusmn;\u0026thinsp;2\u0026deg;C). The Film was periodically removed from the distilled water and reweighed until a constant film mass (Ww) was attained. The test was performed in triplicate. The water uptake was determined using Eq.\u0026nbsp;(2).\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec15\" class=\"Section2\"\u003e \u003ch2\u003eWAC =\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\:\\:\\frac{Ww-Wd}{Wd}\\times\\:100\\)\u003c/span\u003e\u003c/span\u003e (2)\u003c/h2\u003e \u003cdiv id=\"Sec16\" class=\"Section3\"\u003e \u003ch2\u003eDetermination of Water Vapor Permeability\u003c/h2\u003e \u003cp\u003eBefore the water vapor permeability (WVP) test, the film samples were conditioned in a desiccator with a relative humidity of 50% at 25\u0026deg;C. The WVP test was conducted using the method described by Pereda \u003cem\u003eet al.\u003c/em\u003e [\u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e] with minor modifications. The films were cut into rectangular shapes (7.5 cm x 7.5 cm) and then mounted and sealed on the open mouth of cylindrical cups containing 20 g of calcium chloride. The test cups were measured before being kept in a relative humidity chamber (25\u0026deg;C, relative humidity 75%). The weight of the test cups was determined by periodic measurement till the equilibrium state was reached. Weight increments of the test cups were recorded, and WVP was calculated using Eq.\u0026nbsp;(3).\u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec17\" class=\"Section2\"\u003e \u003ch2\u003eWVP=\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\:\\:\\frac{m\\:\\times\\:\\:d}{A\\:\\times\\:t\\:\\times\\:\\:P}\\times\\:100\\)\u003c/span\u003e\u003c/span\u003e (3)\u003c/h2\u003e \u003cp\u003eWhere m (g) is the weight increment of the test cup, d (mm) is the film thickness, A (m\u003csup\u003e2\u003c/sup\u003e) is the area of film exposed, t (s) is the duration for permeation, and P (Pa) is the water vapor partial pressure across the films. The results were expressed in g\u0026middot;mm\u0026middot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e \u0026middot;m\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e \u0026middot;Pa\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e.\u003c/p\u003e \u003c/div\u003e"},{"header":"Results and Discussion","content":"\u003cdiv id=\"Sec19\" class=\"Section2\"\u003e \u003ch2\u003ePhysical properties of the plasticized DeChNF films\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea shows the thickness of the plasticized DeChNF films. It was observed that the film thickness increased from 0.041 to 0.074 mm, 0.054 to 0.105 mm, and 0.052 to 0.097 mm with concentrations of G, H, and C, respectively. The film thickness increased as the plasticizer concentration increased from 5 to 65%, regardless of plasticizer type. Films with H were thicker than those plasticized with C and G. Moreover, the type of plasticizer significantly influences film thickness, indicating a sign of interfacial interactions between the plasticizers and DeChNFs. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb shows the effect of plasticizer type and concentration on the density of DeChNF films plasticized with different ratios of plasticizers. The addition of plasticizers reduced the density of native DeChNF (1.24 g/cm\u003csup\u003e3\u003c/sup\u003e). All the plasticized films exhibit lower density than the control DeChNF film. Increasing the concentration of plasticizers from 5 to 65 % causes a slight decrease in the density of G-(1.173\u0026thinsp;\u0026minus;\u0026thinsp;1.112 g/cm\u003csup\u003e3\u003c/sup\u003e), H- (1.193\u0026thinsp;\u0026minus;\u0026thinsp;1.154g/cm\u003csup\u003e3\u003c/sup\u003e), and C-plasticized films (1.153\u0026thinsp;\u0026minus;\u0026thinsp;1.127 g/cm\u003csup\u003e3\u003c/sup\u003e). According to Jouki \u003cem\u003eet al.\u003c/em\u003e [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e], an increase in glycerol content from 25\u0026ndash;50% for cress seed gum (CSG) edible films led to a notabe increase in film thickness, from 0.067 mm to 0.079 mm. Likewise, the density values decreased from 1.26 g/cm\u003csup\u003e3\u003c/sup\u003e at 25% to 1.22 g/cm\u003csup\u003e3\u003c/sup\u003e at 50% glycerol [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e]. Tarique et al. [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e] observed a decrease in film density for arrowroot (\u003cem\u003eMaranta arundinacea)\u003c/em\u003e starch films with 15, 30, and 45% glycerol, as observed in DeChNF plasticized films. The higher thickness of H-plasticized film may be related to honey's unique complex molecular composition, which includes a mixture of sugars. In contrast, glycerol is a small, simple molecule of trihydroxy alcohol that penetrates the network of chitin easily. While forming a strong gel-like network, carrageenan does not create a denser network than honey. Increasing film thickness can be attributed to the role of plasticizers in disrupting and restructuring intermolecular polymer chain networks [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]. Percent-wise, the current data demonstrate a much more significant change in thickness.\u003c/p\u003e \u003cp\u003eThe FTIR spectra of both unplasticized and plasticized DeChNF films are presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec-e. The spectral peak conforms to intra- and intermolecular O-H stretching at 3444 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, while the peaks at 3245 and 3100 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e are associated with the N-H stretching band [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e, \u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e, \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]. The doublets observed at 1654 cm⁻\u0026sup1; and 1621 cm⁻\u0026sup1; correspond to amide I (C\u0026thinsp;=\u0026thinsp;O stretching). The amide II band (N\u0026ndash;H bending) is present at 1554 cm⁻\u0026sup1;, along with the amide III band (C\u0026ndash;N stretching) at 1310 cm⁻\u0026sup1; [\u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e, \u003cspan citationid=\"CR51\" class=\"CitationRef\"\u003e51\u003c/span\u003e]. These spectral peaks characterize the α-chitin in the DeChNFs material. The frequency shift of the broad bands of hydroxyl functional groups in DeChNF indicates the presence of hydrogen bonding between DeChNF and the plasticizers. The peaks around 2950 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e are attributed to C-H aliphatic absorption peaks, and the characteristic peaks at 1004 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e are assigned to the C-O bond stretching of C-O-C groups in the anhydrous-glucose ring of DeChNF. These results from the FTIR analysis provide valuable insights into the molecular interactions in the films, highlighting the complex interplay between chitin and plasticizers. In essence, the interactions are primarily dominated by physical bonding between the nanofibrils and the plasticizers. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef presents XRD patterns of DeChNF films plasticized with 20 wt. % of glycerol, honey, and carrageenan. All the plasticized nanofilms retained the α-chitin structure, as indicated by the four sharp crystalline reflections at 2ϴ = 9.3, 12.6, 19.3, and 26.4, corresponding to the (020), (021), (110), and (013) lattice planes [\u003cspan citationid=\"CR52\" class=\"CitationRef\"\u003e52\u003c/span\u003e, \u003cspan citationid=\"CR53\" class=\"CitationRef\"\u003e53\u003c/span\u003e]. The X-ray diffraction patterns of unplasticized DeChNF films are similar to those of G-plasticized, H-plasticized, and C-plasticized films, indicating that plasticization did not affect the chitin crystal structure, in support of the FTIR mentioned above.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec20\" class=\"Section2\"\u003e \u003ch2\u003eRegular light transmittance of the plasticized DeChNF films\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea presents photographic images of free-standing films prepared from deacetylated chitin nanofibers (DeChNF) with varying ratios of plasticizers, while Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e outlines their visual characteristics. Notably, free-standing DeChNF plasticized films were successfully obtained even at higher concentrations of plasticizers. In contrast, DeChNF films without plasticizers appeared wavy, brittle, semi-rigid, and fragile. This phenomenon can be attributed to the strong inter- and intramolecular hydrogen bonds within DeChNF due to the capillary condensation, common during the drying process, which restricts the mobility of the macromolecular chains and leads to brittle and semi-rigid films. The addition of plasticizers to the DeChNF films enhanced their flexibility and smoothness. Among the tested films, those with 65% plasticizer content exhibited the greatest flexibility, while flexibility decreased as the amount of plasticizer was reduced, regardless of its type. Among all plasticized DeChNF films, those with honey (H65) were particularly flexible but weak and highly sticky, making them difficult to peel off the petri dish (data not shown here). This stickiness is attributed to honey's complex, sugary constituents, which become more pronounced at higher concentrations. In contrast, films with glycerol and carrageenan were easier to peel off due to the more effective incorporation of these plasticizers within the intermolecular spaces of the DeChNF. This integration strengthens the cohesive nature of the chitin molecules, contributing to the easier peeling of the glycerol- and carrageenan-plasticized films. Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb displays the regular light transmittance spectra for a series of plasticized DeChNF films. The transmittance of the deacetylated ChNF film without plasticizer was found to be 84.9% at 800 nm. In comparison, films with 20 wt% plasticizers \u0026mdash; G20, H20, and C20 \u0026mdash; showed approximate transparency values of 87.8%, 83.6%, and 85.4%, respectively. Light transmittance measured using a UV-Vis spectrophotometer allows for comparing the transparency of different films over a wide spectrum. The plasticizers' smaller molecular size, i.e., glycerol, likely enhances molecular interactions, reducing voids within the DeChNF matrix and creating a more homogeneous structure that minimizes light scattering.\u003c/p\u003e \u003cp\u003eWhile the refractive index values are essential to increase understanding, this data was inferred rather than directly measured. Research on transparent wood showed that transparency depends on the similarity in refractive indices among constituents such as cellulose nanofibrils, methyl methacrylate, and styrene monomers [\u003cspan citationid=\"CR54\" class=\"CitationRef\"\u003e54\u003c/span\u003e]. According to the literature, the refractive index of glycerol is approximately 1.472 [\u003cspan citationid=\"CR55\" class=\"CitationRef\"\u003e55\u003c/span\u003e], DeChNF ranges from 1.56 to 1.58 [\u003cspan citationid=\"CR56\" class=\"CitationRef\"\u003e56\u003c/span\u003e], carrageenan varies between 1.33 and 1.45 [\u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e57\u003c/span\u003e], and honey ranges from 1.488 to 1.504 [\u003cspan citationid=\"CR58\" class=\"CitationRef\"\u003e58\u003c/span\u003e]. These values can change based on moisture content, crystallinity, polymer conformation, nanofibril size, processing methods, and composition. Therefore, combining glycerol, honey, or carrageenan with DeChNF likely facilitates effective matching, leading to minimized light scattering at interfaces. As such, all films exhibited high transmittance regardless of plasticizer content. The low transparency of honey-plasticized films remains to be investigated.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab2\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 2\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eAppearance of unplasticized and plasticized DeChNF films\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"3\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eSample\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003ePlasticizer type\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAppearance of the films\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, brittle, and fragile, rigid surface cracks\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, slightly sticky/tacky, slightly difficult to peel\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eG65\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eGlycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, sticky/tacky, slightly difficult to peel\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, slightly sticky/tacky, slightly difficult to peel\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eH65\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eHoney\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, highly sticky/tacky, difficult to peel\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, rigid, no surface cracks, flexible, not sticky/tacky, peelable\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, not sticky/tacky, peelable\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, no surface cracks, flexible, slightly sticky/tacky, slightly difficult to peel\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC65\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCarrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTransparent, not brittle and fragile, not rigid, no surface cracks, flexible, sticky/tacky, slightly difficult to peel\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec21\" class=\"Section2\"\u003e \u003ch2\u003eDSC of the DeChNF-plasticized films\u003c/h2\u003e \u003cp\u003eThe DSC curves are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea-c, and a bar chart of the relaxation temperatures with plasticizer type and content is summarized in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed. An initial endothermic peak is observed between temperatures (T\u003csub\u003e1\u003c/sub\u003e) 40\u0026ndash;80\u0026deg;C (highlighted in yellow) for both the control DeChNF and the plasticized films. The endothermic peak for the glycerol-plasticized DeChNF films (G5) is less pronounced than those plasticized with honey and carrageenan. At elevated temperatures, a significant exothermic peak appears between temperatures (T\u003csub\u003e2\u003c/sub\u003e) 300\u0026ndash;370\u0026deg;C (also highlighted in yellow) for both the control and plasticized films. Notably, there is a shift in the relaxation temperature towards lower values as the plasticizer content increases. For the control DeChNF films, which have a transition temperature of around 365\u0026deg;C, the relaxation temperature shifts dramatically to 301\u0026deg;C for the honey-plasticized films. By comparison between the plasticized films, the trend in the relaxation behavior closely matches that observed in films at lower temperatures. Based on the relaxation trend, a more substantial plasticization effect appears to be associated with honey, followed by glycerol, and finally, carrageenan. This could be due to the disrupted film structure and thus plasticization, which is noteworthy.\u003c/p\u003e \u003cp\u003eAccording to literature data [\u003cspan citationid=\"CR59\" class=\"CitationRef\"\u003e59\u003c/span\u003e], chitin has a relaxation temperature of around 60\u0026ndash;100\u0026deg;C, which is sensitive to its moisture content and degree of crystallinity. The composition of honey is complex, and its relaxation temperature is not clearly defined. However, softening temperatures range between \u0026minus;\u0026thinsp;51\u0026deg;C and \u0026minus;\u0026thinsp;33\u0026deg;C, depending on its water content [\u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e]. Carrageenan exhibits primary relaxation behavior in the 150\u0026ndash;200\u0026deg;C range, with additional secondary relaxations occurring between 60\u0026deg;C and 90\u0026deg;C, depending on carrageenan sulfate content and properties, as well as moisture content [\u003cspan citationid=\"CR61\" class=\"CitationRef\"\u003e61\u003c/span\u003e]. Glycerol undergoes a transition around \u0026minus;\u0026thinsp;94\u0026deg;C [\u003cspan citationid=\"CR62\" class=\"CitationRef\"\u003e62\u003c/span\u003e], with secondary relaxation processes observable in the 10\u0026ndash;30\u0026deg;C range [\u003cspan citationid=\"CR63\" class=\"CitationRef\"\u003e63\u003c/span\u003e], which is also influenced by moisture. When these components are combined, their relaxation behavior becomes more complex and may be affected by the relative ratios and interactions with ChNF at the interfaces. Both DeChNFs, glycerol, honey, and carrageenan can absorb moisture. Since moisture significantly impacts the relaxation temperature, the transition occurring at lower temperatures, around 40\u0026ndash;80\u0026deg;C, may indicate the loss of freely bound water within the films. Additionally, the relaxation temperatures of carrageenan, glycerol, and honey may overlap with water evaporation. Water interaction can be classified based on different states. Water evaporates at lower temperatures, while bound water evaporates at slightly higher temperatures due to its stronger interaction with the materials. The DSC relaxation peak at 365\u0026deg;C in DeChNF can be attributed to molecular relaxation, breaking of hydrogen bonds, and amorphous phase transitions, as complete decomposition occurs at higher temperatures around 400\u0026ndash;450\u0026deg;C [\u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e64\u003c/span\u003e]. Tarique et al. [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e] used a dry processing technique (hot pressing) and observed a reduction in transition temperature from 294.6\u0026deg;C to 291.9\u0026deg;C for starch films plasticized with 15, 30, and 45% glycerol. Similarly, Hazrati et al. [\u003cspan citationid=\"CR65\" class=\"CitationRef\"\u003e65\u003c/span\u003e] observed decreased relaxation temperature in starch films plasticized with 30, 45, and 60% glycerol, sorbitol, and urea, respectively. Thus, the shift in the relaxation temperature of chitin towards lower values reflects increased molecular mobility, which signifies a crucial indication of plasticization.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec22\" class=\"Section2\"\u003e \u003ch2\u003eMechanical properties of the DeChNF-plasticized films\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea-c show the stress-strain curves of the DeChNF films with varying plasticizer contents, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea-c, reveal two distinct deformation behaviors. In pure DeChNF, the elastic deformation is followed by the plastic deformation, resulting in a more developed curve than the films containing plasticizers. As plasticizer content increases, the tensile strain to failure in the plastic region increases. Initially, DeChNF networks dominated the elastic region, with the plasticization effect becoming more pronounced with higher plasticizer content. Consequently, the slope of the elastic region gradually decreases. Apart from other arguments, and by the assumption that the nanofibril dimensions are distributed homogeneously, the molar mass of the plasticizers plays an essential role in controlling strain-hardening behavior in the plastic region. Glycerol, a commercially available plasticizer, displayed the same trend as honey and carrageenan. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed-f, Young\u0026rsquo;s modulus, tensile strength, and strain of DeChNF film without plasticizer were comparatively high, measuring 3.1 GPa, 41.3 MPa, and 8.2%, respectively. The addition of plasticizers from 0\u0026ndash;65% resulted in a significant reduction in the tensile strength of films, regardless of the type of plasticizer used. Nevertheless, for G-plasticized films, tensile strength notably decreased from 41.3 MPa to 6.3 MPa, while for H-plasticized films, it dropped from 41.3 MPa to 4.3 MPa. In the case of C-plasticized films, the tensile strength decreased from 41.3 MPa to 9.4 MPa over the same range of plasticizer concentrations. These reductions correspond to 85%, 90%, and 77%. H-plasticized films showed the highest reduction in tensile strength, at 90%, compared to G- and C-plasticized films. The data on elastic modulus, which indicates the stiffness of materials, is represented in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed. It is evident that the effect of plasticizer concentration (0\u0026ndash;65%) on Young\u0026rsquo;s modulus of DeChNF-plasticized films closely resembles the behavior of their corresponding tensile strength, although different factors govern them. Increasing the plasticizer concentration from 0\u0026ndash;65% led to a noticeable decrease in film stiffness, from 3.1 GPa to 0.7 GPa for G-plasticized films, 3.1 GPa to 0.5 GPa for H-plasticized films, and 3.1 GPa to 1.1 GPa for C-plasticized films. These reduction values corresponded to a 74%, 80%, and 65% decrease in stiffness for G-plasticized, H-plasticized, and C-plasticized, respectively. The effect of plasticizer concentration (0\u0026ndash;65%) on the tensile strain of DeChNF plasticized films is also analyzed. As anticipated, increasing the plasticizer concentration resulted in a considerable increase in film tensile strain from 8.5\u0026ndash;24.74% for G-plasticized films, 8.5\u0026ndash;31.5% for H-plasticized films, and 8.5\u0026ndash;21.65% for CG-plasticized films. The observed mechanical data suggest that the DeChNF matrix is indeed plasticized. The high mechanical properties of the plain DeChNF films can be attributed to the strong hydrogen bonding, which sometimes co-crystallizes, between strong nanofibrils caused by the ambient drying process. DeChNFs derived from crab shells possess an extended-type crystalline structure, contributing to increased stiffness and strength. Moreover, nanofibril-nanofibril interaction controls the strength in the plastic region. The plasticizer disrupts the hydrogen bonds between chitin-chitin nanofibril molecules. As a result, this led to an enhancement in flexibility by allowing greater chain mobility. Although dynamic thermomechanical data on molecular mobility could further support these findings, this study does not present them. Decreasing tensile modulus, strength, and increasing strain to failure have been reported in the literature [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e, \u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e, \u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e, \u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe decrease in tensile strength of DeChNF-based films with plasticizer concentration is a significant observation. Mushi et al. [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e] investigated DeChNF films plasticized with honey (35%) and compared them to films plasticized with glycerol (25%), both prepared through the casting technique. The much higher tensile strength for honey-plasticized DeChNF films (35% concentration, 21.32 MPa) was striking [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. According to Muscat et al. [\u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e67\u003c/span\u003e], tensile strength in starch films decreased with increasing glycerol and xylitol concentrations above 15%. Hazrati et al. [\u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e] focused on starch films with sorbitol and fructose, where 35% sorbitol yielded the highest elongation at break, and 35% fructose yielded the highest tensile strength. Suppakul et al. [\u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e] found that tensile strength vastly decreased with increasing sorbitol concentration while the elongation percentage increased significantly. Here, a low-weight fraction of honey achieves higher strain results. With honey (20 wt%) in DeChNF films, a higher tensile strain (31.5%) was reported compared to glycerol (24.74%), while glycerol (6.3 MPa) showed a higher tensile strength than honey (4.3 MPa) at the same concentration. For the Suppakul et al. [\u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e] results on cassava flour starch films with sorbitol, the present data showed a decrease in tensile strength and an increase in tensile strain (elongation) in DeChNF films with increasing concentrations of glycerol, honey, and carrageenan. Both studies by Muscat et al. [\u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e67\u003c/span\u003e] and Suppakul et al. [\u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e] focused on starch-based films whose commercial applicability is hindered by poor ductility. The higher strength data is intriguing with honey-plasticized DeChNF films (35% concentration, 21.32 MPa) in the literature, suggesting a promising potential for this material. In general, the presented DSC and mechanical data could suffice to demonstrate the effectiveness of the materials studied as plasticizers for controlling the mechanical properties of DeChNF films. Finally, the mechanical properties of the obtained films are comparable to those of significant packaging films, as shown in Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. Although synthetic polymers such as PE, PP, Nylon, PET, and EVOH exhibit higher tensile strain to failure [\u003cspan additionalcitationids=\"CR7 CR8 CR9 CR10 CR11 CR12 CR13 CR14\" citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e, \u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e] than the biopolymeric films, molecular weight and polymer structure differences may account for this disparity.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab3\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 3\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eMechanical properties of the major packaging films\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"5\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePackaging films\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eTensile strength (MPa)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eModulus\u003c/p\u003e \u003cp\u003e(GPa)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eElongation\u003c/p\u003e \u003cp\u003e(%)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eReferences\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF/Glycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e6.3 (0.2)-41.3 (0.4)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.7\u0026ndash;3.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e8.5\u0026ndash;24.7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF/Honey\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e4.3 (0.2)-41.3 (0.4)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.5\u0026ndash;3.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e8.5\u0026ndash;31.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e\u003cb\u003eThis work\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF/Carrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e9.4 (0.3)-41.3 (0.4)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e1.1\u0026ndash;3.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e8.5\u0026ndash;21.7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eChitosan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20.8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e12.7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eGelatin\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e41\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e34\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCarboxymethyl cellulose\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e28\u0026ndash;51\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2\u0026ndash;4\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e65\u0026ndash;91\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eHydroxymethyl methylcellulose\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e38.35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e1.6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e9.40\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCellulose acetate\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e46.56\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e6.8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eEthylcellulose\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e14\u0026ndash;29\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.5-1.0\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e11]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eStarch\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e4.48\u0026ndash;8.14\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.12\u0026ndash;0.29\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e35\u0026ndash;100\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eXyloglucan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e55\u0026ndash;78\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e4.6\u0026ndash;5.4\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.7\u0026ndash;5.7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e14]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCellulose nanofibers\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e42\u0026ndash;175\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e1.5\u0026ndash;15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e15\u0026ndash;50\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolyethylene (PE)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u0026ndash;40\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.2\u0026ndash;1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e100\u0026ndash;700\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolypropylene (PP)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u0026ndash;50\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e1\u0026ndash;2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e200\u0026ndash;600\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolyvinyl chloride (PVC)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e40\u0026ndash;60\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e1\u0026ndash;3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e10\u0026ndash;400\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolyamide (Nylon)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e70\u0026ndash;80\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2\u0026ndash;3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e100\u0026ndash;200\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eEthylene vinyl alcohol (EVOH)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e50\u0026ndash;60\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e3\u0026ndash;4\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e100\u0026ndash;200\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolyethylene Terephthalate (PET)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e50\u0026ndash;70\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2\u0026ndash;3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e50\u0026ndash;150\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cdiv id=\"Sec23\" class=\"Section3\"\u003e \u003ch2\u003e* Data were not reported. The bracket for experimental data indicates the standard deviation\u003c/h2\u003e \u003cdiv id=\"Sec24\" class=\"Section4\"\u003e \u003ch2\u003eWater interaction properties of the plasticized DeChNF films\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea presents the MC of the control and plasticized films. For all plasticized DeChNF films, the moisture content increased significantly as plasticizer concentration increased from 5 to 65%. Generally, DeChNF-based films absorbed more moisture with higher plasticizer concentrations. Several researchers have reported that adding more plasticizers increases the MC of the films [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e, \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e]. Figure\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb presents the WAC of unplasticized and plasticized films when immersed in water. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb, adding plasticizers significantly raised the WAC of the plasticized DeChNF films. At all concentrations, films with C were more water-resistant and less hygroscopic than those with G and H. The increase of plasticizer content had a notable effect on the WAC of the plasticized DeChNF films. The concentration of plasticizers has less influence on the C-plasticized films. This is attributed to the strong hydrogen bonding between the plasticizer and chitin. In addition, a limited solubility of water in carrageenan may contribute. The impact of different plasticizer types and their concentrations on the WVP of DeChNF films is summarized in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ec. The WVP values of plasticized DeChNF films increased with higher plasticizer content. Specifically, the results indicate that increasing the plasticizer concentration from 5\u0026ndash;65% led to WVP values rising from 3.82 \u0026times; 10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e to 8.41 \u0026times; 10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e g\u0026middot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;m\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;Pa\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e for G-plasticized films, from 4.24\u0026times;10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e to 9.17\u0026times;10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e g\u0026middot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;m\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e Pa\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e for H-plasticized films, and from 3.02\u0026times;10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e to 6.78\u0026times;10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e g\u0026middot;s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;m\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e\u0026middot;Pa\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e for C and G-plasticized films. All plasticized films, regardless of the type of plasticizer, exhibited increased WVP values. Among the plasticizers tested in this study, DeChNF film with glycerol (G-plasticized) and honey (H-plasticized) demonstrated the highest WVP values.\u003c/p\u003e \u003cp\u003eFor MC, Jouki et al. [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e] observed an increase with increasing glycerol concentration, from 16.37% at 25% glycerol to 18.78% at 50% glycerol. For WAC, Sanyang et al. [\u003cspan citationid=\"CR69\" class=\"CitationRef\"\u003e69\u003c/span\u003e] observed from the casted films of glycerol, sorbitol or their combination as plasticizers at the ratio of 15, 30, and 45 (wt%) with sugar palm starch (SPS) that the moisture content increased from 7.9\u0026ndash;12.4% for glycerol, 6.6\u0026ndash;8.1% for sorbitol and 11.4\u0026ndash;18.6% for glycerol-sorbitol blend. Tarique et al. [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e] demonstrated in arrowroot starch films plasticized with glycerol (15, 30, and 45 wt. %) that moisture content and solubility in water increased with the glycerol content. For WVP, Muscat et al. [\u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e67\u003c/span\u003e] have reported low WVP in films plasticized by combined plasticizers at a 20% concentration for low and high amylose starch-based films plasticized with glycerol and xylitol. WVP results showed an increased value from 0.55 to 1.34 g mm/m2 h, and the glycerol concentration ranged from 20, 30, and 40 (wt.%). In contrast, the current study observed an increased value of WVP with plasticizer content. An increase in WVP can be attributed to plasticizers modifying the structure of the DeChNF networks.\u003c/p\u003e \u003cp\u003eThe ability of materials to minimize moisture transfer in the surrounding environment is essential for adequate packaging [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]. As such, Table\u0026nbsp;\u003cspan refid=\"Tab4\" class=\"InternalRef\"\u003e4\u003c/span\u003e was developed to compare the WVP of some selected, most common films [\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e] with those from the plasticized DeChNF films. The WVP of materials should be as low as possible, particularly for food packaging. More hydrophobic polymers, mainly derived from fossil-based resources, such as LDPE, HDPE, PVC, PP, and BOPP, exhibit lower WVP, which aligns with expectations. In contrast, because the unique character of biopolymeric materials has strength in the presence of moisture, the higher WVP, or MAC, in that regard, is not surprising but may be attributed to their superior characteristics in the presence of moisture.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab4\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 4\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eWAC and WVP of plasticized DeChNF films and the reference films from the major packaging materials\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"4\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePackaging films\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eWater absorption capacity (g)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eWVP\u003c/p\u003e \u003cp\u003e(\u0026times;10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e g.s\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003em\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e Pa\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eReferences\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF/0\u0026ndash;65%Glycerol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e0.9\u0026ndash;3.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2.84\u0026ndash;8.41\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF/0\u0026ndash;65%Honey\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e1.8\u0026ndash;4.7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2.84\u0026ndash;9.17\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e\u003cb\u003eThis work\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDeChNF/0\u0026ndash;65%Carrageenan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e0.5\u0026ndash;2.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2.84\u0026ndash;6.78\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eChitosan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eGelatin\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e4.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.81\u0026ndash;1.14\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCarboxymethyl cellulose\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2\u0026ndash;4\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eHydroxymethyl methylcellulose\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e4.41\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCellulose acetate\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2.6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eEthylcellulose\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e8\u0026ndash;14\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eStarch\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.12\u0026ndash;0.29\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR65\" class=\"CitationRef\"\u003e65\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003exyloglucan\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.5\u0026ndash;1.9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eLow-density polyethylene (LDPE)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.003\u0026ndash;0.005\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eHigh-density polyethylene (HDPE)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.00125\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolypropylene (PP)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.001-0.00125\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePolyvinyl chloride\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.0075\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBiaxially oriented polypropylene (BOPP)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e0.001-0.00125\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec25\" class=\"Section3\"\u003e \u003ch2\u003e* Data were not reported\u003c/h2\u003e \u003c/div\u003e \u003c/div\u003e"},{"header":"Conclusions","content":"\u003cp\u003eThe DeChNF films, which incorporated glycerol, honey, and carrageenan as plasticizers, were prepared through casting, and their effectiveness on the DeChNF films was examined. The DeChNF films that contained up to 65% w/w of plasticizer content demonstrated impressive properties as a packaging material and have been presented. The mechanical performance is good. Due to the plasticizing effect of glycerol, honey, and carrageenan, Young\u0026rsquo;s modulus and tensile strength were reduced, while the tensile strain increased, depending on the amount of plasticizer added. Concurrently, a shift in the relaxation temperature of the DeChNF film towards lower temperatures with plasticizer content observed around 40\u0026ndash;90\u0026ordm;C and 300\u0026ndash;370\u0026ordm;C, suggests a notable plasticization effect, with a more substantial plasticization appears to be associated with honey, followed by glycerol, and finally, carrageenan. Consequently, this shows that the mechanical properties of the deacetylated ChNF film can be optimized or tailored without compromising their essential attributes, including high transparency, thermal stability, WAC, and WVP. The mechanical performance of the film containing carrageenan is superior to that of the films plasticized with honey and glycerol. Furthermore, the tensile strengths of the DeChNF films with 5% w/w glycerol, honey, and carrageenan surpassed those of commercial polyethylene films, which have a tensile strength of only 10.9 MPa. Interestingly, this study is particularly significant since honey and carrageenan are high-quality, food-grade materials that are naturally occurring compared to glycerol. The implications of this study are substantial, as it enhances not only the potential applications of ChNFs in the development of high-performance films but also promotes the use of chitin as a natural, eco-friendly material, especially for edible films in packaging.\u003c/p\u003e \u003cdiv id=\"Sec27\" class=\"Section2\"\u003e \u003ch2\u003eLimitations and Future perspectives of the DeChNF plasticized films in Packaging\u003c/h2\u003e \u003cp\u003eIn summary, this study successfully demonstrated that honey and carrageenan can serve as natural plasticizers to replace glycerol and potentially other conventional plasticizers such as sorbitol, xylitol, fructose, and urea, thereby enhancing the applicability of DeChNF films. The literature has extensively reported the impact of plasticizer concentration on the mechanical and barrier properties of biopolymer films, particularly those made from starch and chitosan, and recently, on cellulose and DeChNF. Summarizing the results from the previous studies presented in this work. Firstly, Jouki et al. [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e] demonstrated that increasing glycerol concentration in cress seed gum films enhanced water vapor permeability, thickness, moisture content, water solubility, elongation at break, and surface smoothness, while decreasing density, tensile strength, and Young's modulus. Secondly, Sanyang et al. [\u003cspan citationid=\"CR69\" class=\"CitationRef\"\u003e69\u003c/span\u003e] observed increased moisture content, film thickness, and water solubility, while sugar palm starch films' density and water absorption decreased. Thirdly, Tarique et al. [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e] demonstrated reduced moisture content and water solubility, along with increased tensile strain, but a decrease in tensile strength and modulus in arrowroot starch films plasticized with glycerol (at 15, 30, and 45 wt%). In contrast, Muscat et al. reported that combining glycerol and xylitol as plasticizers resulted in low WVP in low and high-amylose starches. Fourthly, Suppakul et al. [\u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e] also observed a decrease in tensile strength and MVP, alongside an increase in the percentage of elongation to failure, with a rise in plasticizer content up to a certain level. These changes have been attributed to the molecular properties of the plasticizers. Consequently, the film structure may alter, affecting density and thickness. Despite the different focuses in the literature compared to the current study, particularly in preparation techniques and materials, the performance of glycerol and similar conventional plasticizers, alongside honey and carrageenan as alternatives, is apparent, highlighting the potential applicability of these natural plasticizers.\u003c/p\u003e \u003cp\u003eHowever, several limitations exist. Firstly, while plasticization improved the flexibility of the films, it significantly reduced their tensile strength and Young's modulus of the DeChNF film. This reduction may limit the application of these films in packaging scenarios where high mechanical strength is critical. The optimization of the preparation technique and conditions can mitigate this issue. Nonetheless, our novel approach, using natural plasticizers to enhance the properties of DeChNF films, represents a unique contribution to the field. Future research should explore reinforcement strategies to balance flexibility and strength, such as cross-linking or blending with other biopolymers [\u003cspan citationid=\"CR69\" class=\"CitationRef\"\u003e69\u003c/span\u003e]. Secondly, issues related to higher water absorption and permeability were observed. The high WAC and WVP of the plasticized films indicate a concern about the susceptibility of the film properties to moisture. This could impact the films' structural integrity and effectiveness in protecting food in high-humidity environments. Further optimization, such as using hydrophobic coatings, nanocomposites, or lamination techniques, could enhance the moisture resistance of these films [\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e, \u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e67\u003c/span\u003e]. Chemical modification will improve compatibility for blending with the vast available polymers, such as LDPE, which are hydrophobic. Thirdly, the compatibility and long-term stability of the plasticizers need to be considered. The stickiness and adhesion issues noted in honey-plasticized films could affect handling and practical use in packaging. Over time, plasticizer migration and phase separation may alter the films' mechanical and barrier properties. Fourthly, imaging of the microstructure was not conducted in this study. However, we can infer the homogeneity and structural integrity of the films from their optical transparency, mechanical properties, and XRD data, which suggest a uniform dispersion of the plasticizers. Fifthly, scalability and economic viability are crucial. Although the study successfully developed DeChNF films, scaling production will require cost-effective and industrial-friendly methods. Exploring alternative processing techniques, such as vacuum filtration, melt-processing techniques, e.g., extrusion, or bio-composite layering, could enhance the feasibility of mass production. The potential of chitin-based films in packaging applications can be further enhanced through specific future studies. For instance, incorporating scanning electron microscopy (SEM) imaging could help investigate the film morphology and confirm the impact of plasticization at the nanoscale. Additionally, enhancing mechanical performance can be achieved by blending DeChNF with other biopolymers like starch, polylactic acid (PLA), or nanocellulose, or through nanocomposite reinforcement by incorporating clay nanoparticles, cellulose nanocrystals, carbon nanofibers, or graphene oxide [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR70\" class=\"CitationRef\"\u003e70\u003c/span\u003e]. Improving moisture barrier properties is another avenue for development. This can include layering DeChNF films with hydrophobic coatings such as wax, zein protein, or biodegradable polyesters. Cross-linking agents like tannins, citric acid, or enzymatic treatments can strengthen the intermolecular network, thereby reducing WVP [\u003cspan citationid=\"CR71\" class=\"CitationRef\"\u003e71\u003c/span\u003e]. Moreover, biodegradability can be tailored to meet specific applications. For example, controlled degradation profiles can be developed by modifying the degree of deacetylation of chitin to match different packaging needs, such as short-term food wrapping versus long-term storage. Lastly, utilizing chitin from the seafood industry promotes a circular economy and supports cost-effective production. Exploring innovative packaging applications, such as antimicrobial coatings, pH-sensitive food freshness indicators, and oxygen scavenging films, can help extend food shelf life.\u003c/p\u003e \u003c/div\u003e"},{"header":"Declarations","content":"\u003ch2\u003eFunding:\u003c/h2\u003e \u003cp\u003eThis project was supported by Knut och Alice Wallenbergs\u003c/p\u003e \u003cp\u003e \u003cb\u003eData availability\u003c/b\u003e: No data sets were generated or analyzed during the current study.\u003c/p\u003e \u003cp\u003e \u003cb\u003eCompeting interest\u003c/b\u003e: The authors declare no competing interest\u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eN.E Conceptualizations, Methodology, Analysis, and Writing. C.F.K. Experimentation, Writing, and Analysis. N.M Conceptualization, Writing, and Reviewing. All authors reviewed and approved the manuscript.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eProf LA Berglund at KTH Royal Institute of Technology is acknowledged for constructive discussions and provision of partial funding through his grant with the Knut and Alice Wallenberg Foundation.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eAbotbina W, Sapuan SM, Sulaiman S, Ilyas RA (2020) Review of Corn Starch Biopolymer. In Proceedings of the 7th Postgraduate Seminar on Natural Fibre Reinforced Polymer Composites Serdang, Malaysia: Institute of Tropical Forest and Forest Products (INTROP), University Putra Malaysia. 37\u0026ndash;40\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIram D, Riaz R, Iqbal RK (2019) Usage of Potential Micro-organisms for Degradation of Plastics. Open J Environ Biol 4:7\u0026ndash;15. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.17352/ojeb.000010\u003c/span\u003e\u003cspan address=\"10.17352/ojeb.000010\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAbotbina W, Sapuan SM, Sultan MTH, Alkbir MFM, Ilyas RA (2021) Development and Characterization of Cornstarch-Based Bioplastics Packaging Film Using a Combination of Different Plasticizers. Polym 13:3487. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/polym13203487\u003c/span\u003e\u003cspan address=\"10.3390/polym13203487\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSyafiq RMO, Sapuan SM, Zuhri MYM, Othman SH, Ilyas RA (2022) Effect of plasticizers on the properties of sugar palm nanocellulose/cinnamon essential oil reinforced starch bio-nanocomposite films. Nanotechnol Rev 11:423\u0026ndash;437. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1515/ntrev-2022-0028\u003c/span\u003e\u003cspan address=\"10.1515/ntrev-2022-0028\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIlyas M, Ahmad W, Khan H, Yousaf S, Khan K, Nazir SP (2018) Plastic Waste as A Significant threat to Environment-A Systematic Literature Review. Rev Environ Health 33:383\u0026ndash;406. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1515/reveh-2017-0035\u003c/span\u003e\u003cspan address=\"10.1515/reveh-2017-0035\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eQin YY, Zhang ZH, Li L, Yuan ML, Fan J, Zhao TR (2015) Physio-mechanical properties of an active chitosan film incorporated with montmorillonite and natural antioxidants extracted from pomegranate rind. J food Sci Techno 52:1471\u0026ndash;1479. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1007/s13197-013-1137-1\u003c/span\u003e\u003cspan address=\"10.1007/s13197-013-1137-1\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eRawdkuen S, Sai-Ut S, Benjakul S (2010) Properties of gelatin films from giant catfish skin and bovine bone: a comparative study. Eur Food Res Technol 23:907\u0026ndash;916. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1007/s00217-010-1340-5\u003c/span\u003e\u003cspan address=\"10.1007/s00217-010-1340-5\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eLaith SA, Al-Hashimi AG (2019) Mechanical Properties of carboxymethyl cellulose edible films. Basrah J Agri Sci 32:68\u0026ndash;78. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.37077/25200860.2019.129\u003c/span\u003e\u003cspan address=\"10.37077/25200860.2019.129\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eShivakumara LR, Demappa T, Singh V (2017) Mechanical and barrier properties of hydroxy propyl methyl cellulose edible polymer films with plasticizer combinations. J Food Proc Pre 4:745\u0026ndash;4549. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1111/jfpp.13020\u003c/span\u003e\u003cspan address=\"10.1111/jfpp.13020\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eGon\u0026ccedil;alves SM, Dos Santos DC, Motta JFG, Dos Santos RR, Ch\u0026aacute;vez DWH, de Melo NR (2019) Structure and functional properties of cellulose acetate films incorporated with glycerol. Carbohyr Polym 209:190\u0026ndash;197. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2019.01.031\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2019.01.031\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eHorvat G, Žvab K, Knez Ž, Novak Z (2022) Simple, one-pot method for preparing transparent ethyl cellulose films with good mechanical properties. Polym 14:2399. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/polym14122399\u003c/span\u003e\u003cspan address=\"10.3390/polym14122399\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eDomene-L\u0026oacute;pez D, Garc\u0026iacute;a-Quesada JC, Martin-Gullon I, Montalb\u0026aacute;n MG 2019 Influence of starch composition and molecular weight on physicochemical properties of biodegradable films. Polym 11: 1084. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/polym11071084\u003c/span\u003e\u003cspan address=\"10.3390/polym11071084\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSantos NL, Braga RC, Bastos MS, Cunha PL, Mendes FR, Galv\u0026atilde;o AM, Passos AA (2019) Preparation and characterization of Xyloglucan films extracted from Tamarindus indica seeds for packaging cut-up \u0026lsquo;Sunrise Solo\u0026rsquo;papaya. Int J Biol Macromol 132:1163\u0026ndash;1175. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.ijbiomac.2019.04.044\u003c/span\u003e\u003cspan address=\"10.1016/j.ijbiomac.2019.04.044\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eKochumalayil JJ, Berglund LA (2014) Water-soluble hemicelluloses for high humidity applications\u0026ndash;enzymatic modification of xyloglucan for mechanical and oxygen barrier properties. Green Chem 16:1904\u0026ndash;1910. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1039/C3GC41823E\u003c/span\u003e\u003cspan address=\"10.1039/C3GC41823E\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eLarsson PA, Berglund LA, Wagberg L 2014 Ductile all-cellulose nanocomposite films fabricated from core\u0026ndash;shell structured cellulose nanofibrils. Biomacromol 15: 2218\u0026ndash;2223. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/bm500360c\u003c/span\u003e\u003cspan address=\"10.1021/bm500360c\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eYang X, Jungstedt E, Reid MS, Berglund LA (2021) Polymer films from cellulose nanofibrils\u0026mdash;effects from interfibrillar interphase on mechanical behavior. Macromol 9:4443\u0026ndash;4452. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/acs.macromol.1c00305\u003c/span\u003e\u003cspan address=\"10.1021/acs.macromol.1c00305\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eBai L, Liu L, Esquivel M, Tardy BL, Huan S, Niu X, Rojas OJ (2022) Nanochitin: chemistry, structure, assembly, and applications. Chem Rew 13:11604\u0026ndash;11674. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/acs.chemrev.2c00125)\u003c/span\u003e\u003cspan address=\"10.1021/acs.chemrev.2c00125)\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSalaberria AM, Fernandes SCM, Diaz RH, Labidi J (2015) processing of α-chitin nanofibers by dynamic high pressure homogenization: Characterization and antifungal activity against A. niger. Carbohydr Polym 116:286\u0026ndash;291. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2014.04.047\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2014.04.047\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIfuku S, Saimoto H (2012) Chitin nanofibers: preparations, modifications, and applications. Nanoscale 11:3308\u0026ndash;3318. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1039/c2nr30383c\u003c/span\u003e\u003cspan address=\"10.1039/c2nr30383c\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eFAO, The State of World Fisheries and Aquaculture (2020) Sustainability in Action. Rome: FAO, 2020. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003e10.4060/ca9229en\u003c/span\u003e\u003cspan address=\"10.4060/ca9229en\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e. https://doi.org/10.4060/ca9229en\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eChen C, Wu Q, Wan Z, Yang Q, Xu Z, Li D, Rojas OJ (2022) Mildly processed chitin used in one-component drinking straws and single use materials: Strength, biodegradability and recyclability. Chem Eng J 442:136173. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.cej.2022.136173\u003c/span\u003e\u003cspan address=\"10.1016/j.cej.2022.136173\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eYan N, Chen X (2015) Sustainability: Don\u0026rsquo;t waste seafood waste 2015. Nature 524:155\u0026ndash;157\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSvensson SE, Oliveira AO, Adolfsson KH, Heinmaa I, Root A, Kondori N, Zamani A (2022) Turning food waste to antibacterial and biocompatible fungal chitin/chitosan monofilaments. Int J Biol Macromol. 209: 618\u0026ndash;630. https://doi.10.1016/j.ijbiomac.2022.04.031\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMushi NE (2021) A review on native well-preserved chitin nanofibrils for materials of high mechanical performance. Int J Biol Macromol 178:591\u0026ndash;606. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.ijbiomac.2021.02.149\u003c/span\u003e\u003cspan address=\"10.1016/j.ijbiomac.2021.02.149\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eFan Y, Saito T, Isogai A (2010) Individual chitin nano-whiskers prepared from partially deacetylated α-chitin by fibril surface cationization. Carbohydr Polym 4:1046\u0026ndash;1051. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2009.10.044\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2009.10.044\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eChen C, Wang Y, Yang Y, Pan M, Ye T, Li D (2018) High strength gelatin-based nanocomposites reinforced by surface-deacetylated chitin nanofiber networks. Carbohydr Polym 195:387\u0026ndash;392. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2018.04.095\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2018.04.095\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIfuku S, Ikuta A, Egusa M, Kaminaka HH, Izawa M, Saimoto M (2013) Preparation of high-strength transparent chitosan film reinforced with surface-deacetylated chitin nanofibers. Carbohydr Polym 98:1198\u0026ndash;1202. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2013.07.033\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2013.07.033\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eLi M, Wu Q, Song K, Cheng HN, Suzuki S, Lei T (2016) Chitin Nanofibers as Reinforcing and Antimicrobial Agents in Carboxymethyl Cellulose Films: Influence of Partial Deacetylation. ACS Sustain Chem Eng 4:4385\u0026ndash;4395. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/acssuschemeng.6b00981\u003c/span\u003e\u003cspan address=\"10.1021/acssuschemeng.6b00981\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIfuku S, Ikuta A, Izawa H, Morimoto M, Saimoto H (2014) Control of mechanical properties of chitin nanofiber film using glycerol without losing its characteristics. Carbohydr Polym 101:714\u0026ndash;717. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2013.09.076\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2013.09.076\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMushi NE, Meela E, Kaombe D (2023) Effective Enhancement of Post-Harvest Tomato Storage through Wrapping Using Deacetylated Chitin Nanofibril-Plasticized Honey Films. Tanz J Sci 14:711\u0026ndash;724. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.4314/tjs.v49i3.14\u003c/span\u003e\u003cspan address=\"10.4314/tjs.v49i3.14\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMushi NE, Nishino T, Berglund LA, Zhou Q (2019) Strong and Tough Chitin Film from α-Chitin Nanofibers Prepared by High Pressure Homogenization and Chitosan Addition. ACS Sustain Chem Eng 7:1692\u0026ndash;1697. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/acssuschemeng.8b05452\u003c/span\u003e\u003cspan address=\"10.1021/acssuschemeng.8b05452\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMushi NE, Utsel S, Berglund LE (2014) Nanostructured biocomposite films of high toughness based on native chitin nanofibers and chitosan. Frontier Chem 2:99. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3389/fchem.2014.00099\u003c/span\u003e\u003cspan address=\"10.3389/fchem.2014.00099\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eChen C (2019) Relationship between Water Activity and Moisture Content in Floral Honey, Foods (Basel, Switzerland) 1: 30. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/foods8010030\u003c/span\u003e\u003cspan address=\"10.3390/foods8010030\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eKunat-Budzyńska M, Rysiak A, Wiater A, Grąz M, Andrejko M, Budzyński M, Bryś MS, Sudziński M, Tomczyk M, Gancarz M, Rusinek R, Ptaszyńska AA (2023) Chemical Composition and Antimicrobial Activity of New Honey Varietals. Int J Environ Res Public Health 3:2458. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/ijerph20032458\u003c/span\u003e\u003cspan address=\"10.3390/ijerph20032458\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eFu M, Wu Y, Zhang Q, Xue Z, Geng C, Xia Y (2021) Study on the mechanical and flame retardant properties of a novel carrageenan fiber-CAF-K,Al. European. Polym J 150:110408. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1515/polyeng-2022-0237\u003c/span\u003e\u003cspan address=\"10.1515/polyeng-2022-0237\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eHan J, Han X, Xue Z, Wang Q, Xia Y, Zhao Z (2021) An eco-friendly procedure for achieving high-yield carrageenan from Hypnea cervicornis suitable for wet spinning. J Appl Polym Sci 138:1\u0026ndash;9. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1002/app.50833\u003c/span\u003e\u003cspan address=\"10.1002/app.50833\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMarangoni L, Garcia R, Maria R, Alves V (2021) Water vapor sorption and permeability of sustainable alginate/collagen/SiO\u003csub\u003e2\u003c/sub\u003e composite films. 152:112261. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.lwt.2021.112261\u003c/span\u003e\u003cspan address=\"10.1016/j.lwt.2021.112261\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eZia KM, Tabasum S, Nasif M, Sultan N, Aslam A, Noreen, Zuber m (2019) A review on synthesis, properties, and applications of natural polymer-based carrageenan blends and composites. Int J Biol Macromol 96:282\u0026ndash;301. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.ijbiomac.2016.11.095\u003c/span\u003e\u003cspan address=\"10.1016/j.ijbiomac.2016.11.095\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSormin RBD, Masela A, Idris A (2019) Physicochemical properties of carrageenan originated from Lermatang Village, Southwest Maluku District, and IOP Conference Series. Earth Environ Sci 339: 012053\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eTasende MG, Manr\u0026iacute;quez-Hern\u0026aacute;ndez JA (2016) Carrageenan properties and applications: A review. Carrageenans Sources and Extraction. Methods, Molecular Structure Bioactive. Properties and Health Effects. Edition 1st Chap. Nova Sci Publisher 2:17\u0026ndash;49\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMushi NE, Butchosa N, Salajkova M, Zhou Q, Berglund LA (2014) Nanostructured membranes based on native chitin nanofibers prepared by mild process. Carbohydr Polym 112:255\u0026ndash;263. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2014.05.038\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2014.05.038\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eDong M, Wu D, Han J, Wang Y, Xue Z, Xia Y (2020) Comparison of Two Different Preparation Methods of Wet-Spun Carrageenan Fibers Directly from Chondrus Extractions. ACS omega 5:6661\u0026ndash;6665. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/acsomega.9b04435\u003c/span\u003e\u003cspan address=\"10.1021/acsomega.9b04435\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eWang K, Kasuya H, Koga M, Nogi, Uetani K (2021) Thermal conductivity analysis of chitin and deacetylated-chitin nanofiber films under dry conditions. Nanomaterials 3:658. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/nano11030658\u003c/span\u003e\u003cspan address=\"10.3390/nano11030658\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eJumaidin R, Sapuan SM, Jawaid M, Ishak MR, Sahari J (2017) Thermal, mechanical, and physical properties of seaweed/sugar and palm fibre reinforced thermoplastic sugar palm Starch/Agar hybrid composites. Int J Biol Macromol 97:606\u0026ndash;615. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.ijbiomac.2017.01.079\u003c/span\u003e\u003cspan address=\"10.1016/j.ijbiomac.2017.01.079\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003ePereda M, Aranguren MI, Marcovich NE (2009) Water vapor absorption and permeability of films based on chitosan and sodium caseinate. J Appl Poly Sci 6:2777\u0026ndash;2784. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1002/app.29347\u003c/span\u003e\u003cspan address=\"10.1002/app.29347\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eTarique J, Sapuan SM, Khalina A (2021) Effect of glycerol plasticizer loading on the physical, mechanical, thermal, and barrier properties of arrowroot (Maranta arundinacea) starch biopolymers. Sci Rep 1:13900. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1038/s41598-021-93094-y\u003c/span\u003e\u003cspan address=\"10.1038/s41598-021-93094-y\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eJouki M, Khazaei N, Ghasemlou M, HadiNezhad M (2013) Effect of glycerol concentration on edible film production from cress seed carbohydrate gum. Carbohydr Polym 1:39\u0026ndash;46. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2013.03.077\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2013.03.077\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eTanpichai S, Srimarut Y, Woraprayote W, Malila Y (2022) Chitosan coating for the preparation of multilayer coated paper for food-contact packaging: Wettability, mechanical properties, and overall migration. Int J Biol Macromol 213:534\u0026ndash;545. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.ijbiomac.2022.05.193\u003c/span\u003e\u003cspan address=\"10.1016/j.ijbiomac.2022.05.193\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eTanpichai S, Pumpuang L, Srimarut Y, Woraprayote W, Malila Y (2023) Development of chitin nanofiber coatings for prolonging shelf life and inhibiting bacterial growth on fresh cucumbers. Sci Rep 1:13195. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1038/s41598-023-39739-6\u003c/span\u003e\u003cspan address=\"10.1038/s41598-023-39739-6\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIfuku S, Nogi K, Abe M, Yoshioka M, Morimoto H, Saimoto H, Yano H (2009) Preparation of chitin nanofibers with a uniform width as alpha-chitin from crab shells. Biomacromol 6:1584\u0026ndash;1588. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1021/bm900163d\u003c/span\u003e\u003cspan address=\"10.1021/bm900163d\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eBoonmahitthisud A, Thongdonson K, Tanpichai S (2023) Preparation of Chitin Nanofibers from Shrimp Shell Waste by Partial Deacetylation and Mechanical Treatment Preparation of Chitin Nanofibers from Shrimp Shell Waste by Partial Deacetylation and Mechanical Treatment. J Natural Fibers 2: 2229515. https://doi.10.1080/15440478.2023.2229515\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eIfuku S, Nogi M, Morimoto MY, Yano M, Saimoto H (2010) H Fibrillation of dried chitin into 10\u0026ndash;20nm nanofibers by a simple grinding method under acidic conditions. Carbohydr Polym 1; 134\u0026ndash;139. https://doi.10.1016/j.carbpol.2010.02.006\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAklog YK, Nagae T, Izawa H, Morimoto M, Saimoto H, Ifuku S (2016) Preparation of chitin nanofibers by surface esterification of chitin with maleic anhydride and mechanical treatment. Carbohydr Polym 153:55\u0026ndash;59. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2016.07.060\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2016.07.060\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eChen H, Montanari C, Yan M, Popov S, Li Y, Sychugov I, Berglund LA (2020) Refractive index of delignified wood for transparent biocomposites. RSC Adv 10:40719\u0026ndash;40724. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1039/d0ra07409h\u003c/span\u003e\u003cspan address=\"10.1039/d0ra07409h\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMartini N, J\u0026ouml;rg B, Hell SW (2002) A new high-aperture glycerol immersion objective lens and its application to 3D‐fluorescence microscopy. J Microscopy 206:146\u0026ndash;151. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1046/j.1365-2818.2002.01016.x\u003c/span\u003e\u003cspan address=\"10.1046/j.1365-2818.2002.01016.x\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eZewude DA, Akamatsu M, Ifuku S (2024) Structural Color of Partially Deacetylated Chitin Nanowhisker Film Inspired by Jewel Beetle. Materials 21:5357. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3390/ma17215357\u003c/span\u003e\u003cspan address=\"10.3390/ma17215357\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eChan SW, Mirhosseini H, Taip FS, Ling TC, Tan CP (2013) Comparative study on the physicochemical properties of κ-carrageenan extracted from Kappaphycus alvarezii (doty) doty ex Silva in Tawau, Sabah, Malaysia and commercial κ-carrageenans. Food Hydrocolloids 2: 581\u0026ndash;588. https://doi.10.1016/j.foodhyd.2012.07.010)\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAlbu, Frunză G, Zaharia R, Pop IM 2021 Estimation of some quality parameters of honey\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eKittur FS, Prashanth KV, Sankar KU, Tharanathan RN (2002) Characterization of chitin, chitosan and their carboxymethyl derivatives by differential scanning calorimetry. Carbohydr Polym 49:185\u0026ndash;193\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eKim MJ, Yoo BS (2010) Glass Transition Temperature of Honey Using Modulated Differential Scanning Calorimetry (MDSC): Effect of Moisture Content. Prev Nutr Food Sci 4:356\u0026ndash;359. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3746/jfn.2010.15.4.356\u003c/span\u003e\u003cspan address=\"10.3746/jfn.2010.15.4.356\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAbdullah AHD, Firdiana B, Nissa RC, Satoto R, Karina M, Fransisk D (2021) Effect of κ-carrageenan on mechanical, thermal and biodegradable properties of starch\u0026ndash;carboxymethyl cellulose (CMC) bioplastic. Cell Chem Technol 9\u0026ndash;10:1109\u0026ndash;1117. https://doi.org/10.35812\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAngell C, Austen Sare EJ, Bressel RD (1967) Concentrated electrolyte solution transport theory: directly measured glass temperatures and vitreous ice. J Phy Chem 71:2759\u0026ndash;2761\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003ePatil SP, Mehrotra SC (1995) Dielectric Relaxation of Glycerol and Glycerol/Water Mixtures\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eNam YS, Park WH, Ihm D, Hudson SM (2010) Effect of the degree of deacetylation on the thermal decomposition of chitin and chitosan nanofibers. Carbohydr Polym 1:291\u0026ndash;295. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.carbpol.2009.11.030\u003c/span\u003e\u003cspan address=\"10.1016/j.carbpol.2009.11.030\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eHazrati KZ, Sapuan SM, Zuhri MYM, Jumaidin R (2021) Effect of plasticizers on physical, thermal, and tensile properties of thermoplastic films based on Dioscorea hispida starch. Int J Biol Macromol 185:219\u0026ndash;228. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.ijbiomac.2021.06.099\u003c/span\u003e\u003cspan address=\"10.1016/j.ijbiomac.2021.06.099\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSuppakul P, Chalernsook B, Ratisuthawat B, Prapasitthi S, Munchukangwan N (2013) Empirical modeling of moisture sorption characteristics and mechanical and barrier properties of cassava flour film and their relation to plasticizing\u0026ndash;antiplasticizing effects. LWT - Food Sci Technol 1:290\u0026ndash;297. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.lwt.2012.05.013\u003c/span\u003e\u003cspan address=\"10.1016/j.lwt.2012.05.013\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMuscat D, Adhikari B, Adhikari R, Chaudhary D (2010) Comparative study of film forming behavior of low and high amylose starches using glycerol and xylitol as plasticizers. J Food Eng 2:189\u0026ndash;201. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.jfoodeng.2011.10.019\u003c/span\u003e\u003cspan address=\"10.1016/j.jfoodeng.2011.10.019\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eMangaraj S, Goswami TK, Mahajan PV (2009) Applications of plastic films for modified atmosphere packaging of fruits and vegetables: a review. Food Eng Rev 1:133\u0026ndash;158. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1007/s12393-009-9007-3\u003c/span\u003e\u003cspan address=\"10.1007/s12393-009-9007-3\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSanyang ML, Sapuan SM, Jawaid M, Ishak MR, Sahari J (2016) Effect of plasticizer type and concentration on physical properties of biodegradable films based on sugar palm (arenga pinnata) starch for food packaging. J Food Sci Technol 1:326\u0026ndash;336. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1007/s13197-015-2009-7)\u003c/span\u003e\u003cspan address=\"10.1007/s13197-015-2009-7)\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eLiu X, Zhang T, Pang K, Duan Y, Zhang J (2016) Graphene oxide/cellulose composite films with enhanced UV-shielding and mechanical properties prepared in NaOH/urea aqueous solution. RSC Adv 77:73358\u0026ndash;73364. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1039/C6RA16535D\u003c/span\u003e\u003cspan address=\"10.1039/C6RA16535D\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eWu H, Lei Y, Lu J, Zhu R, Xiao D, Jiao C, Li M (2019) Effect of citric acid induced crosslinking on the structure and properties of potato starch/chitosan composite films. Food Hydrocolloids 97:105208. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.foodhyd.2019.105208\u003c/span\u003e\u003cspan address=\"10.1016/j.foodhyd.2019.105208\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"Deacetylated chitin nanofibrils, bees' honey, carrageenan, glycerol, films, mechanical properties","lastPublishedDoi":"10.21203/rs.3.rs-6343422/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6343422/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eHoney from bees and carrageenan from red seaweeds may act as alternative plasticizers to commercial glycerol in improving the mechanical flexibility of deacetylated chitin nanofibril (DeChNF) films. Free-standing films with plasticizer content up to 65% were produced using a casting technique. Transparency, thermal relaxation, tensile properties, water absorption capacity, and water vapor permeability of the films were evaluated as essential properties in packaging. Firstly, the deacetylated ChNF film had a transmittance of 84.9% at 800 nm, with films containing 20 wt% plasticizers displaying transmittance values of 87.8% (glycerol), 83.6% (honey), and 85.4% (carrageenan). Secondly, Differential Scanning Calorimetry (DSC) indicated relaxation temperatures between 40\u0026ndash;80\u0026ordm;C and 300\u0026ndash;370\u0026ordm;C towards lower values with the plasticizer content. A more profound plasticization effect appears to be associated with honey, followed by glycerol, and finally, carrageenan. Thirdly, mechanical testing revealed a decrease in tensile strength from 41.3 MPa for pure DeChNF to 6.3 MPa (glycerol), 4.3 MPa (honey), and 9.4 MPa (carrageenan). Tensile strain increased from 8.5% for DeChNF to 24.74% (glycerol), 31.5% (honey), and 21.65% (carrageenan). Fourthly, water absorption capacity and water vapor permeability performance are compared to commercial packaging films. Thus, the data from DeChNF plasticized films with honey and carrageenan are novel and promising for innovative chitin nanofibril applications in packaging.\u003c/p\u003e","manuscriptTitle":"Strong and Transparent Deacetylated Chitin Nanofibril Films using Bees’ Honey and Carrageenan as Potential Plasticizers in Packaging","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-06-18 19:02:31","doi":"10.21203/rs.3.rs-6343422/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"7636c7b5-b9d5-49d8-9070-e46158f9ac5c","owner":[],"postedDate":"June 18th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2025-06-18T19:02:31+00:00","versionOfRecord":[],"versionCreatedAt":"2025-06-18 19:02:31","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-6343422","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6343422","identity":"rs-6343422","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}