Effect of different natural plasticizers on Ethyl Cellulose Oleogel bioplastic

Effect of different natural plasticizers on Ethyl Cellulose Oleogel bioplastic | 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 Effect of different natural plasticizers on Ethyl Cellulose Oleogel bioplastic Luca Cafuero, Muhammad Waheed, Marco Friuli, Christian Demitri, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7490012/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 Growing concerns about the environmental impact of fossil-based plastics has highlighted the need for bioplastics. Recently, Ethyl Cellulose-based Oleogels have been proposed as a promising bioplastic alternative due to their biodegradability, biocompatibility, and processability. However, Oleogels require improved plasticity to compete with traditional bioplastics, which are often brittle and difficult to process, limiting their ability to match conventional plastics. Plasticizers are a major bottleneck in the development of sustainable materials, as many are toxic to the environment. This study focused on plasticizing Oleogels using natural origin plasticizers, specifically, Cardanol, Castor Oil, Oleic Acid and Tributyl Citrate. The results demonstrate that these additives significantly influence the mechanical and processing properties of the material. The most effective plasticizers resulted are Cardanol, which increased the maximum elongation by ~ 450% and reduced the gelation temperature by 15–30°C compared to the plasticizer-free Oleogel, and Castor Oil, which enhanced elongation at break by about 380% while preserving the maximum load close to that of the plasticizer-free formulation. These findings highlight the potential of these bio-plasticizers in improving the mechanical and thermal properties of Oleogel-based materials. bioplastic Ethyl Cellulose Oleogel green plasticizers sustainability biodegradability Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Introduction Plastics derived from petroleum are spread in everyday life, from the electronic devices to vehicle components and food packaging. In 2019, the packaging sector led plastic consumption over 146 million tons, with construction sector in second place with about 70 million tons [ 1 ]. Nowadays, plastic waste is a major environmental issue, as 79% ends up in landfills or in the environment [ 2 ], where it persists for centuries [ 3 , 4 ], breaking into microplastics which are found in oceans, ice, drinking water, and food chains [ 5 ]. Plastic’s fossil fuel origin intensifies the problem, with plastic production accounting for 3–5% of global CO 2 equivalent emissions, primarily during the production and conversion phases [ 6 ]. Unfortunately, plastic’s success relay on many advantages due to their technical features, consequently it is not easy to find technically and cost comparable green alternatives. The main advantage of petroleum-derived plastics lies in their ability to be tailored for diverse applications using the same polymer [ 7 – 10 ]. Plasticizers play a key role in modifying mechanical properties, thermal stability, processability, and durability [ 11 ]. An effective plasticizer must exhibit high compatibility with the polymer matrix to prevent phase separation and migration over time while efficiently lowering the glass transition temperature [ 11 , 12 ]. Additionally, it should possess low volatility to minimize evaporation during processing and use, as well as high thermal and chemical stability to withstand heat, UV exposure, and environmental stressors [ 12 ]. Resistance to extraction by water, oils, or solvents is also essential, particularly in medical and food-related applications[ 12 ]. Phthalates are a widely used class of plasticizers, particularly in the production of vinyl medical products, such as intravenous tubing. The most commonly used phthalate is di-2-ethylhexyl phthalate (DEHP), which provides excellent gelling properties, remains relatively non-volatile under heat, enhances the electrical properties of compounds, and is favoured in medical devices for its ability to maintain flexibility at low temperatures while also withstanding high-temperature sterilization [ 13 ]. Bisphenol A (BPA) is a commonly used plasticizer that enhances the mechanical properties of plastics by improving elasticity, thermal resistance, and moisture resistance, playing a crucial role as a monomer in the production of polycarbonate plastics and epoxy resins [ 14 ]. On the other hand, some of most spread plasticizers have been found to have toxic effects on health [ 15 ]. In recent years, the shift towards bioplastics—defined as materials derived from renewable sources and/or designed to be biodegradable or compostable—has gained traction as a sustainable alternative aimed at reducing environmental impact throughout their lifecycle. Bioplastics, although currently representing only 0.5% of the global market [ 16 ], are experiencing growth. In particular, thermoplastic polyesters such as Polylactic acid (PLA), polyhydroxybutyrate (PHB), and polybutylene succinate (PBS) are among the most promising materials for consumer applications, owing to their balance of durability and biodegradability and production from renewable sources (e.g. PLA is mainly produced by the fermentation of starch plants such as from corn, sugarcane, etc. and the possibility to be compostable [ 17 ]). However, these biopolymers are brittle. For example, PLA has a Young’s Modulus typically over 3 GPa, a strain at break about 5% [ 18 ]. To expand its applications, various plasticizers have been tested, including Epoxidated Soybean Oil [ 19 ] and Acetylized Tributyl Citrate [ 20 ] though issues like leaching and reduced performance remain challenges. PBS it’s a biodegradable aliphatic polyester [ 21 ] with melting temperatures which range from ~ 100°C to ~ 120°C and with a tensile Modulus between ~ 30 MPa and ~ 700 MPa [ 22 ]. It’s used in food applications such as packaging, compostable bags, etc. [ 22 ], and its properties were improved by augmenting branches in polymeric chain using 1,2,4-butane-triol or augmenting the PBS’s crosslinks density with Castor Oil or Rutin [ 21 ]. Its brittleness and mechanical characteristics need to be improved for specific applications. PHB has a Young’s Modulus which ranges from 3 to 3.5 GPa with a ultimate strength around 30 MPa; its melting temperature is ~ 170°C and, further, it has good barrier properties making it suitable for different field, from food packaging to biomedical applications [ 23 , 24 ]. A major challenge involves PHB’s difficulties in its processability and aging. Developing high-performing, low-impact materials is key to establishing bioplastics as a sustainable alternative. In this study we focus on a promising biodegradable bioplastic class, Oleogels (OG) already proposed by our research group in the previous work [ 25 ]. They are a particular class of gel-like thermoplastic polymers composed of Ethyl Cellulose (EC) as structuring polymer and vegetable oil as organic solvent. The oil is entrapped within the EC tridimensional network [ 26 ] as well as water is trapped in hydrogels [ 27 ], and OG properties can be roughly modulated by changing EC concentration or oil type allowing to obtain a soft and jelly or a rigid bioplastic. Consequently, exactly as standard plastic and the other bioplastic, to extend the range of applications and make OG more competitive to standard plastics it is crucial to fine tune and enhance its properties. In this work we tested the effects on OG of different concentrations of naturally derived and green plasticizers presumably oil and EC compatible such as Cardanol (CAR, derived from cashew nutshell liquid [ 28 ], Castor Oil (CO from the seeds of the Ricinus communis plant [ 29 ]), Oleic Acid (OA, a monounsaturated fatty acid found in nature [ 30 ]), and Tributyl Citrate (TBC, a gold standard as bioplastic plasticizer [ 31 ]). The goal was to identify the optimal green plasticizer that could provide enhanced performance while maintaining the biobased and biodegradable nature of the Oleogel. Materials and Methods Ethyl Cellulose was produced by ChemPoint with viscosity in the range of 90–110 mPa*s and a degree of substitution about 2.5 (48,9–49,5%). For the OG was employed commercially available Soybean Oil (SBO), specifically Desantis, composed by 9–13% of saturated fatty acid, 25–33% mono-unsaturated, 55–65% poly-unsaturated fatty acid [ 25 ]. As plasticizers were employed Tributyl Citrateproduced by BCD Chemie under the name of Citrofol B1. Oleic Acid of technical grade 90% was purchased by Sigma – Aldrich. Commercial Castor Oil Matt purchased from the local market. Cardanol was purchased from Oltremare (Bologna, Italy). The production of Oleogels followed the method described in [ 25 ]. The difference in formulations was the Oil:Plasticizer ratio and two formulations were prepared: 25.0 and 37.5% w/w. An Oleogel without plasticizers was produced as control, named CTRL (Table 1 ) Table 1 Coded name of different Oleogels produced and characterized. Material Id Plasticizer Percentage CTRL - - CAR 25.0 Cardanol 25.0 CAR 37.5 Cardanol 37.5 CO 25.0 Castor Oil 25.0 CO 37.5 Castor Oil 37.5 OA 25.0 Oleic Acid 25.0 OA 37.5 Oleic Acid 37.5 TBC 25.0 Tributyl Citrate 25.0 TBC 37.5 Tributyl Citrate 37.5 To produce OG dogbone ASTM D638 Type V specimens, the material was grinded after being frozen using liquid nitrogen (to facilitate grinding avoiding overwarming). OG pellets were hot pressed at 165°C and 25 Bar (2.5 MPa) into a specifically shaped mould. Mechanical characterization The mechanical traction test was performed at room temperature on a Lloyd LR50K-plus machine on dogbone ASTM D638 Type V. A speed of 5 mm/s a room temperature was used to execute the test, and it was repeated on 3 dogbone specimens until their failure. Cyclical compression The visco-elastic response of the materials was analysed through cyclic compression tests, with a particular focus on shape memory, i.e., the material's ability to return to its original configuration after the application and removal of a load. To evaluate the impact of plasticizers on the material, two parameters were considered: the residual strain and the residual stress. The residual strain is intended as the permanent strain after the load was removed in the last compression cycle; the residual stress has been calculated as percentage of the maximum stress reached in the first compression cycle. The cyclical compression test was performed at room temperature on a Lloyd machine on cylindrical specimens (4 mm in thickness and 14 mm in diameter) fabricated by hot-pressing with the same parameters of the dogbone specimen. The test consisted of 10 consecutive compression-decompression cycles. The compression stage was brought until 1 mm of deformation starting from the original size, then the load was removed, then applied again without time gap between cycles. The tests were performed on the Lloyd LR50K-plus machine at room temperature. Dynamic Thermo-Mechanical Analysis (DTMA) Gelation temperature was determined on a Malvern rheometer using a flat plate of 20 mm in diameter using a dynamic thermo-mechanical analysis (DTMA) with temperature ramp 25–200°C with a heating rate of 5°C/min. The viscoelastic region was determined by an amplitude test after which the strain was set at 0.04% at a frequency of 0.4 Hz. The test consisted of the monitoring the elastic and the viscous moduli (respectively, G’ and G”) by applying a mono-frequency shear strain on cylindrical shaped samples (0,5 mm in thickness and 15 mm in diameter) obtained from a hot-pressing process previously described. Thermo-Gravimetric Analysis (TGA) A Thermo-Gravimetric Analysis test was conducted on the TGA Q500 instrument in the range 25–550°C on pellet samples of 5–10 mg at a flux of 10°C/min, on alumina crucibles. The tests were performed on an inert atmosphere with Nitrogen flux of 50 mL/min on the OGs pellets. The thermal stability of the materials was evaluated based on three key points of the degradation curve. The first point, T₁, corresponds to the temperature at which a 10% mass loss is recorded and is considered the onset of degradation. The second point, T₂, represents the temperature at which 50% of the mass is lost. Finally, the third point, T₃, marks the completion of degradation, when over 90% of the sample degraded. Differential Scanning Calorimetry/ Differential Thermal Analysis – DSC/DTA The DSC-DTA tests were conducted on machine DSC Q2500 (TA Instruments), in a temperature range of -30°C to 200°C at a rate of 5°C/min, on aluminium crucibles. The tests were performed on an inert atmosphere with Nitrogen flux of 50 mL/min using some pellet specimens of 10–15 mg. Fourier Transform Infrared Spectroscopy test – FTIR Fourier transform infrared spectroscopy (FT-IR) analysis, performed with a Jasco 6300 FT-IR spectrometer (JASCO Corporation, Tokyo, Japan), was used to characterize the single components and all the Oleogels. Infrared spectra were recorded in the wavelength range between 750 and 3,500 cm − 1 , 50 scans, and 4 cm − 1 of resolution, by using ATR Pro One X with ZnSe crystal. Wettability Test The wettability test was performed using the classical sessile drop test at room temperature. The drop of distilled water was carefully laid on the surface of a thin film (1 mm thickness) obtained by a hot-pressing process. The image was captured by a camera and the angles were measured by using First Ten Angstroms, FTA 1000 software (Newark, California, USA) equipped with a CDD camera. The test was repeated in triplicate. Results and Discussion Mechanical Test Young’s Moduli E, maximum strength σ max and maximum elongation ε max were investigated. Plasticizers reduced the elastic modulus (E) compared to CTRL by one order of magnitude (CAR and CO) or two (OA and TBC). Castor Oil and TBC 25.0 exhibited a slight increase, in ultimate tensile strength that was not statistically significative (Table 2 ). Noteworthy, TBC samples exhibited oil leakage, leading to their results being reported but excluded from further discussion. In all other cases, tensile strength decreased, and for Cardanol and Oleic Acid, this reduction was proportional to their concentration in the sample. Table 2 Young Moduli, Max Stress and Max Strain of all sample tested Material E (MPa) Stress (MPa) Strain (%) CTRL 136.3 ± 1.7 10.6 ± 0.4 38.2 ± 2.2 CAR 25.0 21.5 ± 1.6 5.9 ± 0.2 215.8 ± 8.4 CAR 37.5 11.3 ± 4.0 2.4 ± 0.3 200.5 ± 29.8 CO 25.0 41.5 ± 3.2 11.5 ± 0.9 158.9 ± 21.5 CO 37.5 12.7 ± 3.4 8.3 ± 1.0 184.9 ± 23.0 OA 25.0 22.4 ± 3.5 5.6 ± 0.3 147.4 ± 9.9 OA 37.5 4.8 ± 0.9 1.3 ± 0.2 141.2 ± 12.9 TBC 25.0 34.5 ± 5.4 11.2 ± 0.8 196.2 ± 1.6 TBC 37.5 8.9 ± 3.3 3.5 ± 0.5 221.2 ± 39.6 As reported in Table 2 , all plasticizers had an impact on strain at break increasing it up to ~ 465% for the Cardanol-containing samples compared to CTRL. However, as reported in Table 2 and detailed in Fig. 2 , CAR 37.5 and OA 37.5, differently from CO, displayed no significative difference in strain % compared to the lower plasticizer concentration. Oleic acid and Cardanol did not result in a noticeable increase in strain at break, despite causing a reduction in Young’s modulus. Conversely, Castor Oil displayed a stress–strain behaviour characterized by a progressive decrease in slope as the plasticizer concentration increased (see supplementary S.1). Elastic recovery was assessed by comparing the strain at the tenth cycle to that at the first cycle: a higher residual strain indicates a lower ability of the material to regain its original shape. The analysis of the maximum stress for cycle highlights that most of the max stress lowering occurs within the first 5 cycles (see Fig. 4 .b), ranging from 70–87% of the stress accumulated by the 10th cycle (see Supplementary S.2). Among the plasticizers, Cardanol retain high max stresses as much as CTRL and a similar value is observed in the CO 37.5 sample too (~ 80% of the initial maximum stress). Oleic Acid experimented the higher reduction in maximum stress after the test. Castor Oil had the best performance in the shape recovery, especially in the higher concentration, showing the lower residual deformation of ~ 7% (Fig. 3 .a-b). Among the plasticized materials, Oleic Acid (OA) exhibited the lowest elastic recovery, concurrently demonstrating the highest residual deformation and the minimal shape recovery (~ 10%). This observation is consistent with the plasticizing mechanism of small molecules such as OA, which likely acted as a lubricant within the Oleogel network [ 32 , 33 ]. This lubricating effect facilitated a reduction in accumulated stress, consequently leading to the diminished shape recovery. Generally, all the plasticizers have augmented the memory shape of the Oleogel showing less residual deformation between the first and the last compression stages. Wettability test Regardless of the plasticizer and its amount presence in the samples, none of the OGs proved to be hydrophobic (Table 3 , Supplementary S.3, S.4). The highest contact angle value is about 86° and it was performed by the OG with 37.5% of Oleic Acid as plasticizer while the lowest value showed by the OG with 25.0% of Castor Oil as plasticizer. Table 3 Contact Angles for each material. Material Contact Angle (°C) CTRL 69.0 ± 4 CAR 25.0 73.9 ± 2 CAR 37.5 68.0 ± 6 CO 25.0 48.1 ± 1 CO 37.5 73.6 ± 7 OA 25.0 65.5 ± 4 OA 37.5 86.5 ± 3 A positive correlation exists between contact angle and plasticizer concentration, except for cardanol, which exhibits a slight decrease (from 73.9° to 68.0°, see Table 3 ). FTIR – ATR To understand the chemical interactions between the solvent, the plasticizer, and the oleogelator, an FTIR analysis was performed. By comparing the FTIR spectra of EC, SBO, and OG, it is possible to observe that the Oleogel spectrum is a superposition of EC and SBO. The carbonyl double bond of SBO, visible at 1742 cm − 1 [ 34 ], and the OH- stretching at approximately 3500 cm − 1 [ 35 ] of EC appear at the same wavenumber in the OG spectra. Table 4 All characteristics groups of the materials used for the fabrication and plasticization of OGs are reported. Material Functional Groups Wavenumber (cm − 1 ) Ethyl Cellulose -OH C-O-C -CH 3500 1050 1750 Soybean Oil -CO 1742 Castor Oil -CO -OH 1730 1750 Cardanol -OH 3350–3400 Oleic Acid -CO -CH 1708 2850–3000 The same kind of superposition is visible when plasticizers are added to the OG (Supplementary S.5 and S.6). Indeed, when comparing Oleogels with the same plasticiser but with different amounts of plasticizer (i.e. with oil-plasticiser ratios 1:1 and 1:3), no particular differences can be detected other than slight differences in peak intensity. For example, the double peak of Oleogel where Oleic Acid is used as a plasticizer, is a superposition of the asymmetric stretch at 1708 cm⁻¹ of -C = O of the OA [ 36 ] and the peak due to the same group of SBO at 1742 cm − 1 [ 37 ] (Fig. 5 .c). Dynamic Thermo-Mechanical Analysis (DMTA) The gel temperature (T gel ) is defined as the point at which a material passes from a behaviour solid-like to a behaviour liquid-like and it’s identified as the crossover point between the elastic modulus G' and the viscous modulus G", i.e., the temperature at which G' = G" [ 38 ]. The effect of the plasticizer on T gel it’s variable: it shown substantial reductions for the Oleogel with 37.5% of Oleic Acid more than 50°C with respect to the Oleogel without plasticizer. The networking ability of EC is due to the formation H-bonds [ 39 ]; Oleic Acid, as a small molecule of fatty acid, interfere with the polymer matrix reducing the number of H-bonds and this has the effect to lower the gelation temperature of OG. Furthermore, the more is present the plasticizer the more the temperature falls (Fig. 6 b, supplementary S.7). Castor Oil has very little effect on T gel of OG because its high content of Ricinoleic Acid (90%) makes suitable a large number of H-bonds [ 29 ], favouring the formation of a stable structure. Cardanol shows an intermediate behaviour because has a more rigid structure due to the aromatic ring and the doble C = C bonds along the Carbon chain [ 40 ]. The presence of a transition between solid-like and liquid-like is confirmed by the peaks shown in the Differential Scanning Calorimetry (DSC) test (Supplementary S.8) Thermo-Gravimetric Analysis (TGA) Castor Oil (CO) does not appear to significantly affect thermal degradation, regardless of its concentration, as indicated by the similar values of T₁, T₂, and T₃ between CO-based samples and the control (CTRL). In contrast, Cardanol (CAR) and Oleic Acid (OA) have a pronounced impact on the onset degradation temperature (T₁), reducing it proportionally to their concentration. However, their effect on T₂ is less pronounced, and on T₃ it is negligible, suggesting that the final stage of degradation is predominantly governed by the decomposition of the polymeric matrix of OG rather than the plasticizer. The most significant effect in reducing T₁ and T₂, suggesting a greater susceptibility of the material to thermal degradation due to the platicizers with smaller molecule, like OA and CAR, in the early stages of the process. Further, it’s possible to detect a different mode of degradation: the CTRL sample and the samples with Castor Oil as a plasticizer have a single stage degradation process and in all the other cases the weight loss is a multistage process with no stable intermediate phase. The higher thermal stability of the base Oleogel and the ones with Castor Oil as plasticizer are consistent with the mechanical properties and the gelation temperatures of these materials. In fact, a higher number of H-bonds correspond to a higher energy required to break them: in one case by applying a mechanical stress and in the other by furnishing thermal energy. Oleic Acid (OA), like in the T gel test, exhibited the most significant effect in reducing T₁ and T₂. Conclusions This study demonstrated that is possible to modulate Oleogel’s properties through the use of green plasticizers. In particular, they significantly improved the elongation at break, the elastic recovery and the processability by lowering the T gel of the Oleogel, expanding its potential applications. Among the tested plasticizers, Cardanol proved to be the most effective in enhancing the material’s stretchability. Specifically, it increased the strain at break of the OG by over 450%. Additionally, it significantly lowered the gelation temperature. Castor Oil, on the other hand, exhibited a well-balanced plasticizing effect, increasing the strain at break while maintaining good mechanical properties with modulus at break remained unchanged compared to the non-plasticized Oleogel and a good elastic response as the cyclical compression test confirms. Furthermore, Castor Oil did not significantly alter the thermal and viscoelastic properties of the material. Oleic Acid had the most pronounced effect on the thermal and viscoelastic properties of the Oleogel, reducing the gelation point by more than 50°C. This trend was confirmed by TGA analyses. Finally, none of the tested plasticizers significantly affected the wettability of the material, which exhibited a stable and intermediate behaviour between hydrophobicity and hydrophilicity. TBC is not a good plasticizer because of its leakage at the concentrations studied. These findings suggest that Oleogel plasticized with green plasticizers can play a crucial role in developing sustainable bioplastics with enhanced properties, making them viable alternatives to traditional plastics in different fields where stretchability and processability play a crucial role, for example in the packaging industry or in the wearable devices. Future research will focus on further optimizing the formulations and the exploration in fields like 3D printing of the Oleogel, the production of conductive Oleogel, etc. The integration of these advanced materials into various applications could contribute significantly to reducing the environmental impact of plastic waste while promoting a circular economy. Declarations Author Contribution L.C. wrote the main manuscript, produced test, elaborated data with graphs, tables and images. M.W. done experimental part.M.F. Reviewd the manuscript, collaborated for analysis.C.D., A.S and C.C Reviewd the manuscript.L.L. Conceptualiced the experimental part and the methodology, reviewd the manuscript in all parts. Acknowledgments This work was supported by the European Union – Next Generation EU – National Recovery and Resilience Plan (PNRR), Mission 4 “Education and Research”, Component 1 “Enhancement of educational services from nurseries to universities”, Investment 4.1, D.M. 118/2023, CUP F83C23000930002. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. A.S. and L.L. acknowledge the support of the PNRR – MUR for the funding allocated to Research Initiatives for Innovative Technologies and Pathways in Healthcare and Assistance (Decree No. 931, June 6, 2022), under the ANTHEM project (AdvaNced Technologies for HumancentEred Medicine), CUP B53C22006710001. References Annual global plastic use In: Our World in Data. https://ourworldindata.org/grapher/plastic-waste-by-sector . Accessed 28 Nov 2024 Geyer R, Jambeck JR, Law KL (2017) Production, use, and fate of all plastics ever made. 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Mater Res Express 2:095010. https://doi.org/10.1088/2053-1591/2/9/095010 Farid Z, Abdennouri M, Barka N et al (2022) Study of the effect of pH, conditioning and flotation time on the flotation efficiency of phosphate ores by a soybean oil collector. J Met Mater Minerals 32:101–108. https://doi.org/10.55713/jmmm.v32i1.1212 Davidovich-Pinhas M, Barbut S, Marangoni AG (2015) The gelation of oil using ethyl cellulose. Carbohydr Polym 117:869–878. https://doi.org/10.1016/j.carbpol.2014.10.035 Laredo T, Barbut S, Marangoni AG (2011) Molecular Interactions of polymer oleogelation. Soft Matter. https://doi.org/10.1039/c0sm00885k Gartili A, Lapinte V, Caillol S et al (2025) CNSL-based plasticizers, a promising and sustainable alternative to phthalates, a review. RSC Sustain 3:81–111. https://doi.org/10.1039/D4SU00282B Additional Declarations No competing interests reported. Supplementary Files SupplementaryData.docx 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-7490012","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":514578328,"identity":"c82064c7-93ba-45e0-9579-5aa2d4b0e6cf","order_by":0,"name":"Luca Cafuero","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAABD0lEQVRIie2OMUvEMBTHXwjEJfTWHBXzFSIFUaj6VVoKmbzBxcXjrlLILcqt93E8Cu1SnDMIWgqdCy4FF3PlHITmbnXIb0hekvfL/wE4HP8Qb79PhrUDoAA4HQ7EovzeT3dtaDMoyNSRebI4fxRMh3qv2GIIS+oO5jdMlC91c63eT/lq+9Tc9yF4PLUoMmBQJExUZRDMVEtFFWfBJpL2wdgdMJTihdCS+DOVUwGx8mmUH1Jwj9IlEx8t8a+Mwtf16vuIQkxKzoQmxEdGAR0rfFCh7cVlVJRsWkl8/vxmBtN15lMpKSHRqDI5SRrdzR+ZVxbos3/Ib/k62X7RMDzj2et4zI7R36i93+FwOBzH+AH7ok77dJD7NQAAAABJRU5ErkJggg==","orcid":"","institution":"University of Salento","correspondingAuthor":true,"prefix":"","firstName":"Luca","middleName":"","lastName":"Cafuero","suffix":""},{"id":514578329,"identity":"bb1bdeab-9015-4dd0-aabc-13f483da4e4b","order_by":1,"name":"Muhammad Waheed","email":"","orcid":"","institution":"University of Salento","correspondingAuthor":false,"prefix":"","firstName":"Muhammad","middleName":"","lastName":"Waheed","suffix":""},{"id":514578330,"identity":"0aae060b-5728-4db8-80d2-42d82a420272","order_by":2,"name":"Marco Friuli","email":"","orcid":"","institution":"University of Salento","correspondingAuthor":false,"prefix":"","firstName":"Marco","middleName":"","lastName":"Friuli","suffix":""},{"id":514578331,"identity":"084633ac-d6bd-43c0-b06c-ed1a977eed11","order_by":3,"name":"Christian Demitri","email":"","orcid":"","institution":"University of Salento","correspondingAuthor":false,"prefix":"","firstName":"Christian","middleName":"","lastName":"Demitri","suffix":""},{"id":514578332,"identity":"95befd78-cf50-4bf8-8208-d6032d3c36d1","order_by":4,"name":"Alessandro Sannino","email":"","orcid":"","institution":"University of Salento","correspondingAuthor":false,"prefix":"","firstName":"Alessandro","middleName":"","lastName":"Sannino","suffix":""},{"id":514578333,"identity":"2002d8a4-c8d9-4a4c-8ebb-385b49135e36","order_by":5,"name":"Carola Corcione","email":"","orcid":"","institution":"University of Salento","correspondingAuthor":false,"prefix":"","firstName":"Carola","middleName":"","lastName":"Corcione","suffix":""},{"id":514578334,"identity":"5dc443e5-4e49-4bef-b0ae-c560b660f838","order_by":6,"name":"Leonardo Lamanna","email":"","orcid":"","institution":"University of Salento","correspondingAuthor":false,"prefix":"","firstName":"Leonardo","middleName":"","lastName":"Lamanna","suffix":""}],"badges":[],"createdAt":"2025-08-29 15:38:26","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7490012/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7490012/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":91348847,"identity":"10158d97-dc92-4809-bf1c-2042f4598126","added_by":"auto","created_at":"2025-09-15 14:16:28","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":1063507,"visible":true,"origin":"","legend":"\u003cp\u003eIn the upper part of the image are shown the cylindrical samples for the compression-decompression test, in the lower part are shown the dogbone specimen for the traction test. From left to right are shown, respectively, CTRL, CAR 25.0 and CAR 37.5.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/98d47dd3f7b6f323f5e46b4c.png"},{"id":91350330,"identity":"59978f73-19bc-409a-b477-de9e1d3186a3","added_by":"auto","created_at":"2025-09-15 14:32:28","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":181593,"visible":true,"origin":"","legend":"\u003cp\u003eTraction curves of all materials.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/88bd516e69ddccfc6e48e391.png"},{"id":91348845,"identity":"0c3dd3a2-5f4d-4cf5-8b41-7d76408a87b5","added_by":"auto","created_at":"2025-09-15 14:16:28","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":129031,"visible":true,"origin":"","legend":"\u003cp\u003ea)Residual strain at 10\u003csup\u003eth\u003c/sup\u003e cycle. b) Residual strain after Cycle 1, 3, 6 and 10 of all plasticized Oleogels compared to the CTRL.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/189117298e5fd18d2f1629f7.png"},{"id":91349997,"identity":"e4484af3-90e4-452a-b131-bb5769921aa3","added_by":"auto","created_at":"2025-09-15 14:24:28","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":188472,"visible":true,"origin":"","legend":"\u003cp\u003ea) Maximum stress at first compression stage. b) Maximum stress after each cycle for plasticized Oleogels compared to CTRL.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/b2ed5abce5f3cf0ffa035d69.png"},{"id":91348859,"identity":"b834a8df-f149-4f59-89d8-cdd338dc7193","added_by":"auto","created_at":"2025-09-15 14:16:29","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":449940,"visible":true,"origin":"","legend":"\u003cp\u003ea, b, c show, respectively, the sessile drop on OG-CAR 25, OG-CAR 37.5, OG-OA 37.5.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/380455869b143b4d3a4455f3.png"},{"id":91348850,"identity":"f291f76c-9220-4e2f-96a0-739e7532265d","added_by":"auto","created_at":"2025-09-15 14:16:28","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":64779,"visible":true,"origin":"","legend":"\u003cp\u003ea. The FTIR spectra of EC, SBO and the OG. b. All the spectra of OGs with different plasticizers. c. The double peak of the asymmetric stretch at 1708 cm⁻¹ of -C=O of the Oleic Acid and the peak of -C=O at 1742 of SBO.\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/c0cab02ec07c68dcbc17d00b.png"},{"id":91351765,"identity":"c08be2d1-0ef7-4405-b5af-7c8abd1735af","added_by":"auto","created_at":"2025-09-15 14:40:29","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":127338,"visible":true,"origin":"","legend":"\u003cp\u003ea) The crossover point represents the temperature at which the material's behaviour becomes liquid-like. b) In all cases but CO, the gelation temperature is strongly lowered by the plasticizer.\u003c/p\u003e","description":"","filename":"7.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/740929760ac6d030f302c6b8.png"},{"id":91350336,"identity":"2992b208-ef16-4e41-8ea6-1d38d525cc95","added_by":"auto","created_at":"2025-09-15 14:32:29","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":212401,"visible":true,"origin":"","legend":"\u003cp\u003eUnnumbered image in the Results and Discussion section.\u003c/p\u003e","description":"","filename":"8.png","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/168098779e1ccefb7d8c6456.png"},{"id":92606440,"identity":"befde65f-95e1-454f-8bae-2cbf35f77090","added_by":"auto","created_at":"2025-10-01 15:09:41","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2957533,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/91f1370f-eb63-4e91-9179-a2b574d5614b.pdf"},{"id":91349994,"identity":"95d49f36-da93-4f8a-a491-85178cf8f278","added_by":"auto","created_at":"2025-09-15 14:24:28","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":1970926,"visible":true,"origin":"","legend":"","description":"","filename":"SupplementaryData.docx","url":"https://assets-eu.researchsquare.com/files/rs-7490012/v1/f025c56fe289b3d3929f5d04.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"Effect of different natural plasticizers on Ethyl Cellulose Oleogel bioplastic","fulltext":[{"header":"Introduction","content":"\u003cp\u003ePlastics derived from petroleum are spread in everyday life, from the electronic devices to vehicle components and food packaging. In 2019, the packaging sector led plastic consumption over 146\u0026nbsp;million tons, with construction sector in second place with about 70\u0026nbsp;million tons [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e]. Nowadays, plastic waste is a major environmental issue, as 79% ends up in landfills or in the environment [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e], where it persists for centuries [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e, \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e], breaking into microplastics which are found in oceans, ice, drinking water, and food chains [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]. Plastic\u0026rsquo;s fossil fuel origin intensifies the problem, with plastic production accounting for 3\u0026ndash;5% of global CO\u003csub\u003e2\u003c/sub\u003e equivalent emissions, primarily during the production and conversion phases [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. Unfortunately, plastic\u0026rsquo;s success relay on many advantages due to their technical features, consequently it is not easy to find technically and cost comparable green alternatives.\u003c/p\u003e\u003cp\u003eThe main advantage of petroleum-derived plastics lies in their ability to be tailored for diverse applications using the same polymer [\u003cspan additionalcitationids=\"CR8 CR9\" citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]. Plasticizers play a key role in modifying mechanical properties, thermal stability, processability, and durability [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]. An effective plasticizer must exhibit high compatibility with the polymer matrix to prevent phase separation and migration over time while efficiently lowering the glass transition temperature [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e, \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e]. Additionally, it should possess low volatility to minimize evaporation during processing and use, as well as high thermal and chemical stability to withstand heat, UV exposure, and environmental stressors [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e]. Resistance to extraction by water, oils, or solvents is also essential, particularly in medical and food-related applications[\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e]. Phthalates are a widely used class of plasticizers, particularly in the production of vinyl medical products, such as intravenous tubing. The most commonly used phthalate is di-2-ethylhexyl phthalate (DEHP), which provides excellent gelling properties, remains relatively non-volatile under heat, enhances the electrical properties of compounds, and is favoured in medical devices for its ability to maintain flexibility at low temperatures while also withstanding high-temperature sterilization [\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]. Bisphenol A (BPA) is a commonly used plasticizer that enhances the mechanical properties of plastics by improving elasticity, thermal resistance, and moisture resistance, playing a crucial role as a monomer in the production of polycarbonate plastics and epoxy resins [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e]. On the other hand, some of most spread plasticizers have been found to have toxic effects on health [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eIn recent years, the shift towards bioplastics\u0026mdash;defined as materials derived from renewable sources and/or designed to be biodegradable or compostable\u0026mdash;has gained traction as a sustainable alternative aimed at reducing environmental impact throughout their lifecycle. Bioplastics, although currently representing only 0.5% of the global market [\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e], are experiencing growth. In particular, thermoplastic polyesters such as Polylactic acid (PLA), polyhydroxybutyrate (PHB), and polybutylene succinate (PBS) are among the most promising materials for consumer applications, owing to their balance of durability and biodegradability and production from renewable sources (e.g. PLA is mainly produced by the fermentation of starch plants such as from corn, sugarcane, etc. and the possibility to be compostable [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]).\u003c/p\u003e\u003cp\u003eHowever, these biopolymers are brittle. For example, PLA has a Young\u0026rsquo;s Modulus typically over 3 GPa, a strain at break about 5% [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e]. To expand its applications, various plasticizers have been tested, including Epoxidated Soybean Oil [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e] and Acetylized Tributyl Citrate [\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e] though issues like leaching and reduced performance remain challenges. PBS it\u0026rsquo;s a biodegradable aliphatic polyester [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e] with melting temperatures which range from ~\u0026thinsp;100\u0026deg;C to ~\u0026thinsp;120\u0026deg;C and with a tensile Modulus between ~\u0026thinsp;30 MPa and ~\u0026thinsp;700 MPa [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]. It\u0026rsquo;s used in food applications such as packaging, compostable bags, etc. [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e], and its properties were improved by augmenting branches in polymeric chain using 1,2,4-butane-triol or augmenting the PBS\u0026rsquo;s crosslinks density with Castor Oil or Rutin [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. Its brittleness and mechanical characteristics need to be improved for specific applications. PHB has a Young\u0026rsquo;s Modulus which ranges from 3 to 3.5 GPa with a ultimate strength around 30 MPa; its melting temperature is ~\u0026thinsp;170\u0026deg;C and, further, it has good barrier properties making it suitable for different field, from food packaging to biomedical applications [\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e, \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. A major challenge involves PHB\u0026rsquo;s difficulties in its processability and aging.\u003c/p\u003e\u003cp\u003eDeveloping high-performing, low-impact materials is key to establishing bioplastics as a sustainable alternative.\u003c/p\u003e\u003cp\u003eIn this study we focus on a promising biodegradable bioplastic class, Oleogels (OG) already proposed by our research group in the previous work [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. They are a particular class of gel-like thermoplastic polymers composed of Ethyl Cellulose (EC) as structuring polymer and vegetable oil as organic solvent. The oil is entrapped within the EC tridimensional network [\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e] as well as water is trapped in hydrogels [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e], and OG properties can be roughly modulated by changing EC concentration or oil type allowing to obtain a soft and jelly or a rigid bioplastic. Consequently, exactly as standard plastic and the other bioplastic, to extend the range of applications and make OG more competitive to standard plastics it is crucial to fine tune and enhance its properties.\u003c/p\u003e\u003cp\u003eIn this work we tested the effects on OG of different concentrations of naturally derived and green plasticizers presumably oil and EC compatible such as Cardanol (CAR, derived from cashew nutshell liquid [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e], Castor Oil (CO from the seeds of the Ricinus communis plant [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]), Oleic Acid (OA, a monounsaturated fatty acid found in nature [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]), and Tributyl Citrate (TBC, a gold standard as bioplastic plasticizer [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]). The goal was to identify the optimal green plasticizer that could provide enhanced performance while maintaining the biobased and biodegradable nature of the Oleogel.\u003c/p\u003e"},{"header":"Materials and Methods","content":"\u003cp\u003eEthyl Cellulose was produced by ChemPoint with viscosity in the range of 90\u0026ndash;110 mPa*s and a degree of substitution about 2.5 (48,9\u0026ndash;49,5%). For the OG was employed commercially available Soybean Oil (SBO), specifically Desantis, composed by 9\u0026ndash;13% of saturated fatty acid, 25\u0026ndash;33% mono-unsaturated, 55\u0026ndash;65% poly-unsaturated fatty acid [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. As plasticizers were employed Tributyl Citrateproduced by BCD Chemie under the name of Citrofol B1. Oleic Acid of technical grade 90% was purchased by Sigma \u0026ndash; Aldrich. Commercial Castor Oil Matt purchased from the local market. Cardanol was purchased from Oltremare (Bologna, Italy).\u003c/p\u003e\u003cp\u003eThe production of Oleogels followed the method described in [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. The difference in formulations was the Oil:Plasticizer ratio and two formulations were prepared: 25.0 and 37.5% w/w. An Oleogel without plasticizers was produced as control, named CTRL (Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\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\u003eCoded name of different Oleogels produced and characterized.\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\u003eMaterial Id\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003ePlasticizer\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e\u003cp\u003ePercentage\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCTRL\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003e-\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e\u003cem\u003e-\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCAR 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eCardanol\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e25.0\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCAR 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eCardanol\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e37.5\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCO 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eCastor Oil\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e25.0\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCO 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eCastor Oil\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e37.5\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eOA 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eOleic Acid\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e25.0\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eOA 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eOleic Acid\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e37.5\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eTBC 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eTributyl Citrate\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e25.0\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eTBC 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eTributyl Citrate\u003c/em\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e37.5\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003eTo produce OG dogbone ASTM D638 Type V specimens, the material was grinded after being frozen using liquid nitrogen (to facilitate grinding avoiding overwarming). OG pellets were hot pressed at 165\u0026deg;C and 25 Bar (2.5 MPa) into a specifically shaped mould.\u003c/p\u003e\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\u003ch2\u003eMechanical characterization\u003c/h2\u003e\u003cp\u003eThe mechanical traction test was performed at room temperature on a Lloyd LR50K-plus machine on dogbone ASTM D638 Type V. A speed of 5 mm/s a room temperature was used to execute the test, and it was repeated on 3 dogbone specimens until their failure.\u003c/p\u003e\u003c/div\u003e\n\u003ch3\u003eCyclical compression\u003c/h3\u003e\n\u003cp\u003eThe visco-elastic response of the materials was analysed through cyclic compression tests, with a particular focus on shape memory, i.e., the material's ability to return to its original configuration after the application and removal of a load. To evaluate the impact of plasticizers on the material, two parameters were considered: the residual strain and the residual stress.\u003c/p\u003e\u003cp\u003eThe residual strain is intended as the permanent strain after the load was removed in the last compression cycle; the residual stress has been calculated as percentage of the maximum stress reached in the first compression cycle.\u003c/p\u003e\u003cp\u003eThe cyclical compression test was performed at room temperature on a Lloyd machine on cylindrical specimens (4 mm in thickness and 14 mm in diameter) fabricated by hot-pressing with the same parameters of the dogbone specimen. The test consisted of 10 consecutive compression-decompression cycles. The compression stage was brought until 1 mm of deformation starting from the original size, then the load was removed, then applied again without time gap between cycles. The tests were performed on the Lloyd LR50K-plus machine at room temperature.\u003c/p\u003e\n\u003ch3\u003eDynamic Thermo-Mechanical Analysis (DTMA)\u003c/h3\u003e\n\u003cp\u003eGelation temperature was determined on a Malvern rheometer using a flat plate of 20 mm in diameter using a dynamic thermo-mechanical analysis (DTMA) with temperature ramp 25\u0026ndash;200\u0026deg;C with a heating rate of 5\u0026deg;C/min. The viscoelastic region was determined by an amplitude test after which the strain was set at 0.04% at a frequency of 0.4 Hz. The test consisted of the monitoring the elastic and the viscous moduli (respectively, G\u0026rsquo; and G\u0026rdquo;) by applying a mono-frequency shear strain on cylindrical shaped samples (0,5 mm in thickness and 15 mm in diameter) obtained from a hot-pressing process previously described.\u003c/p\u003e\n\u003ch3\u003eThermo-Gravimetric Analysis (TGA)\u003c/h3\u003e\n\u003cp\u003eA Thermo-Gravimetric Analysis test was conducted on the TGA Q500 instrument in the range 25\u0026ndash;550\u0026deg;C on pellet samples of 5\u0026ndash;10 mg at a flux of 10\u0026deg;C/min, on alumina crucibles. The tests were performed on an inert atmosphere with Nitrogen flux of 50 mL/min on the OGs pellets.\u003c/p\u003e\u003cp\u003eThe thermal stability of the materials was evaluated based on three key points of the degradation curve. The first point, T₁, corresponds to the temperature at which a 10% mass loss is recorded and is considered the onset of degradation. The second point, T₂, represents the temperature at which 50% of the mass is lost. Finally, the third point, T₃, marks the completion of degradation, when over 90% of the sample degraded.\u003c/p\u003e\n\u003ch3\u003eDifferential Scanning Calorimetry/ Differential Thermal Analysis – DSC/DTA\u003c/h3\u003e\n\u003cp\u003eThe DSC-DTA tests were conducted on machine DSC Q2500 (TA Instruments), in a temperature range of -30\u0026deg;C to 200\u0026deg;C at a rate of 5\u0026deg;C/min, on aluminium crucibles. The tests were performed on an inert atmosphere with Nitrogen flux of 50 mL/min using some pellet specimens of 10\u0026ndash;15 mg.\u003c/p\u003e\u003cdiv id=\"Sec8\" class=\"Section2\"\u003e\u003ch2\u003eFourier Transform Infrared Spectroscopy test \u0026ndash; FTIR\u003c/h2\u003e\u003cp\u003eFourier transform infrared spectroscopy (FT-IR) analysis, performed with a Jasco 6300 FT-IR spectrometer (JASCO Corporation, Tokyo, Japan), was used to characterize the single components and all the Oleogels. Infrared spectra were recorded in the wavelength range between 750 and 3,500 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 50 scans, and 4 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e of resolution, by using ATR Pro One X with ZnSe crystal.\u003c/p\u003e\u003c/div\u003e\n\u003ch3\u003eWettability Test\u003c/h3\u003e\n\u003cp\u003eThe wettability test was performed using the classical sessile drop test at room temperature. The drop of distilled water was carefully laid on the surface of a thin film (1 mm thickness) obtained by a hot-pressing process. The image was captured by a camera and the angles were measured by using First Ten Angstroms, FTA 1000 software (Newark, California, USA) equipped with a CDD camera. The test was repeated in triplicate.\u003c/p\u003e"},{"header":"Results and Discussion","content":"\u003cdiv id=\"Sec11\" class=\"Section2\"\u003e\u003ch2\u003eMechanical Test\u003c/h2\u003e\u003cp\u003eYoung\u0026rsquo;s Moduli E, maximum strength σ\u003csub\u003emax\u003c/sub\u003e and maximum elongation ε\u003csub\u003emax\u003c/sub\u003e were investigated.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003ePlasticizers reduced the elastic modulus (E) compared to CTRL by one order of magnitude (CAR and CO) or two (OA and TBC). Castor Oil and TBC 25.0 exhibited a slight increase, in ultimate tensile strength that was not statistically significative (Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e). Noteworthy, TBC samples exhibited oil leakage, leading to their results being reported but excluded from further discussion. In all other cases, tensile strength decreased, and for Cardanol and Oleic Acid, this reduction was proportional to their concentration in the sample.\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\u003eYoung Moduli, Max Stress and Max Strain of all sample tested\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=\"char\" char=\"\u0026plusmn;\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\"\u0026plusmn;\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\"\u0026plusmn;\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colname=\"c1\"\u003e\u003cp\u003eMaterial\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003eE (MPa)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e\u003cp\u003eStress (MPa)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c4\"\u003e\u003cp\u003eStrain (%)\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCTRL\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e136.3\u0026thinsp;\u0026plusmn;\u0026thinsp;1.7\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e10.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e38.2\u0026thinsp;\u0026plusmn;\u0026thinsp;2.2\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCAR 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e21.5\u0026thinsp;\u0026plusmn;\u0026thinsp;1.6\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e5.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.2\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e215.8\u0026thinsp;\u0026plusmn;\u0026thinsp;8.4\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCAR 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e11.3\u0026thinsp;\u0026plusmn;\u0026thinsp;4.0\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e2.4\u0026thinsp;\u0026plusmn;\u0026thinsp;0.3\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e200.5\u0026thinsp;\u0026plusmn;\u0026thinsp;29.8\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCO 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e41.5\u0026thinsp;\u0026plusmn;\u0026thinsp;3.2\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e11.5\u0026thinsp;\u0026plusmn;\u0026thinsp;0.9\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e158.9\u0026thinsp;\u0026plusmn;\u0026thinsp;21.5\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eCO 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e12.7\u0026thinsp;\u0026plusmn;\u0026thinsp;3.4\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e8.3\u0026thinsp;\u0026plusmn;\u0026thinsp;1.0\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e184.9\u0026thinsp;\u0026plusmn;\u0026thinsp;23.0\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eOA 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e22.4\u0026thinsp;\u0026plusmn;\u0026thinsp;3.5\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e5.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.3\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e147.4\u0026thinsp;\u0026plusmn;\u0026thinsp;9.9\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eOA 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e4.8\u0026thinsp;\u0026plusmn;\u0026thinsp;0.9\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e1.3\u0026thinsp;\u0026plusmn;\u0026thinsp;0.2\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e141.2\u0026thinsp;\u0026plusmn;\u0026thinsp;12.9\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eTBC 25.0\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e34.5\u0026thinsp;\u0026plusmn;\u0026thinsp;5.4\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e11.2\u0026thinsp;\u0026plusmn;\u0026thinsp;0.8\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e196.2\u0026thinsp;\u0026plusmn;\u0026thinsp;1.6\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e\u003cb\u003eTBC 37.5\u003c/b\u003e\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e8.9\u0026thinsp;\u0026plusmn;\u0026thinsp;3.3\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c3\"\u003e\u003cp\u003e3.5\u0026thinsp;\u0026plusmn;\u0026thinsp;0.5\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c4\"\u003e\u003cp\u003e221.2\u0026thinsp;\u0026plusmn;\u0026thinsp;39.6\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003eAs reported in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e, all plasticizers had an impact on strain at break increasing it up to ~\u0026thinsp;465% for the Cardanol-containing samples compared to CTRL. However, as reported in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e and detailed in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e, CAR 37.5 and OA 37.5, differently from CO, displayed no significative difference in strain % compared to the lower plasticizer concentration. Oleic acid and Cardanol did not result in a noticeable increase in strain at break, despite causing a reduction in Young\u0026rsquo;s modulus. Conversely, Castor Oil displayed a stress\u0026ndash;strain behaviour characterized by a progressive decrease in slope as the plasticizer concentration increased (see supplementary S.1).\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eElastic recovery was assessed by comparing the strain at the tenth cycle to that at the first cycle: a higher residual strain indicates a lower ability of the material to regain its original shape.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe analysis of the maximum stress for cycle highlights that most of the max stress lowering occurs within the first 5 cycles (see Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e.b), ranging from 70\u0026ndash;87% of the stress accumulated by the 10th cycle (see Supplementary S.2).\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eAmong the plasticizers, Cardanol retain high max stresses as much as CTRL and a similar value is observed in the CO 37.5 sample too (~\u0026thinsp;80% of the initial maximum stress). Oleic Acid experimented the higher reduction in maximum stress after the test.\u003c/p\u003e\u003cp\u003eCastor Oil had the best performance in the shape recovery, especially in the higher concentration, showing the lower residual deformation of ~\u0026thinsp;7% (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e.a-b). Among the plasticized materials, Oleic Acid (OA) exhibited the lowest elastic recovery, concurrently demonstrating the highest residual deformation and the minimal shape recovery (~\u0026thinsp;10%). This observation is consistent with the plasticizing mechanism of small molecules such as OA, which likely acted as a lubricant within the Oleogel network [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e, \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e]. This lubricating effect facilitated a reduction in accumulated stress, consequently leading to the diminished shape recovery.\u003c/p\u003e\u003cp\u003eGenerally, all the plasticizers have augmented the memory shape of the Oleogel showing less residual deformation between the first and the last compression stages.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec12\" class=\"Section2\"\u003e\u003ch2\u003eWettability test\u003c/h2\u003e\u003cp\u003eRegardless of the plasticizer and its amount presence in the samples, none of the OGs proved to be hydrophobic (Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e, Supplementary S.3, S.4).\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe highest contact angle value is about 86\u0026deg; and it was performed by the OG with 37.5% of Oleic Acid as plasticizer while the lowest value showed by the OG with 25.0% of Castor Oil as plasticizer.\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\u003eContact Angles for each material.\u003c/p\u003e\u003c/div\u003e\u003c/caption\u003e\u003ccolgroup cols=\"2\"\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\"\u0026plusmn;\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colname=\"c1\"\u003e\u003cp\u003eMaterial\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003eContact Angle (\u0026deg;C)\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCTRL\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e69.0\u0026thinsp;\u0026plusmn;\u0026thinsp;4\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCAR 25.0\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e73.9\u0026thinsp;\u0026plusmn;\u0026thinsp;2\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCAR 37.5\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e68.0\u0026thinsp;\u0026plusmn;\u0026thinsp;6\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCO 25.0\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e48.1\u0026thinsp;\u0026plusmn;\u0026thinsp;1\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCO 37.5\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e73.6\u0026thinsp;\u0026plusmn;\u0026thinsp;7\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eOA 25.0\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e65.5\u0026thinsp;\u0026plusmn;\u0026thinsp;4\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eOA 37.5\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\"\u0026plusmn;\" colname=\"c2\"\u003e\u003cp\u003e86.5\u0026thinsp;\u0026plusmn;\u0026thinsp;3\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003eA positive correlation exists between contact angle and plasticizer concentration, except for cardanol, which exhibits a slight decrease (from 73.9\u0026deg; to 68.0\u0026deg;, see Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e).\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec13\" class=\"Section2\"\u003e\u003ch2\u003eFTIR \u0026ndash; ATR\u003c/h2\u003e\u003cp\u003eTo understand the chemical interactions between the solvent, the plasticizer, and the oleogelator, an FTIR analysis was performed. By comparing the FTIR spectra of EC, SBO, and OG, it is possible to observe that the Oleogel spectrum is a superposition of EC and SBO. The carbonyl double bond of SBO, visible at 1742 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e[\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e], and the OH- stretching at approximately 3500 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e] of EC appear at the same wavenumber in the OG spectra.\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\u003eAll characteristics groups of the materials used for the fabrication and plasticization of OGs are reported.\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\u003eMaterial\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003eFunctional Groups\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e\u003cp\u003eWavenumber (cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e)\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eEthyl Cellulose\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e-OH\u003c/p\u003e\u003cp\u003eC-O-C\u003c/p\u003e\u003cp\u003e-CH\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e3500\u003c/p\u003e\u003cp\u003e1050\u003c/p\u003e\u003cp\u003e1750\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eSoybean Oil\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e-CO\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1742\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCastor Oil\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e-CO\u003c/p\u003e\u003cp\u003e-OH\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1730\u003c/p\u003e\u003cp\u003e1750\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eCardanol\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e-OH\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e3350\u0026ndash;3400\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eOleic Acid\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e-CO\u003c/p\u003e\u003cp\u003e-CH\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1708\u003c/p\u003e\u003cp\u003e2850\u0026ndash;3000\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003eThe same kind of superposition is visible when plasticizers are added to the OG (Supplementary S.5 and S.6). Indeed, when comparing Oleogels with the same plasticiser but with different amounts of plasticizer (i.e. with oil-plasticiser ratios 1:1 and 1:3), no particular differences can be detected other than slight differences in peak intensity.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eFor example, the double peak of Oleogel where Oleic Acid is used as a plasticizer, is a superposition of the asymmetric stretch at 1708 cm⁻\u0026sup1; of -C\u0026thinsp;=\u0026thinsp;O of the OA [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e] and the peak due to the same group of SBO at 1742 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e [\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e] (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e.c).\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec14\" class=\"Section2\"\u003e\u003ch2\u003eDynamic Thermo-Mechanical Analysis (DMTA)\u003c/h2\u003e\u003cp\u003eThe gel temperature (T\u003csub\u003egel\u003c/sub\u003e) is defined as the point at which a material passes from a behaviour solid-like to a behaviour liquid-like and it\u0026rsquo;s identified as the crossover point between the elastic modulus G' and the viscous modulus G\", i.e., the temperature at which G' = G\" [\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e]. The effect of the plasticizer on T\u003csub\u003egel\u003c/sub\u003e it\u0026rsquo;s variable: it shown substantial reductions for the Oleogel with 37.5% of Oleic Acid more than 50\u0026deg;C with respect to the Oleogel without plasticizer. The networking ability of EC is due to the formation H-bonds [\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]; Oleic Acid, as a small molecule of fatty acid, interfere with the polymer matrix reducing the number of H-bonds and this has the effect to lower the gelation temperature of OG. Furthermore, the more is present the plasticizer the more the temperature falls (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb, supplementary S.7).\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eCastor Oil has very little effect on T\u003csub\u003egel\u003c/sub\u003e of OG because its high content of Ricinoleic Acid (90%) makes suitable a large number of H-bonds [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e], favouring the formation of a stable structure. Cardanol shows an intermediate behaviour because has a more rigid structure due to the aromatic ring and the doble C\u0026thinsp;=\u0026thinsp;C bonds along the Carbon chain [\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]. The presence of a transition between solid-like and liquid-like is confirmed by the peaks shown in the Differential Scanning Calorimetry (DSC) test (Supplementary S.8)\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec15\" class=\"Section2\"\u003e\u003ch2\u003eThermo-Gravimetric Analysis (TGA)\u003c/h2\u003e\u003cp\u003eCastor Oil (CO) does not appear to significantly affect thermal degradation, regardless of its concentration, as indicated by the similar values of T₁, T₂, and T₃ between CO-based samples and the control (CTRL). In contrast, Cardanol (CAR) and Oleic Acid (OA) have a pronounced impact on the onset degradation temperature (T₁), reducing it proportionally to their concentration. However, their effect on T₂ is less pronounced, and on T₃ it is negligible, suggesting that the final stage of degradation is predominantly governed by the decomposition of the polymeric matrix of OG rather than the plasticizer.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe most significant effect in reducing T₁ and T₂, suggesting a greater susceptibility of the material to thermal degradation due to the platicizers with smaller molecule, like OA and CAR, in the early stages of the process.\u003c/p\u003e\u003cp\u003eFurther, it\u0026rsquo;s possible to detect a different mode of degradation: the CTRL sample and the samples with Castor Oil as a plasticizer have a single stage degradation process and in all the other cases the weight loss is a multistage process with no stable intermediate phase.\u003c/p\u003e\u003cp\u003eThe higher thermal stability of the base Oleogel and the ones with Castor Oil as plasticizer are consistent with the mechanical properties and the gelation temperatures of these materials. In fact, a higher number of H-bonds correspond to a higher energy required to break them: in one case by applying a mechanical stress and in the other by furnishing thermal energy. Oleic Acid (OA), like in the T\u003csub\u003egel\u003c/sub\u003e test, exhibited the most significant effect in reducing T₁ and T₂.\u003c/p\u003e\u003c/div\u003e"},{"header":"Conclusions","content":"\u003cp\u003eThis study demonstrated that is possible to modulate Oleogel\u0026rsquo;s properties through the use of green plasticizers. In particular, they significantly improved the elongation at break, the elastic recovery and the processability by lowering the T\u003csub\u003egel\u003c/sub\u003e of the Oleogel, expanding its potential applications. Among the tested plasticizers, Cardanol proved to be the most effective in enhancing the material\u0026rsquo;s stretchability. Specifically, it increased the strain at break of the OG by over 450%. Additionally, it significantly lowered the gelation temperature. Castor Oil, on the other hand, exhibited a well-balanced plasticizing effect, increasing the strain at break while maintaining good mechanical properties with modulus at break remained unchanged compared to the non-plasticized Oleogel and a good elastic response as the cyclical compression test confirms. Furthermore, Castor Oil did not significantly alter the thermal and viscoelastic properties of the material. Oleic Acid had the most pronounced effect on the thermal and viscoelastic properties of the Oleogel, reducing the gelation point by more than 50\u0026deg;C. This trend was confirmed by TGA analyses. Finally, none of the tested plasticizers significantly affected the wettability of the material, which exhibited a stable and intermediate behaviour between hydrophobicity and hydrophilicity. TBC is not a good plasticizer because of its leakage at the concentrations studied.\u003c/p\u003e\u003cp\u003eThese findings suggest that Oleogel plasticized with green plasticizers can play a crucial role in developing sustainable bioplastics with enhanced properties, making them viable alternatives to traditional plastics in different fields where stretchability and processability play a crucial role, for example in the packaging industry or in the wearable devices.\u003c/p\u003e\u003cp\u003eFuture research will focus on further optimizing the formulations and the exploration in fields like 3D printing of the Oleogel, the production of conductive Oleogel, etc. The integration of these advanced materials into various applications could contribute significantly to reducing the environmental impact of plastic waste while promoting a circular economy.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eL.C. wrote the main manuscript, produced test, elaborated data with graphs, tables and images. M.W. done experimental part.M.F. Reviewd the manuscript, collaborated for analysis.C.D., A.S and C.C Reviewd the manuscript.L.L. Conceptualiced the experimental part and the methodology, reviewd the manuscript in all parts.\u003c/p\u003e\u003ch2\u003eAcknowledgments\u003c/h2\u003e\u003cp\u003eThis work was supported by the European Union \u0026ndash; Next Generation EU \u0026ndash; National Recovery and Resilience Plan (PNRR), Mission 4 \u0026ldquo;Education and Research\u0026rdquo;, Component 1 \u0026ldquo;Enhancement of educational services from nurseries to universities\u0026rdquo;, Investment 4.1, D.M. 118/2023, CUP F83C23000930002. The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript.\u003c/p\u003e\u003cp\u003eA.S. and L.L. acknowledge the support of the PNRR \u0026ndash; MUR for the funding allocated to Research Initiatives for Innovative Technologies and Pathways in Healthcare and Assistance (Decree No. 931, June 6, 2022), under the ANTHEM project (AdvaNced Technologies for HumancentEred Medicine), CUP B53C22006710001.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eAnnual global plastic use In: Our World in Data. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://ourworldindata.org/grapher/plastic-waste-by-sector\u003c/span\u003e\u003cspan address=\"https://ourworldindata.org/grapher/plastic-waste-by-sector\" targettype=\"URL\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e. 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RSC Sustain 3:81\u0026ndash;111. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1039/D4SU00282B\u003c/span\u003e\u003cspan address=\"10.1039/D4SU00282B\" 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":"bioplastic, Ethyl Cellulose, Oleogel, green plasticizers, sustainability, biodegradability","lastPublishedDoi":"10.21203/rs.3.rs-7490012/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7490012/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eGrowing concerns about the environmental impact of fossil-based plastics has highlighted the need for bioplastics. Recently, Ethyl Cellulose-based Oleogels have been proposed as a promising bioplastic alternative due to their biodegradability, biocompatibility, and processability. However, Oleogels require improved plasticity to compete with traditional bioplastics, which are often brittle and difficult to process, limiting their ability to match conventional plastics. Plasticizers are a major bottleneck in the development of sustainable materials, as many are toxic to the environment. This study focused on plasticizing Oleogels using natural origin plasticizers, specifically, Cardanol, Castor Oil, Oleic Acid and Tributyl Citrate. The results demonstrate that these additives significantly influence the mechanical and processing properties of the material. The most effective plasticizers resulted are Cardanol, which increased the maximum elongation by ~\u0026thinsp;450% and reduced the gelation temperature by 15\u0026ndash;30\u0026deg;C compared to the plasticizer-free Oleogel, and Castor Oil, which enhanced elongation at break by about 380% while preserving the maximum load close to that of the plasticizer-free formulation. These findings highlight the potential of these bio-plasticizers in improving the mechanical and thermal properties of Oleogel-based materials.\u003c/p\u003e","manuscriptTitle":"Effect of different natural plasticizers on Ethyl Cellulose Oleogel bioplastic","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-09-15 14:16:24","doi":"10.21203/rs.3.rs-7490012/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":"69f9a9c6-be85-4394-87cd-4f9135a46709","owner":[],"postedDate":"September 15th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2025-10-01T14:57:48+00:00","versionOfRecord":[],"versionCreatedAt":"2025-09-15 14:16:24","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7490012","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7490012","identity":"rs-7490012","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}