The use of low-quality cotton-derived cellulose films as templates for in situ conductive polymer synthesis as promising biomaterials in biomedical applications

The use of low-quality cotton-derived cellulose films as templates for in situ conductive polymer synthesis as promising biomaterials in biomedical applications | 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 The use of low-quality cotton-derived cellulose films as templates for in situ conductive polymer synthesis as promising biomaterials in biomedical applications Sahin Demirci, Mehtap Sahiner, Shaida S. Rumi, Selin S. Suner, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4541295/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 Due to the growing interest in biopolymer-based composites in many applications, noticeable devotion has been directed to natural polymer-derived products not only because of their renewable and eco-friendly characteristics but also for their versatility in processing conditions and cost-effectiveness in fabricating the final products. Here, we report the use of cellulose films (CFs) produced from low-quality cotton as a template for in situ synthesis of well-known conductive polymers, e.g., polyaniline (PANI) and polypyrrole (PPY) via oxidative polymerization. Three successive monomer loading/polymerization cycles of aniline (ANI) and pyrrole (PY) within CFs as PANI@CF or PPY@CF were carried out to increase the extent of conductive polymer content. The contact angle (CA) for three times ANI and PPY loaded and polymerized CFs as 3PANI@CF and 3PPY@CF were determined as 26.3 ± 2.8 o and 42.3 ± 0.6 o , respectively. As the electrical conductivity is increased with increased number of conductive polymer synthesis within CF, the higher conductivity values, 3x10 − 4 ±8.1x10 − 5 S.cm − 1 and 2.1x10 − 3 ±5.8x10 − 4 S.cm − 1 , respectively were measured for 3PANI@CF and 3PPY@CF composites that were approximately 3.3K-fold and 30K-fold higher, respectively, compared to bare CF. It was also found that PANI@CF composites are hemolytic, whereas PPY@CF composites are not at 1 mg/mL concentrations. In the presence of 1 mg of CF-based conductive polymer composites, all PPY@CF composites exhibit better biocompatibility than PANI@CF composites on L929 fibroblast cells with 81 ± 9, 71 ± 8, and 70 ± 8% cell viability for 1PPY@CF, 2PPY@CF, and 3PPY@CF composites, respectively. Moreover, the minimum inhibition concentration (MIC) and minimum bactericidal concentration (MBC) of 3PPY@CF composites for Escherichia coli ATCC8739, Staphylococcus aureus ATCC6538 are determined as 2.5 and 5 mg/mL, whereas these values were estimated to 5 and 10 mg/mL for Candida albicans ATCC10231. cotton derived cellulose films cellulose-conductive polymer composite conductive cellulose antimicrobial cellulose composite Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 1. Introduction Fossil fuels dominate the materials currently used in various industries. The urgent concerns about climate change and plastic pollution have spurred the the development of a bioeconomy, which involves substituting petroleum-based products with materials of biological origin or bio-based materials and with biodegradable alternatives (Wang et al. 2021 ). An effective approach to address this issue is to utilize eco-friendly products. The benefits of ecologically friendly materials include non-toxicity, capacity to be sustained over time, and inherent biodegradability (Khamwongsa et al. 2022 ). The need to establish a sustainable consumption has initiated exploration into utilizing natural cellulose as a substitute for non-renewable resources in many applications (Du et al. 2017 ; Chen et al. 2020 ; Liu et al. 2020 ). Cellulose has gained significant attention as a distinctive material due to its several inherent characteristics, including biodegradability, renewability, and widespread availability (Rodrigues et al. 2019 ; Chen et al. 2020 ; Liu et al. 2020 ). Cellulose is progressively recognized as a versatile source material for various applications, serving as a flexible biopolymer capable of producing hydrogels for absorbents, aerogels for insulation, membranes for filters, films for packaging, fibers for textiles and reinforcements, (Wang et al. 2021 ). Cellulose and its derivatives are commonly utilized in food packaging (Saedi et al. 2021 ), wound dressing (Tudoroiu et al. 2021 ), and many other biomedical applications (Aditya et al. 2022 ; Hasanin 2022 ), as cellulose based materials are readily biodegradable, and their degradation products are compatible with living organisms. Some intriguing and remarkable organic materials, known as conducting polymers (CPs), are thought to possess special electrical and optical qualities analogous to those of inorganic semiconductors and metals. It is possible to synthesize CPs in an easy, adaptable, and economical manner (Nezakati et al. 2018 ; K and Rout 2021 ). Different approaches have been devised to adapt and adjust methods to prepare CPs to enable their integration and interaction with biological environments in biomedical applications such as biosensors and diagnostic devices (Runsewe et al. 2019 ; Maziz et al. 2021 ). These materials are continually sought for a number of biomedical uses, including bioengineering, regenerative medicine, and biosensors (Balint et al. 2014 ; Distler and Boccaccini 2020 ; Lee et al. 2020 ). Some examples of common conductive polymers are polyacetylene (PA), polyaniline (PANI), polypyrrole (PPY), polythiophene (PTH), poly(para-phenylene) (PPP), poly(phenylenevinylene) (PPV), and polyfuran (PF ) (Nambiar and Yeow 2011 ; Nezakati et al. 2018 ; Guo and Facchetti 2020 ). Amongst them, the two conductive polymers most frequently employed are PANI (Zare et al. 2020 ; Bednarczyk et al. 2021 ; Beygisangchin et al. 2021 ) and PPY(Ateh et al. 2006 ; Kim et al. 2016b ; Samwang et al. 2023 ). Conductive polymers and their composites have a wide range of applications, including photo-catalysis (Kumar et al. 2020 ), anti-corrosion coatings (Racicot et al. 1995 ), biomedical tools (Zare et al. 2020 ; Hasanin 2022 ), energy storage materials (Kim et al. 2016a ), and sensing devices (Wang et al. 2020 ). In this study, cellulose films (CFs) prepared from low-quality cotton were used as templates for in-situ synthesis of PANI and PPY conductive polymers. Structural and thermal characterization of the prepared CF-based conductive polymer composites, referred to as PANI@CF and PPY@CF, were performed to ascertain the relevant functional groups. The change in wettability properties of CF-based conductive polymer composites upon multiple ANI and PY monomer loading/polymerization cycles was investigated. The effect of multiple monomer loading/polymerization cycles on the conductivity of CF-based composites was also examined. Furthermore, blood compatibility of the CF-based materials was evaluated via hemolysis% and blood clotting index% (BCI) assays. Moreover, the cytotoxicity of CF-based composites on L929 fibroblast cells was investigated. The antimicrobial activity of CF-based conductive polymer composites was also analyzed against Escherichia coli ATCC8739 ( E. coli ), Staphylococcus aureus ATCC6538 ( S. aureus ), or Candida albicans ATCC10231 ( C. albicans), microorganisms. 2. Experimental 2.1 Materials Extra pure DMAc (N, N-Dimethylacetamide, 99%, A0403006) and anhydrous LiCl (Lithium chloride, 99%, A0386841) were purchased from Acros Organics™ (NJ, USA). Glycerol (202397, certified ACS) was purchased from Fisher Scientific (MA, USA). Low-quality cotton was collected from the Fiber and Biopolymer Research Institute (FBRI, Texas Tech University Lubbock, TX, USA). Ammonium persulfate (APS, 98%, Sigma-Aldrich) was employed as an oxidation agent in hydrochloric acid (HCl, 36–38%, Sigma Aldrich) for the oxidative polymerization of aniline (ANI, 98%, Sigma Aldrich) for the in-situ production of conductive polymer within CFs. Also, pyrrole (PY, 98%, Aldrich) was used as received for the synthesis of poly(pyrrole) (PPY). Iron (III) chloride anhydrous (FeCl 3 , 99%, Acros) solution in water was employed as an initiating system. Diiodomethane (99%, Alfa Aesar) was used for SFE calculations. In the cytotoxicity analysis, L929 fibroblast cells (Mouse C3 and connective tissue) were obtained from SAP Institute, Ankara, Turkey. Trypsin (0.25%, EDTA 0.02% in PBS), Dulbecco’s Modified Eagle’s Medium (DMEM, with 4.5 g/L glucose, 3.7 g/L sodium pyruvate, L-Glutamine 0.5 g/mL), fetal bovine serum (FBS, heat-inactivated), and penicillin/streptomycin (10,000 U/mL penicillin, 10 mg/mL streptomycin) were products of Pan Biotech GmbH. Dimethyl sulfoxide (DMSO, 99.9%, Carlo Erba), trypan blue (0.5% solution, Biological Industries), and 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT agent, BioFroxx) were used as received. Gram-negative bacteria Escherichia coli (( E. coli , ATCC8739), Gram-positive bacteria Staphylococcus aureus ( S. aureus , ATCC6538), and yeast Candida albicans ( C. albicans , ATCC10231) were acquired from KWIK-STIK™ Microbiologics (St. Cloud, Minnesota, USA) for antibacterial activity tests. Nutrient agar (NA, Difco), and potato dextrose agar (Difco) as solid growth media and nutrient broth (NB, RPI, Merck, Darmstadt, Germany) as a liquid medium were used as received. 2.2 Purification of cotton fibers Raw cotton (micronaire = 2.4) was cleaned three times using a Microdust and Trash Monitor (MTM). Then, cotton fibers were scoured and bleached in order to obtain purified cotton cellulose. For the scouring process, cotton fibers were boiled in an alkaline scouring solution (liquor ratio 1:10) containing a non-ionic wetting agent-Triton-X 100 (1 g/L) and high concentration of NaOH (8 g/L) at 90°C for 1 h. After that, the solution was poured off and cotton was rinsed with fresh water. The scoured fibers were boiled in a bleaching solution (liquor ratio 1:10) containing wetting agent - Triton-X 100 (0.25 g/L), NaOH (0.35 g/L), sodium silicate (3 g/L), sodium carbonate (0.7 g/L), and sodium hypochlorite (6 g/L) at 90°C for 90 min. Purified cotton fibers were then boiled in fresh water at 90°C for 20 min and neutralized with 0.25g/L acetic acid. Finally, the purified cotton was air-dried for the next use. The air-dried cotton fibers were opened twice using the Microdust and Trash Monitor (MTM). 2.3 Dissolution of cotton fibers and cellulose film preparation Scoured and bleached cotton fibers were dissolved in DMAc/LiCl solvent system. Initially, oven-dried cotton fibers (105°C, 24 h) were added to a hot DMAc solution at 80°C (1% w:v) and stirred for 30 min. Subsequently, oven dried LiCl (8% w: v) was added to the solution, and stirring was continued for another 3 h at 80°C. Following that, the temperature was lowered to 50°C, and the dissolution was carried out overnight. Afterward, the solution was transferred to an oven (105°C) for 12 h. Then, the solution was taken out of the oven and allowed to reach room temperature. Cellulose solution was poured into glass molds and left inside a fume hood for 24 h. Deionized (DI) water was used to regenerate the gelated films for five days. After two days of plasticization with a 30% aqueous glycerol (w:v) solution, the regenerated cellulose films were hot-pressed for 15 min at 120°C. 2.4 In situ conductive polymer synthesis within cellulose films For the preparation of conductive polymer containing cellulose films as composites, a previous protocol from our research group was followed with some modifications (Sahiner and Demirci 2016 , 2017 ). For this purpose, the cellulose films (CFs) were cut into several pieces with a size of 1.5x1.5 cm, and each piece was placed into 5 mL of aniline (ANI) and pyrrole (PY), separately, and stirred at 250 rpm for 12 h to load the relevant monomers into CFs. Then, the ANI and PY loaded CFs were polymerized in situ as conductive polymer@CF composites, as given below. 2.4.1 Preparation of PANI@CF composites The ANI loaded CF pieces were placed into 10 mL of DI water and decanted after stirring for 1 min to remove un-adsorbed ANI molecules, and this washing procedure was repeated three times. Next, 20 mL of solutions of APS in 1 M HCl were freshly prepared by dissolving 1 g of APS in 20 mL 1M HCl solution, and the ANI loaded CF pieces were placed into these solutions separately. The in-situ polymerization reactions of ANI monomers within CF pieces were carried out for 12 h under constant stirring at 250 rpm at room temperature. Finally, the prepared 1PANI@CF composites were separated from the solution via decantation of supernatant and were washed via stirring in 10 mL of fresh DI water (x3), and ethanol (x1) each for 1 min. The washed 1PANI@CF composites were dried in an oven at 50 o C, and the ANI monomer loading/polymerization step was employed two more times to prepare 2PANI@CF, and 3PANI@CF composites. The prepared 1PANI@CF, 2PANI@CF, and 3PANI@CF composites were stored in closed tubes for characterization and further use. 2.4.2 Preparation of PPY@CF composites Firstly, the CF pieces loaded with PY were rinsed according to the previously described method to eliminate any remaining un-loaded PY monomers from the CFs, repeating the process three times with DI water. Subsequently, each PY-loaded CF piece was submerged in freshly prepared 20 mL of 0.5 M FeCl 3 solution and stirred at 250 rpm for 12 h at room temperature to facilitate the in-situ polymerization of the loaded PY monomers within the CFs. The prepared 1PPY@CF composites were then separated from the supernatant and washed using the same process mentioned above. Similarly, the washed and dried 1PPY@CF composites were used to prepare 2PPY@CF and 3PPY@CF composites through repeated cycles of PY monomer loading and polymerization, as detailed above. These composites, 1PPY@CF, 2PPY@CF, and 3PPY@CF were stored in sealed containers for subsequent use. 2.5 Biomedical properties of PANI@CF and PPY@CF composites The details of the biomedical properties of conductive polymer containing CF composites were evaluated via hemocompatibility, biocompatibility, and antimicrobial assays, and the relevant details were provided in Supporting Information . 3. Results and discussion 3.1 Structural characterization of conductive polymer@CF composites Previously, Rumi et al. reported successful preparation of transparent and strong cellulose films (CFs) from low quality cotton fiber through dissolution, casting, regeneration, plasticization, and hot-pressing (Rumi et al. 2021 ). They exhibited improved stretchability, homogeneity, flexibility, and deformation recovery upon glycerol plasticization. According to the findings, plasticizing films containing 30% aqueous glycerol (w:v) had the highest deformation recovery, whereas adding more glycerol resulted in even weaker and more fragile films (Rumi et al. 2021 ). Therefore, in this investigation, cellulose film (CF) plasticized with 30% glycerol was used as a matrix for the in-situ synthesis of conductive polymer. The schematic presentation of in-situ conductive polymer synthesis within CF is given in Fig. 1 (a) and (b) . It was noticed that the transparent CFs (size: 1.5x1.5 cm 2 ) changed colors upon placing into aniline (ANI) (slight yellow) and pyrrole (PY) (brownish) monomers. Upon polymerization of loaded ANI and PY monomers within CFs via oxidative polymerization technique (Wu et al. 1991 ; Moon et al. 2007 ; Kumar Sharma et al. 2015 ), as shown in Fig. 1 , a dark black coloration within CFs was observed for both composites. The in-situ polymerization of ANI within CF pieces was carried out in APS/HCl solution (Tang et al. 2011 ). In contrast, in-situ polymerization of PPY within CF pieces was carried out in aqueous FeCl 3 solution (Beneventi et al. 2006 ). Several studies have reported that the radical coupling mechanism occurs in the chemical polymerization of both ANI and PY (Ballav and Biswas 2004 ; Ahmed 2004 ; Tan and Ghandi 2013 ; Grzybowski et al. 2020 ; Peng et al. 2021 ). Thus, the visual dark black appearance (Fig. 1 ) of the resultant composite confirmed successful synthesis of conductive polymer within CF matrixes. Furthermore, the in-situ synthesis of PANI and PPY conductive polymers was repeated up to three times in order to enhance the amount of conductive polymer within CF matrices. Therefore, to increase the amount of conductive polymer within CFs matrices, the in-situ synthesis of PANI and PPY conductive polymers within CF pieces was were carried out up to three times, repetitively. For this purpose, the prepared 1PANI@CF and 1PPY@CF pieces were placed in ANI and PY monomers to load more of the related monomers into corresponding CFs by mixing at 250 rpm for 12 h again. Next, the excess amount of monomer from the surface of ANI and PY loaded 1PANI@CF and 1PPY@CF pieces were gently removed with a paper tissue. Then, the ANI and PY loaded 1PANI@CF and 1PPY@CF pieces were placed into initiators solutions, which what is APS:HCl solution for polymerization of ANI, and aqueous FeCl 3 solution for polymerization of PY within 1PANI@CF and 1PPY@CF pieces, respectively. For the third loading/polymerization cycles of ANI and PY within CFs, the same procedure was applied to 2PANI@CF and 2PPY@CF pieces, as mentioned above. FT-IR spectra of CFs, PANI@CFs, and PPY@CFs were collected to confirm the in-situ synthesis of the conductive polymer in the matrix. Also, the FT-IR spectra after the multiple monomersloading and then in situ conductive polymer synthesis within CFs, for PANI@CFs, and PPY@CFs were recorded and shown in Fig. 2 . The most noticeable standing out peaks in FT-IR spectra of CFs were broad -OH stretching vibrations at 3287 cm − 1 , -OH bending at 1655 cm − 1 , and -CH 2 scissoring at 1459 cm − 1 , C-H bending at 1314 cm − 1 , asymmetric ring stretching at 1112 cm − 1 , C-O stretching at 1032 cm − 1 , and beta linkage of cellulose at 853 cm − 1 , respectively (Rumi et al. 2021 ). On the other hand, the peaks at 2994 and 2881 cm − 1 assigned to -CH stretching from glycerol were also observed (Rumi et al. 2021 ). The FT-IR spectrum of 1PANI@CF composite exhibited the distinctive peak for PANI at 1580 cm − 1 associated with benzenoic–quinonic nitrogen vibration (John et al. 2010 ; Ahmad et al. 2016 ) along with CF peaks (Fig. 2 (a)) . In the FT-IR spectra of 2PANI@CF and 3PANI@CF composites, all of the peaks found for neat CFs almost disappeared, with the exception of the peaks arising from cellulose between 1100 − 800 cm − 1 . Nevertheless, the intensity of the peak at 1580 cm − 1 increased as the number of in situ PANI synthesis increased. The spectra also showed the appearance of additional vibration bands that were characteristics of PANI, including aromatic C–C peaks at 1478 cm − 1 , aromatic amine peaks at 1285 cm − 1 , and C–N–C peaks at 1146 cm − 1 (John et al. 2010 ; Ahmad et al. 2016 ; Sahiner and Demirci 2017 ). Besides, the FT-IR spectra of PPY@CFs displayed in Fig. 2 (b) revealed the disappearance of almost all peaks observed in the FT-IR spectra of neat CFs, such as the peaks originating from cellulose in the range of 1100 − 800 cm − 1 , even after the first synthesis of PPY within CFs. Consequently, there were newly appeared peaks with higher intensity as the number of polymerization cycles increased. These included -C = C peak at 1701 cm − 1 , fundamental PPY ring vibration at 1539 cm − 1 , N–C stretching vibrations at 1288 cm − 1 , and out-of-plane bending of C-H at 976 cm − 1 , deriving from PPY (Sahiner and Demirci 2017 ). These spectroscopic changes related to respective conductive polymers confirmed their effective synthesis within the matrix and the increase of their quantity with each synthesis cycle. Furthermore, the thermal degradation profiles of bare CF, PANI@CF, and PPY@CF are illustrated in Fig. 2 (c) , and (d) , respectively. A significant weight loss was observed for CF between 150–240 o C, accounting for an 80.3% reduction, attributed to glycerol decomposition (Rumi et al. 2021 ). Additionally, the observed cumulative weight loss of 92.8% between 270–315 o C was related to the decomposition of cellulose (Rumi et al. 2021 ). The weight of 1PANI@CF decreased by 12.7% between 165–195 o C (Fig. 2 (c) ), an indication of a lesser amount of glycerol content in the composite due to the presence of PANI. In addition, the weight loss in the range of 200–460°C and 465–650 o C, corresponding to 45.3% and 95.3% reduction, could be ascribed to the decomposition of cellulose and PANI, respectively. Similarly, the weight losses in the temperature range of 160–230°C were 22.7% and 8.4% for 1PPY@CF and 3PPY@CF, respectively. In addition, the respective recorded weight losses between 200–460°C were 42.2% and 30.9% for 1PPY@CF and 3PPY@CF. The cumulative weight loss at 700 o C exceeded 99% for 1PPY@CF and was 94.7% for 3PPY@CF, respectively. These findings indicated that PANI@CF and PPY@CF composites exhibited greater thermal stability compared to CF, as the presence of PANI and PPYs in the CFs cellulose afforded excellent thermal degradation profile due to the interactions between the guest polymers (PANI or PP) and the host, CF (Stejskal et al. 2005 ). Also, the thermal degradation behavior of CFs and its’ situ prepared PPY composites were compared, and the corresponding results were illustrated in Fig. 2 (d) . It was also noted that the in-situ preparation of PPY within CFs caused removal of glycerol from structure pertaining to decrease in weight losses at 160–230 o C range with 22.7, and 8.4% weight losses for 1PPY@CF, and 3PPY@CF respectively. The weight loss in 200–460°C range was determined as 42.2, and 30.9% for 1PPY@CF, and 3PPY@CF, respectively. The cumulative weight loss at 700 o C was > 99, and 94.7% for 1PPY@CF, and 3PPY@CF correspondingly. It can be presumed that after three loading/polymerization cycles of PANI and PPY within CFs, the amount of glycerol is decreased due the replacement of it with ANI and/or PY because of the increased amount of PANI and PPY within CF upon their individual polymerizations were observed. Also, it is reasonable to conclude that PANI@CF and PPY@CF composites have higher thermal stability than bare CF, as the presence of PANI and PPYs in the CFs cellulose afford new thermal degradation profiles due to their interactions between the guest (PANI or PP) and the host, CF (Stejskal et al. 2005 ). The amounts of PANI and PPY synthesized within CF pieces upon in-situ polymerizations were determined gravimetrically following each loading/polymerization cycle, and the corresponding results are summarized in Table 1 . The FT-IR analysis indicated the replacement of glycerol from the CF structure even during the initial monomer loading/polymerization procedure. To quantify the amount of PANI and PPY synthesized with or insitu in CFs, five pieces of CF (1.5x1.5 cm 2 ) were washed in 50 mL of water for 24 h, and after drying, their weight was measured as the control. The digital camera images of washed and dried CF and conductive polymer@CF composites are shown in Figure S1 . It was noticed that the CFs wrinkled, visibly hardened, and became more brittle after washing and drying. Table 1 The amount of in-situ synthesized conductive polymers within CFs upon multiple monomer loading/polymerization cycles. Weight of bare CF (mg) * CF-based composites Amount of in situ synthesized conductive polymers within CFs (mg.g − 1 ) / (mmoles)** Numbers of conductive polymer loading 1 2 3 23.2 ± 1.9 PANI 176.6 ± 10.2 / 1.9 ± 0.1 355.7 ± 26.8 / 3.8 ± 0.3 724.8 ± 99.7 / 7.8 ± 1.1 PPY 231.1 ± 39.6 / 3.4 ± 0.6 595.1 ± 62.7 / 8.9 ± 0.9 833.8 ± 25.3 / 12.4 ± 0.4 * The weight of CFs was measured after washing in water for 24 h. ** mmoles were calculated according to repeating units of related conductive polymers. The average weight of five pieces of CF was 93.2 ± 8.1 mg, which decreased to 23.2 ± 1.9 mg after 24 h of washing in water. This reduction indicated the removal of 75.1 ± 2.0% of glycerol from the structure, a finding consistent with the TGA results presented in Fig. 2 (b) . The quantities of PANI in CF after 1, 2, and 3 cycles of monomer loading/polymerization were measured as 176.6 ± 10.2, 355.7 ± 26.8, and 724.8 ± 99.7 mg. g − 1 , respectively, illustrating an increase in polymer content within the CF with each successive cycle. Likewise, the quantities of PPY in 1PPY@CF, 2PPY@CF, and 3PPY@CF were determined to be 231.1 ± 39.6, 595.1 ± 62.7, and 833.8 ± 25.3 mg.g − 1 , respectively. This demonstrated that the amount of in situ synthesized PANI increased from 1.9 ± 0.1 to 7.8 ± 1.1 mmoles (based on repeating unit of PANI) through successive monomer loading and polymerization cycles, while the amount of in situ synthesized PPYs within CFs increased from 3.4 ± 0.6 to 12.4 ± 04 mmoles (based on repeating unit of PPY) . 3.2 The wettability properties of conductive polymer@CF composites The wetting ability of CFs and conductive polymer@CF composites were assessed through contact angle (CA) measurements. A droplet of 10 µL of DI water was deposited on the samples. As per our previous study, the contact angle of water on plasticized CFs was 80 o . The decrease in CA was attributed to the inherent hydrophilicity of glycerol (Rumi et al. 2021 ). The CA value of 11.6 ± 0.4 o for CF was determined in this study after washing and drying whereas the contact angle value was measured as 90.6 ± 3.7 o before washing and drying and corresponding values compared in Fig. 3 (a) . The CA values were determined in two different states. The first state, referred to as ‘as is’, involved measuring the contact angles of composites immediately after the completion of the in-situ conductive polymer synthesis process. Water from the sample surface was wiped off before taking the measurement. In the second state, the composites were in their dried forms. Bare CF (‘as is’) was washed and also dried to make a comparison of CA with composites in the second state. The CA of dried CF increased to 90.6 ± 3.7 o from 11.6 ± 0.4 o due to the loss of hydrophilic glycerol. The measured CA values (‘as is’ state) for 1PANI@CF, 2PANI@CF, and 3PANI@CF composites were calculated as 42.9 ± 0.6, 39.5 ± 1.9, and 26.3 ± 2.8 o , respectively, which were at least 2-fold higher than bare CF (11.6 ± 0.4 o ). The CA of PANI@CF composites after washing and drying, increased as well to 86.5 ± 1.6, 65.5 ± 1.3, and 38.7 ± 08 o for consecutive cycle of polymerization, although remaining lower than bare CF. The images of water droplets on CF and PANI@CF composites in both states were given in Figure S2 . In both instances, it was observed that wettability of the composites increased with increase of PANI content in the substrate. This phenomenon could be explained by the fact that PANI structures transform into the emeraldine salt during polymerization in the presence of HCl. PANI is relatively hydrophobic in emeraldine base form, and its water CA value is between 94 − 84 o (Liu et al. 1994 ; Shishkanova et al. 2005 ). On the other hand, the emeraldine salt form of PANI occurred in the presence of acid such as HCl, HNO 3 , etc. shows lower contact angles (Zhang et al. 2002 ; Blinova et al. 2008 ). The SFE values for CF in ‘as is’ form was 71.1 ± 0.1 mN/m (CA is 11.6 ± 0.4 o ), whereas it was 56.9 ± 0.5, 59.8 ± 1.3, 66.2 ± 1.4 mN/m for PANI@CF 1PANI@CF, 2PANI@CF, and 3PANI@CF, respectively, as fiven in Fig. 3 (b) . On the other hand, the surface free energy (SFE) for washed and dried CF was 34.2 ± 0.6 mN/m, while SFE was 35.8 ± 0.5, 43.1 ± 1.8, 65.4 ± 1.1 mN/m for dried PANI@CF 1PANI@CF, 2PANI@CF, and 3PANI@CF, respectively. The calculated SFE values are in agreement compatible with the calculated CA values for each related CF-based structure prepared in this study. In contrast, it was found that monomer loading/polymerization cycle had a positive impact on increasing CA of PPY@CF composites as illustrated in Fig. 3 (c) . The CA values for 1PPY@CF, 2PPY@CF, and 3PPY@CF composites increased to 57.6 ± 1.4, 60.7 ± 1.2, and 66.8 ± 1.0 o in the second state from 24.9 ± 0.2, 25.3 ± 1.1, and 42.3 ± 0.6 o , respectively. The photographs of water droplet on PPY@CF composites are given in Figure S3 . The CA of composites increased with the increased amount of PPY in the matrix. Similarly, a study by Fraser and van Zyl also reported the increase of CA from 35.8° to 48.5 ° with an increase of polymerization time from 50 min to 20 h for the bacterial cellulose-PPY composites (Fraser and van Zyl 2022 ). Another study also noted that covering individual cellulose fibers with a continuous PPy coating led to decreased capillary forces, thereby enhancing the contact angle between water and the composite fibers. Additionally, the presence of PPy hindered the formation of hydrogen bonds between the individual fibers when they were in a dry state (Nyström et al. 2010 ). The SFE values for PPY@CF composites were found to decrease with the increasing value of CA after multiple PPY loading/polymerization cycles (Fig. 3 (d)) . The ‘as is’ SFE value for 1PPY@CF, 2PPY@CF, and 3PPY@CF composites were calculated as 68.7 ± 0.7, 66.3 ± 0.5, and 60.4 ± 1.1 mN/m, respectively. These values decreased to 8.1 ± 0.9, 47.4 ± 0.5, and 46.2 ± 1.1 mN/m, respectively, in the subsequent state. In summary, the in-situ synthesis of conductive polymer within CFs directly affected their wettability properties. The presence of conductive polymers provided tunable hydrophilicity of the composites depending on the specific monomers used and the quantity of polymer present in the substrate. Various studies have documented the ability to manipulate the wetting properties through applied voltages (Xu et al. 2005 ; Liu et al. 2010 ; Darmanin and Guittard 2014 ; Tan et al. 2020 ; Pramanik and Suzuki 2020 ; Menamparambath 2024 ). The prepared conductive polymer@CF composites could be potentially used not only in sensors but also in providing controlled hydrophilicity/hydrophobicity to render additional functionalities. 3.3 Electrical conductivity comparisons of conductive polymer@CF composites Commercial application of conductive polymers presents a number of challenges because of their high cost, poor processability, and lack of repeatability. However, these materials are appealing owing to their unconventional properties, such as the ability for chemical modification, optical capabilities, and potential use in energy and sensor applications. They are considered cutting-edge materials with a variety of potential uses (Nambiar and Yeow 2011 ; Nezakati et al. 2018 ; K and Rout 2021 ; Sharma et al. 2021 ; Liu et al. 2023 ). The unique electrical conductivity of these organic polymers is due to the existence of conjugated bonds and linkages and/or heteroatoms with unshared electron pairs. During polymerization, the oxidation of monomers, either chemically or electrochemically, generates the conjugated backbone of conductive polymers. The conjugation process occurs in two distinct phases: firstly, the monomers undergo oxidation, followed by the polymerization and the oxidation of the polymers. This oxidation creates a space for the incorporation of negatively charged dopants or counter ions, such as chloride (Lota et al. 2004 ). The dopant concentration in polymers is usually below one per polymer unit, often ranging from 0.3 to 0.5. This concentration is strongly influenced by the proximity of the polymer units along the polymer chain. In supercapacitor devices, PANI and PPY are commonly utilized as conductive polymers (Suematsu et al. 2000 ). Polarons and bipolarons play a crucial role in realizing the conductivity and electrical conduction along the polymer backbone in the presence of an electric field. The widely recognized conduction process entails the movement of electric charge along the chains of conductive electroactive polymers, as well as the transfer of carriers across chains through hopping. In this study, the electrical conductivities of prepared conductive polymer@CF composites were also studied. The details and the depiction of the experimental arrangement used to test the conductivity of CF, PANI@CF, and PPY@CF composites using I-V curves were conducted in accordance with the literature (Sahiner and Demirci 2016 , 2017 ). The electrodes of the electrometer were in contact with the CFs, with conductive carbon tapes connected to both the top and bottom sides. The I-V curves were recorded via a computer. Figure 4 (a) and (b) depict the comparisons of I-V curves of bare CFs with PANI@CFs and PPY@CFs composites, respectively. The conductivities of the bare CF, PANI@CF, and PPY@CF composites were calculated using Eqs. (1) and (2) and are summarized in Fig. 4 (c) . The conductivity of bare CFs, as shown in Fig. 4 (c) , was determined to be 7.0x10 − 8 ±1.0x10 − 8 S.cm − 1 . After in situ synthesis of PANI and PPY within CF, the conductivity values were increased to 3.2x10 − 6 ±9.4x10 − 7 S.cm − 1 and 1.3x10 − 3 ±7.9x10 − 4 S.cm − 1 , respectively. The conductivity of bare CFs improved by roughly 50-fold and 20,000-fold, respectively, following the in-situ synthesis of conductive polymers PANI and PPY in 1st cycles. On the other hand, the conductivity of 2PANI@CF and 2PPY@CF were recorded as 7.6x10 − 5 ±9.3x10 − 6 S.cm − 1 and 1.7x10 − 3 ±7.0x10 − 4 S.cm − 1 , respectively. The conductivity of 2PANI@CF and 2PPY@CF composites increased by roughly 1.1 K and 24K times, respectively, compared to bare CF, while the enhancement was 24-fold and 1.3-fold for 1PANI@CF and 1PPY@CF composites, respectively. Moreover, the repeated monomer loading/polymerization cycle to CFs 3rd time to attain 3PANI@CF and 3PPY@CF increased the conductivity to 2.3x10 − 4 ±8.1x10 − 5 S.cm − 1 and 2.1x10 − 3 ±5.8x10 − 4 S.cm − 1 , respectively. The conductivity of 3PANI@CF and 3PPY@CF composites exhibited about 3.3K-fold and 30K-fold increase, respectively in comparison to bare CF. Nevertheless, it represented roughly a 1.2- and 3-fold increase compared to the 2PANI@CF and 2PPY@CF composites, respectively, indicating that the in situ synthesized PANI and PPY were approaching close to their maximum limits, as given in Table 1 . The significant improvements in the conductivity of conductive polymer@CF composites unequivocally demonstrated the successful production of conductive polymers within the CFs, and multiple monomer loading/polymerization cycles of ANI and PPY to CFs provided a higher amount of in-situ synthesized conductive polymers with higher conductivity values. The conductivity values for 3PANI@CF and 3PPY@CF composites are comparable to conductive polymer composites with similar architectures reported in different other studies (Alonso et al. 2018 ; Demirci et al. 2020 ; Kim et al. 2020 ; Parit et al. 2020 ; Huang et al. 2021 ; Fraser and van Zyl 2022 ). For instance, carboxymethyl cellulose-conductive polymer composite cryogels, CMC-PANI, and CMC-PP, exhibited conductivities of 4.6x10 − 4 and 5.0x10 − 5 S·cm − 1 , respectively (Demirci et al. 2020 ). Additionally, bacterial cellulose, methyl cellulose, hydroxypropyl methyl cellulose, and carboxymethyl cellulose PANI composite fabrics displayed conductivities of 199x10 − 2 , 2.84x10 − 2 , 2.08x10 − 2 , and 0.96x10 − 2 S.cm − 1 respectively (Kim et al. 2020 ). The cellulose nanofiber-PPY composite had a conductivity of 2x10 − 2 S.cm − 1 (Parit et al. 2020 ). Moreover, bacterial cellulose-PANI blend showed a conductivity of 1.4x10 − 1 S.cm − 1 (Alonso et al. 2018 ), while another study reported a remarkably high conductivity of 1.94x10 0 S.cm − 1 for bacterial cellulose-PPY composite (Fraser and van Zyl 2022 ). Various formulation of cellulose are reported for conductive material preparation, e.g., the coating of cellulosic paper with PANI/cellulose nanocrystal composites also afforded very high conductivity, 4x10 0 S.cm − 1 (Huang et al. 2021 ). 3.5 Biocompatibilities of conductive polymer@CF composites Hemocompatibility and biocompatibility of materials are the most essential requirements for for determining their potential use in biomedical applications. Therefore, the hemocompatibility of prepared PANI@CF and PPY@CF composites was investigated via hemolysis and BCI assays. In Fig. 5 (a) , the hemolysis% results for bare CF, PANI@CF, and PPY@CF composites are compared. According to the American Society for Testing and Materials (ASTM), hemolysis below 5% is referred to as non-toxic, up to 10% is regarded as minor, and more than 10% is considered significant (Luna-Vázquez-Gómez et al. 2021 ). Hemolysis is defined as the rupture or alteration of the red blood cell membrane, leading to the release of hemoglobin (Sowemimo-Coker 2002 ). The hemolysis% values for bare CF were found to be 0.13 ± 0.12% at 1 mg/mL concentrations, which indicated that bare CFs are nonhemolytic. However, the hemolysis ratio increased due to the in-situ synthesis of PANI, and at 1 mg/mL concentrations, the 1PANI@CF, 2PANI@CF, and 3PANI@CF composites showed significant hemolysis with values of 37.6 ± 2.8, 29.2 ± 4.2, and 19.7 ± 2.9%, respectively. Conversely, the hemolysis% values of the 1PPY@CF, 2PPY@CF, and 3PPY@CF composites were 3.0 ± 0.6%, 5.5 ± 0.7, and 2.6 ± 0.4, respectively, implying a non-hemolytic nature. As PPY was introduced into an animal's body, no carcinogenic effects, allergies, or hemolysis of red blood cells were reported (Wang et al. 2004 ). It was also reported that PPY-polyvinyl alcohol composites showed great hemocompatibility with non-hemolytic nature (Mezhuev et al. 2015 ). So, it is apparent that PPY-based composites are non-hemolytic materials. Another test that is widely used to evaluate the compatibility of materials with blood is the blood clotting index (BCI). Clotting agents play a crucial role in controlling bleeding, thus making them vital componentss of wound dressing materials. BCI is particularly important in assessing the efficacy of any clotting agents, with lower values indicating superior coagulation effects.The effect of bare CF, PANI@CF, and PPY@CF composites on the blood coagulation process is shown in Fig. 5 (b). It was observed that the bare CFs had no effect on coagulation, while PANI@CF and PPY@CF composites exerted a modest impact with 90% BCI. Depending on the specific needs, such as excessive bleeding or the need to prevent blood loss, clotting agents may be necessary to stop bleeding in certain application including surgery or accidents. These agents can also be valuable for wound dressing materials. However, it is often imperative to avoid any disruption to the blood coagulation systems when using materials in biological applications. In general, BCI is around 100% considered no interaction with the blood clothing mechanisms. It was observed that the bare CFs did not affect the blood clotting mechanism with 100.2 ± 0.7% BCI value. On the other hand, the prepared PANI@CF and PPY@CF composites exhibit slight effect on blood coagulation mechanism about 90% BCI values. Furthermore, the cytotoxicity of PANI@CF and PPY@CF composites was compared with neat CF on L929 fibroblast cells and the results are shown in Fig. 5 (c) . The cell viability% at 1 mg of CF was determined as 103 ± 2%, while the cell viability of 1PANI@CF, 2PANI@CF, and 3PANI@CF composites was determined as 61.2, 52.1, and 53.1%, respectively. The toxicity of PANI@CF composites increased due to the increased PANI content in CFs. However, the results for 1 mg PPY@CF composites showed moderate toxicity on L929 fibroblast cell (López-García et al. 2014 ). Nevertheless, the cell viability% of 1PPY@CF, 2PPY@CF, and 3PPY@CF composites against L929 fibroblast cells at the same concentration was found to be 81 ± 9, 71 ± 8, and 70 ± 8%, respectively. While 1PPY@CF composites were within the limit of non-toxicity, both 2PPY@CF and 3PPY@CF composites revealed modest toxicity toward L929 fibroblast cells. It is apparent that the types of polymers (PANI vs PPY) have some impact on the cytotoxicity of the composite materials. However, other parameters such as the addition of different oxidizing agents, e.g., whether of chemical or biological origin-, or the amounts of doping agents, or even or type of cell lines, should be taken into consideration. The cytotoxic effects of PANI-based composites on various cell lines vary depending on factors such as PANIs’s size, shape, oxidation state, and impurity level (Zare et al. 2020 ). PANI exhibits higher cytotoxicity in its emeraldine salt form compared to its emeraldine base form (Chia et al. 2022 ). However, a mouse embryonic fibroblast cell line (NIH/3T3) or embryonic stem cells (ES R1 (ESc)) did not show any cytotoxicity when the concentration of emeraldine salt was kept below 2.5 µg/mL (Humpolíček et al. 2018 ). Nevertheless, the cytotoxicity of PANI on mouse embryonic fibroblast cells can be influenced by an acid dopant. Zhang et al. demonstrated that the cytotoxicity increased in the following order: PANI-phosphoric acid < PANI-hydrochloric acid < PANI-sulfuric acid < PANI-methanesulfonic acid < PANI-nitric acid. Even at 20 ppm doses, the most common HCl-doped PANI did not appear to be cytotoxic (Zhang et al. 2019 ). A different investigation indicated that PPY nanoparticles demonstrated non-toxic behavior at a concentration of 100 µg/mL when tested on fibroblast (L929), colorectal adenocarcinoma (HT29), and pancreatic acinar (266 − 6) cells (Guo et al. 2019 ). Conversely, PPY particles synthesized via oxidative polymerization in the presence of sodium dodecyl sulfate (SDS) exhibited cytotoxic effects at concentrations exceeding 19.4 µg/mL on primary mouse embryonic fibroblasts (MEF), mouse hepatoma (MH-22A) cells, and human T lymphocyte Jurkat cells (Vaitkuviene et al. 2013 ). Therefore, it is essential to consider various parameters when utilizing conductive polymer-containing composite materials for in vivo biomedical applications. 3.6 Antimicrobial activities of conductive polymer@CF composites Two of the important applications of cellulose-based materials are in packaging (Yaradoddi et al. 2020 ; Liu et al. 2021 ; Asim et al. 2022 ) and wound dressing (Zheng et al. 2020 ; Kanikireddy et al. 2020 ; Cidreira et al. 2021 ). Given this, it is crucial for cellulose based materials to possess some level of antimicrobial properties against various microorganisms. Therefore, the antimicrobial effectiveness of the conductive polymer@CF composites was evaluated against gram-negative E. coli , gram-positive S. aureus , and a fungus, C. albicans , and the results are summarized in Table 2 . Table 2 Antimicrobial activities of CF-based conductive polymer composites against gram-negative E. coli , gram-positive S. aureus , and a fungus, C. albicans . Materials E. coli S. aureus C. albicans MIC (mg/mL) MBC (mg/mL) MIC (mg/mL) MBC (mg/mL) MIC (mg/mL) MBC (mg/mL) CF *N.D. N.D. N.D. N.D. N.D. N.D. 3PANI@CF N.D. N.D. N.D. N.D. N.D. N.D. 3PANI@CF + 10 N.D. 10 N.D. 10 N.D. 3PPY@CF 2.5 10 2.5 10 5 10 3PPY@CF + 2.5 10 2.5 10 5 10 *N.D. is not detected. As anticipated, bare CF displayed no antimicrobial effect up to a concentration of 10 mg/mL, consistent with prior studies (George and S N 2015 ; Hasanin et al. 2018 ; Abou Hammad et al. 2019 ). Similarly, no antimicrobial activity was observed for the 3PANI@CF composites at the same concentration. However, the 3PPY@CF composites exhibited some antibacterial activity against three microorganisms. Specifically, the MIC value for E. coli and S. aureus bacteria was 2.5 mg/mL, with MBC values of 10 mg/mL. Conversely, the MIC and MBC values against C. albicans were 5 mg/mL and 10 mg/mL, respectively. To assess the potential enhancement of antimicrobial activity following the protonation of amine-containing polymers, the conductive polymer@CF composites were treated with 25 mL of 1M HCl. For the 3PANI@CF + composites, the MIC value against E. coli , S. aureus bacteria, and C. albicans fungus was determined to be 10 mg/mL. In contrast, there were no changes observed in the antimicrobial effect of the 3PPY@CF composites after protonation. The MIC value remained at 2.5 mg/mL for E. coli and S. aureus bacteria, and 5 mg/mL for C. albicans , with corresponding MBC values of 10 mg/mL. Accordingly, for 3PPY@CF composites, the MIC value against E. coli and S. aureus bacteria was found to be 2.5 mg/mL, and the MBC values were found to be 10 mg/mL. On the other hand, MIC, and MBC values for 3PPY@CF composites against C. albicans were determined as 5 and 10 mg/mL, respectively. These results are comparable with some previously reported in different literature (George and S N 2015 ; Shalini et al. 2016 ; Bideau et al. 2016 ; Hasanin et al. 2018 ; Abou Hammad et al. 2019 ; Du et al. 2021 ; Maruthapandi et al. 2022 ). For instance, PANI/Cell composite displayed slight antimicrobial activity at 10 mg/mL concentrations with 27.7 ± 0.5, 32.9 ± 0.7, and 39.1 ± 0.6% inhibitions against E. coli , B.subtilis , and C. albicans , respectively (Abou Hammad et al. 2019 ). Another study reported MIC values of 2.5 mg/mL and 1.25 mg/mL for cellulose/PANI composites against E. coli and S. aureus , respectively (Shalini et al. 2016 ). Likewise, a composite composed of PPY (cellulose nanopaper/chitosan/PPY: 1 inch x1 inch) demonstrated a bacterial reduction of 95.59% against E. coli and 99.28% against S. aureus (Du et al. 2021 ). It is suggested that the antibacterial efficacy of conductive composites may increase at higher concentrations (e.g.,100 mg) (Bideau et al. 2016 ). The antimicrobial properties of conductive polymer composites can be attributed to either (a) the release of acidic dopant ions from the conducting polymers, which interact with the bacterial cell wall and/or membrane, leading to its destruction and subsequent death, or (b) the electrostatic adhesion between the bacteria and conductive polymers, facilitated by their opposite charges, which results in the rupture of the bacterial cell wall and/or membrane and ultimately causing death (George and S N 2015 ; Bideau et al. 2016 ; Abou Hammad et al. 2019 ; Maruthapandi et al. 2022 ). 4. Conclusions In this study, it was demonstrated that the synthesis of PANI and PPY within CFs, made from low-quality cotton, through a chemical oxidative polymerization process yields highly versatile conductive polymer@CF composites. The amount of conductive polymers within CF was increased by repeatedly loading ANI and PY monomers into CF structures and then conducting in-situ oxidative polymerization cycles. The resulting conductive polymer-containing composites exhibited excellent thermal stability compared to pure cellulose due to interactions between PANI and PPY chains with cellulose molecules. Multiple cycles of ANI loading/polymerization led to decreased CA values for PANI@CF composites, while multiple PY loading/polymerization cycles resulted in increased CA values for PPY@CF composites. The decrease in CA values of PANI@CF could be attributed to the conversion of PANI structures formed in the previous polymerization process into the emeraldine salt form induced by the presence of HCl. Conversely, the increase in CA of PPY@CF could be ascribed to the heightened amount of in situ synthesized PPY within CFs. The electrical conductivity of the PANI@CF and PPY@CF composites also increased with the multiple cycles of monomer loading/polymerization. The highest electrical conductivity was attained for 3PANI@CF and 3PPY@CF composites and was calculated to be 3.3K and 30K times higher than the conductivity of neat CF, respectively. Additionally, it was found that PANI@CF composites were very hemolytic at 1 mg/mL concentration, resulting in damage to red blood cells. In contrast, PPY@CF composites at the same concentration showed no hemolytic activity and did not cause damage to red blood cells. Moreover, the cytotoxicity of the conductive polymer@CF composites was evaluated on L929 fibroblast cells, demonstrating that at a concentration of 1 mg, the PPY@CF composites exhibited greater biocompatibility compared to PANI@CF composites. In addition, 3PPY@CF composites displayed notable antibacterial properties against both gram-negative and gram-positive bacteria, including E. coli and S. aureus , as well as against the fungus C. albicans . Cellulose, with special attributes of high purity, crystallinity, strong mechanical properties, and biocompatibility, has expanded its usage beyond its traditional application in the food and beverage industry. Electroactive cellulose films hold great potential as adaptable functional materials suitable for many biomedical applications. The results of this study demonstrate the use of cellulose based conductive polymer composites for a wide range of potential applications in biotechnological domains. Declarations Supporting Information Supporting Information is available from the Springer Library or from the author. Conflict of Interest The authors declare no conflict of interest. Author Contribution Sahin Demirci, Mehtap Sahiner, Shaida S. Rumi, Selin S. Suner: Methodology, validation, investigation, writing- original draft preparation.Noureddine Abidi: Conceptualization, methodology, formal analysis, investigation, Supervision Resources, Writing - review and editingNurettin Sahiner: Conceptualization, Methodology, formal analysis, investigation, Resources, Investigation, Writing - review and editing, Visualization, Supervision, Project administration, Funding acquisition. Acknowledgement The startup fund through the University of South Florida, Ophthalmology department is greatly appreciated. Data Availability Statement The data generated is contained within this manuscript and in supplementary materials. References Abou Hammad AB, Abd El-Aziz ME, Hasanin MS, Kamel S (2019) A novel electromagnetic biodegradable nanocomposite based on cellulose, polyaniline, and cobalt ferrite nanoparticles. 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ACS Omega 8:48946–48957. https://doi.org/10.1021/acsomega.3c06511 Shalini A, Nishanthi R, Palani P, Jaisankar V (2016) One pot synthesis, characterization of polyaniline and cellulose/polyaniline nanocomposites: application towards in vitro measurements of antibacterial activity. Mater Today Proc 3:1633–1642. https://doi.org/10.1016/j.matpr.2016.04.053 Sharma S, Sudhakara P, Omran AAB, et al (2021) Recent Trends and Developments in Conducting Polymer Nanocomposites for Multifunctional Applications. Polymers (Basel) 13:2898. https://doi.org/10.3390/polym13172898 Shi X, Hu Y, Fu F, et al (2014) Construction of PANI–cellulose composite fibers with good antistatic properties. J Mater Chem A 2:7669–7673. https://doi.org/10.1039/C4TA01149J Shishkanova T V., Sapurina I, Stejskal J, et al (2005) Ion-selective electrodes: Polyaniline modification and anion recognition. 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Synth Met 175:183–191. https://doi.org/10.1016/j.synthmet.2013.05.014 Tang S-J, Wang A-T, Lin S-Y, et al (2011) Polymerization of aniline under various concentrations of APS and HCl. Polym J 43:667–675. https://doi.org/10.1038/pj.2011.43 Tudoroiu E-E, Dinu-Pîrvu C-E, Albu Kaya MG, et al (2021) An Overview of Cellulose Derivatives-Based Dressings for Wound-Healing Management. Pharmaceuticals 14:1215. https://doi.org/10.3390/ph14121215 Vaitkuviene A, Kaseta V, Voronovic J, et al (2013) Evaluation of cytotoxicity of polypyrrole nanoparticles synthesized by oxidative polymerization. J Hazard Mater 250–251:167–174. https://doi.org/10.1016/j.jhazmat.2013.01.038 Wang J, Wang L, Gardner DJ, et al (2021) Towards a cellulose-based society: opportunities and challenges. Cellulose 28:4511–4543. https://doi.org/10.1007/s10570-021-03771-4 Wang X, Gu X, Yuan C, et al (2004) Evaluation of biocompatibility of polypyrrole in vitro and in vivo. J Biomed Mater Res Part A 68A:411–422. https://doi.org/10.1002/jbm.a.20065 Wang Y, Liu A, Han Y, Li T (2020) Sensors based on conductive polymers and their composites: a review. Polym Int 69:7–17. https://doi.org/10.1002/pi.5907 Wu C-G, Marcy HO, DeGroot DC, et al (1991) Oxidative polymerization of pyrrole and aniline in Hofmann-type inclusion compounds. Synth Met 41:693–698. https://doi.org/10.1016/0379-6779(91)91161-3 Xu L, Chen W, Mulchandani A, Yan Y (2005) Reversible conversion of conducting polymer films from superhydrophobic to superhydrophilic. Angew Chemie - Int Ed 44:6009–6012. https://doi.org/10.1002/anie.200500868 Yaradoddi JS, Banapurmath NR, Ganachari S V., et al (2020) Biodegradable carboxymethyl cellulose based material for sustainable packaging application. Sci Rep 10:21960. https://doi.org/10.1038/s41598-020-78912-z Zare EN, Makvandi P, Ashtari B, et al (2020) Progress in Conductive Polyaniline-Based Nanocomposites for Biomedical Applications: A Review. J Med Chem 63:1–22. https://doi.org/10.1021/acs.jmedchem.9b00803 Zhang Y, Zhou M, Dou C, et al (2019) Synthesis and biocompatibility assessment of polyaniline nanomaterials. J Bioact Compat Polym 34:16–24. https://doi.org/10.1177/0883911518809110 Zhang Z, Wei Z, Wan M (2002) Nanostructures of Polyaniline Doped with Inorganic Acids. Macromolecules 35:5937–5942. https://doi.org/10.1021/ma020199v Zheng L, Li S, Luo J, Wang X (2020) Latest Advances on Bacterial Cellulose-Based Antibacterial Materials as Wound Dressings. Front Bioeng Biotechnol 8:. https://doi.org/10.3389/fbioe.2020.593768 Additional Declarations No competing interests reported. Supplementary Files SupplementaryInformationR.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. 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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-4541295","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":319173237,"identity":"42f2430b-f7af-41c1-8bbb-b29e546c65c9","order_by":0,"name":"Sahin Demirci","email":"","orcid":"","institution":"Canakkale Onsekiz Mart University","correspondingAuthor":false,"prefix":"","firstName":"Sahin","middleName":"","lastName":"Demirci","suffix":""},{"id":319173238,"identity":"0203436a-c850-406c-b87d-54ed981d9924","order_by":1,"name":"Mehtap Sahiner","email":"","orcid":"","institution":"Canakkale Onsekiz Mart University","correspondingAuthor":false,"prefix":"","firstName":"Mehtap","middleName":"","lastName":"Sahiner","suffix":""},{"id":319173239,"identity":"24f1824f-8bb6-4667-9769-dc879ac2a59c","order_by":2,"name":"Shaida S. Rumi","email":"","orcid":"","institution":"Texas Tech University","correspondingAuthor":false,"prefix":"","firstName":"Shaida","middleName":"S.","lastName":"Rumi","suffix":""},{"id":319173240,"identity":"005f4518-2291-49e9-b334-e4cb597defe2","order_by":3,"name":"Selin S. Suner","email":"","orcid":"","institution":"Canakkale Onsekiz Mart University","correspondingAuthor":false,"prefix":"","firstName":"Selin","middleName":"S.","lastName":"Suner","suffix":""},{"id":319173241,"identity":"aff90ce6-e6fd-4fd5-bc5e-35f93f3e3ba1","order_by":4,"name":"Noureddine Abidi","email":"","orcid":"","institution":"Texas Tech University","correspondingAuthor":false,"prefix":"","firstName":"Noureddine","middleName":"","lastName":"Abidi","suffix":""},{"id":319173242,"identity":"f6236cdd-b292-490f-99cf-7c69fcc135d9","order_by":5,"name":"NURETTIN SAHINER","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA2UlEQVRIiWNgGAWjYFACHoYDQLK+jb0BSBlYEK+FsY8HRBlIEKcFBBjnSSSAaCK0yLefPXi4oOIeM5vk86sbfhRIMPC3dyfg1WJwJi/h8IwzxWxs0jllN3uADpM4c3YDfi0MOQaHedsSeIBa0m7wALUYSOTi1yLf/wao5V+CBJvkmbSbf4jRwnADZEtDggGbBPux20TZYnADaAvPsYQENp4cttsyBhI8BP0i359j/JmnJiFBvv34s5tv/tjI8bf3EnAYAvAYgElilYMA+wNSVI+CUTAKRsEIAgD9KESbm7rmZQAAAABJRU5ErkJggg==","orcid":"","institution":"Canakkale Onsekiz Mart University","correspondingAuthor":true,"prefix":"","firstName":"NURETTIN","middleName":"","lastName":"SAHINER","suffix":""}],"badges":[],"createdAt":"2024-06-06 15:08:54","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4541295/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4541295/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":59186439,"identity":"132c0ee8-c36e-45b7-972d-dfd70814d531","added_by":"auto","created_at":"2024-06-27 12:06:30","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":139133,"visible":true,"origin":"","legend":"\u003cp\u003eThe schematic depiction of in situ conductive polymers (a) PANI, and (b) PPY with in CFs as PANI@CF and PPY@CF.\u003c/p\u003e","description":"","filename":"Slide1.png","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/447c9b9956cad6c904efb618.png"},{"id":59185573,"identity":"87eec9d8-2213-43a4-ad91-17876ada63c5","added_by":"auto","created_at":"2024-06-27 11:50:30","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":71618,"visible":true,"origin":"","legend":"\u003cp\u003eThe FT-IR spectra of (a) PANI@CF, (b) PPY@CF, and TGA thermograms of (c) PANI@CF and (d) PPY@CF composites.\u003c/p\u003e","description":"","filename":"Slide2.png","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/20e9537cf77b35b1e160a66a.png"},{"id":59185571,"identity":"cef77bda-8798-404d-873b-e1ae903c7132","added_by":"auto","created_at":"2024-06-27 11:50:30","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":43470,"visible":true,"origin":"","legend":"\u003cp\u003eChanges on (a) CA, and (b) surface free energy values for PANI@CF and the changes on (c) CA, and (d) surface free energy values for PPY@CF composites after multiple monomer loading/polymerization cycles.\u003c/p\u003e","description":"","filename":"Slide3.png","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/aabb4a70eb91d0e057c7d981.png"},{"id":59185572,"identity":"057ff087-ae55-4ce9-b782-d85f0209bba5","added_by":"auto","created_at":"2024-06-27 11:50:30","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":61531,"visible":true,"origin":"","legend":"\u003cp\u003eThe ohmic region of I–V curves for (a) PANI@CF, (b) PANI@CF composites, and (c) the comparison of the conductivity values of PANI@CF and PANI@CF composites.\u003c/p\u003e","description":"","filename":"Slide4.png","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/36e2368fbb5bde48e7e2de4e.png"},{"id":59185574,"identity":"9c479327-e404-4622-a126-a778980541f0","added_by":"auto","created_at":"2024-06-27 11:50:30","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":26542,"visible":true,"origin":"","legend":"\u003cp\u003eBlood compatibility of CF-based conductive polymer composites via (a) hemolysis% assay, (b) blood coagulation assay at 1 mg/mL concentration, and (c) cytotoxicity of conductive polymer@CFcomposites on L929 fibroblast cell.\u003c/p\u003e","description":"","filename":"Slide5.png","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/48e42a6cccc7d16e4f8c1bcd.png"},{"id":59533013,"identity":"60935fd0-ede5-44a1-bf6c-96efb1a7b4c4","added_by":"auto","created_at":"2024-07-03 00:59:22","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1110663,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/05768621-0cd7-41ba-92ba-927ae52dd96d.pdf"},{"id":59185576,"identity":"602b5ca3-a944-4876-964c-08f8002eaabf","added_by":"auto","created_at":"2024-06-27 11:50:31","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":3094008,"visible":true,"origin":"","legend":"","description":"","filename":"SupplementaryInformationR.docx","url":"https://assets-eu.researchsquare.com/files/rs-4541295/v1/ceaac77e52097f6077226057.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"The use of low-quality cotton-derived cellulose films as templates for in situ conductive polymer synthesis as promising biomaterials in biomedical applications","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eFossil fuels dominate the materials currently used in various industries. The urgent concerns about climate change and plastic pollution have spurred the the development of a bioeconomy, which involves substituting petroleum-based products with materials of biological origin or bio-based materials and with biodegradable alternatives (Wang et al. \u003cspan citationid=\"CR82\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). An effective approach to address this issue is to utilize eco-friendly products. The benefits of ecologically friendly materials include non-toxicity, capacity to be sustained over time, and inherent biodegradability (Khamwongsa et al. \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). The need to establish a sustainable consumption has initiated exploration into utilizing natural cellulose as a substitute for non-renewable resources in many applications (Du et al. \u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e2017\u003c/span\u003e; Chen et al. \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Liu et al. \u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Cellulose has gained significant attention as a distinctive material due to its several inherent characteristics, including biodegradability, renewability, and widespread availability (Rodrigues et al. \u003cspan citationid=\"CR63\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Chen et al. \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Liu et al. \u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Cellulose is progressively recognized as a versatile source material for various applications, serving as a flexible biopolymer capable of producing hydrogels for absorbents, aerogels for insulation, membranes for filters, films for packaging, fibers for textiles and reinforcements, (Wang et al. \u003cspan citationid=\"CR82\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Cellulose and its derivatives are commonly utilized in food packaging (Saedi et al. \u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e2021\u003c/span\u003e), wound dressing (Tudoroiu et al. \u003cspan citationid=\"CR80\" class=\"CitationRef\"\u003e2021\u003c/span\u003e), and many other biomedical applications (Aditya et al. \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2022\u003c/span\u003e; Hasanin \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2022\u003c/span\u003e), as cellulose based materials are readily biodegradable, and their degradation products are compatible with living organisms.\u003c/p\u003e \u003cp\u003eSome intriguing and remarkable organic materials, known as conducting polymers (CPs), are thought to possess special electrical and optical qualities analogous to those of inorganic semiconductors and metals. It is possible to synthesize CPs in an easy, adaptable, and economical manner (Nezakati et al. \u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; K and Rout \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Different approaches have been devised to adapt and adjust methods to prepare CPs to enable their integration and interaction with biological environments in biomedical applications such as biosensors and diagnostic devices (Runsewe et al. \u003cspan citationid=\"CR65\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Maziz et al. \u003cspan citationid=\"CR51\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). These materials are continually sought for a number of biomedical uses, including bioengineering, regenerative medicine, and biosensors (Balint et al. \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e2014\u003c/span\u003e; Distler and Boccaccini \u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Lee et al. \u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Some examples of common conductive polymers are polyacetylene (PA), polyaniline (PANI), polypyrrole (PPY), polythiophene (PTH), poly(para-phenylene) (PPP), poly(phenylenevinylene) (PPV), and polyfuran (PF ) (Nambiar and Yeow \u003cspan citationid=\"CR56\" class=\"CitationRef\"\u003e2011\u003c/span\u003e; Nezakati et al. \u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; Guo and Facchetti \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Amongst them, the two conductive polymers most frequently employed are PANI (Zare et al. \u003cspan citationid=\"CR88\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Bednarczyk et al. \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Beygisangchin et al. \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e2021\u003c/span\u003e) and PPY(Ateh et al. \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2006\u003c/span\u003e; Kim et al. \u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e2016b\u003c/span\u003e; Samwang et al. \u003cspan citationid=\"CR69\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). Conductive polymers and their composites have a wide range of applications, including photo-catalysis (Kumar et al. \u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e2020\u003c/span\u003e), anti-corrosion coatings (Racicot et al. \u003cspan citationid=\"CR62\" class=\"CitationRef\"\u003e1995\u003c/span\u003e), biomedical tools (Zare et al. \u003cspan citationid=\"CR88\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Hasanin \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2022\u003c/span\u003e), energy storage materials (Kim et al. \u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e2016a\u003c/span\u003e), and sensing devices (Wang et al. \u003cspan citationid=\"CR84\" class=\"CitationRef\"\u003e2020\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eIn this study, cellulose films (CFs) prepared from low-quality cotton were used as templates for in-situ synthesis of PANI and PPY conductive polymers. Structural and thermal characterization of the prepared CF-based conductive polymer composites, referred to as PANI@CF and PPY@CF, were performed to ascertain the relevant functional groups. The change in wettability properties of CF-based conductive polymer composites upon multiple ANI and PY monomer loading/polymerization cycles was investigated. The effect of multiple monomer loading/polymerization cycles on the conductivity of CF-based composites was also examined. Furthermore, blood compatibility of the CF-based materials was evaluated via hemolysis% and blood clotting index% (BCI) assays. Moreover, the cytotoxicity of CF-based composites on L929 fibroblast cells was investigated. The antimicrobial activity of CF-based conductive polymer composites was also analyzed against \u003cem\u003eEscherichia coli\u003c/em\u003e ATCC8739 (\u003cem\u003eE. coli\u003c/em\u003e), \u003cem\u003eStaphylococcus aureus\u003c/em\u003e ATCC6538 (\u003cem\u003eS. aureus\u003c/em\u003e), or \u003cem\u003eCandida albicans\u003c/em\u003e ATCC10231 (\u003cem\u003eC.\u003c/em\u003e albicans), microorganisms.\u003c/p\u003e"},{"header":"2. Experimental","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Materials\u003c/h2\u003e \u003cp\u003eExtra pure DMAc (N, N-Dimethylacetamide, 99%, A0403006) and anhydrous LiCl (Lithium chloride, 99%, A0386841) were purchased from Acros Organics\u0026trade; (NJ, USA). Glycerol (202397, certified ACS) was purchased from Fisher Scientific (MA, USA). Low-quality cotton was collected from the Fiber and Biopolymer Research Institute (FBRI, Texas Tech University Lubbock, TX, USA). Ammonium persulfate (APS, 98%, Sigma-Aldrich) was employed as an oxidation agent in hydrochloric acid (HCl, 36\u0026ndash;38%, Sigma Aldrich) for the oxidative polymerization of aniline (ANI, 98%, Sigma Aldrich) for the in-situ production of conductive polymer within CFs. Also, pyrrole (PY, 98%, Aldrich) was used as received for the synthesis of poly(pyrrole) (PPY). Iron (III) chloride anhydrous (FeCl\u003csub\u003e3\u003c/sub\u003e, 99%, Acros) solution in water was employed as an initiating system. Diiodomethane (99%, Alfa Aesar) was used for SFE calculations. In the cytotoxicity analysis, L929 fibroblast cells (Mouse C3 and connective tissue) were obtained from SAP Institute, Ankara, Turkey. Trypsin (0.25%, EDTA 0.02% in PBS), Dulbecco\u0026rsquo;s Modified Eagle\u0026rsquo;s Medium (DMEM, with 4.5 g/L glucose, 3.7 g/L sodium pyruvate, L-Glutamine 0.5 g/mL), fetal bovine serum (FBS, heat-inactivated), and penicillin/streptomycin (10,000 U/mL penicillin, 10 mg/mL streptomycin) were products of Pan Biotech GmbH. Dimethyl sulfoxide (DMSO, 99.9%, Carlo Erba), trypan blue (0.5% solution, Biological Industries), and 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT agent, BioFroxx) were used as received. Gram-negative bacteria \u003cem\u003eEscherichia coli\u003c/em\u003e ((\u003cem\u003eE. coli\u003c/em\u003e, ATCC8739), Gram-positive bacteria \u003cem\u003eStaphylococcus aureus\u003c/em\u003e (\u003cem\u003eS. aureus\u003c/em\u003e, ATCC6538), and yeast \u003cem\u003eCandida albicans\u003c/em\u003e (\u003cem\u003eC. albicans\u003c/em\u003e, ATCC10231) were acquired from KWIK-STIK\u0026trade; Microbiologics (St. Cloud, Minnesota, USA) for antibacterial activity tests. Nutrient agar (NA, Difco), and potato dextrose agar (Difco) as solid growth media and nutrient broth (NB, RPI, Merck, Darmstadt, Germany) as a liquid medium were used as received.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Purification of cotton fibers\u003c/h2\u003e \u003cp\u003eRaw cotton (micronaire\u0026thinsp;=\u0026thinsp;2.4) was cleaned three times using a Microdust and Trash Monitor (MTM). Then, cotton fibers were scoured and bleached in order to obtain purified cotton cellulose. For the scouring process, cotton fibers were boiled in an alkaline scouring solution (liquor ratio 1:10) containing a non-ionic wetting agent-Triton-X 100 (1 g/L) and high concentration of NaOH (8 g/L) at 90\u0026deg;C for 1 h. After that, the solution was poured off and cotton was rinsed with fresh water. The scoured fibers were boiled in a bleaching solution (liquor ratio 1:10) containing wetting agent - Triton-X 100 (0.25 g/L), NaOH (0.35 g/L), sodium silicate (3 g/L), sodium carbonate (0.7 g/L), and sodium hypochlorite (6 g/L) at 90\u0026deg;C for 90 min. Purified cotton fibers were then boiled in fresh water at 90\u0026deg;C for 20 min and neutralized with 0.25g/L acetic acid. Finally, the purified cotton was air-dried for the next use. The air-dried cotton fibers were opened twice using the Microdust and Trash Monitor (MTM).\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Dissolution of cotton fibers and cellulose film preparation\u003c/h2\u003e \u003cp\u003eScoured and bleached cotton fibers were dissolved in DMAc/LiCl solvent system. Initially, oven-dried cotton fibers (105\u0026deg;C, 24 h) were added to a hot DMAc solution at 80\u0026deg;C (1% w:v) and stirred for 30 min. Subsequently, oven dried LiCl (8% w: v) was added to the solution, and stirring was continued for another 3 h at 80\u0026deg;C. Following that, the temperature was lowered to 50\u0026deg;C, and the dissolution was carried out overnight. Afterward, the solution was transferred to an oven (105\u0026deg;C) for 12 h. Then, the solution was taken out of the oven and allowed to reach room temperature. Cellulose solution was poured into glass molds and left inside a fume hood for 24 h. Deionized (DI) water was used to regenerate the gelated films for five days. After two days of plasticization with a 30% aqueous glycerol (w:v) solution, the regenerated cellulose films were hot-pressed for 15 min at 120\u0026deg;C.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e2.4 In situ conductive polymer synthesis within cellulose films\u003c/h2\u003e \u003cp\u003eFor the preparation of conductive polymer containing cellulose films as composites, a previous protocol from our research group was followed with some modifications (Sahiner and Demirci \u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e2016\u003c/span\u003e, \u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). For this purpose, the cellulose films (CFs) were cut into several pieces with a size of 1.5x1.5 cm, and each piece was placed into 5 mL of aniline (ANI) and pyrrole (PY), separately, and stirred at 250 rpm for 12 h to load the relevant monomers into CFs. Then, the ANI and PY loaded CFs were polymerized in situ as conductive polymer@CF composites, as given below.\u003c/p\u003e \u003cdiv id=\"Sec7\" class=\"Section3\"\u003e \u003ch2\u003e2.4.1 Preparation of PANI@CF composites\u003c/h2\u003e \u003cp\u003eThe ANI loaded CF pieces were placed into 10 mL of DI water and decanted after stirring for 1 min to remove un-adsorbed ANI molecules, and this washing procedure was repeated three times. Next, 20 mL of solutions of APS in 1 M HCl were freshly prepared by dissolving 1 g of APS in 20 mL 1M HCl solution, and the ANI loaded CF pieces were placed into these solutions separately. The in-situ polymerization reactions of ANI monomers within CF pieces were carried out for 12 h under constant stirring at 250 rpm at room temperature. Finally, the prepared 1PANI@CF composites were separated from the solution via decantation of supernatant and were washed via stirring in 10 mL of fresh DI water (x3), and ethanol (x1) each for 1 min. The washed 1PANI@CF composites were dried in an oven at 50\u003csup\u003eo\u003c/sup\u003eC, and the ANI monomer loading/polymerization step was employed two more times to prepare 2PANI@CF, and 3PANI@CF composites. The prepared 1PANI@CF, 2PANI@CF, and 3PANI@CF composites were stored in closed tubes for characterization and further use.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section3\"\u003e \u003ch2\u003e2.4.2 Preparation of PPY@CF composites\u003c/h2\u003e \u003cp\u003eFirstly, the CF pieces loaded with PY were rinsed according to the previously described method to eliminate any remaining un-loaded PY monomers from the CFs, repeating the process three times with DI water. Subsequently, each PY-loaded CF piece was submerged in freshly prepared 20 mL of 0.5 M FeCl\u003csub\u003e3\u003c/sub\u003e solution and stirred at 250 rpm for 12 h at room temperature to facilitate the in-situ polymerization of the loaded PY monomers within the CFs. The prepared 1PPY@CF composites were then separated from the supernatant and washed using the same process mentioned above. Similarly, the washed and dried 1PPY@CF composites were used to prepare 2PPY@CF and 3PPY@CF composites through repeated cycles of PY monomer loading and polymerization, as detailed above. These composites, 1PPY@CF, 2PPY@CF, and 3PPY@CF were stored in sealed containers for subsequent use.\u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003e2.5 Biomedical properties of PANI@CF and PPY@CF composites\u003c/h2\u003e \u003cp\u003eThe details of the biomedical properties of conductive polymer containing CF composites were evaluated via hemocompatibility, biocompatibility, and antimicrobial assays, and the relevant details were provided in \u003cb\u003eSupporting Information\u003c/b\u003e.\u003c/p\u003e \u003c/div\u003e"},{"header":"3. Results and discussion","content":"\u003cdiv id=\"Sec11\" class=\"Section2\"\u003e \u003ch2\u003e3.1 Structural characterization of conductive polymer@CF composites\u003c/h2\u003e \u003cp\u003ePreviously, Rumi et al. reported successful preparation of transparent and strong cellulose films (CFs) from low quality cotton fiber through dissolution, casting, regeneration, plasticization, and hot-pressing (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). They exhibited improved stretchability, homogeneity, flexibility, and deformation recovery upon glycerol plasticization. According to the findings, plasticizing films containing 30% aqueous glycerol (w:v) had the highest deformation recovery, whereas adding more glycerol resulted in even weaker and more fragile films (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Therefore, in this investigation, cellulose film (CF) plasticized with 30% glycerol was used as a matrix for the in-situ synthesis of conductive polymer. The schematic presentation of in-situ conductive polymer synthesis within CF is given in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e \u003cb\u003e(a)\u003c/b\u003e and \u003cb\u003e(b)\u003c/b\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIt was noticed that the transparent CFs (size: 1.5x1.5 cm\u003csup\u003e2\u003c/sup\u003e) changed colors upon placing into aniline (ANI) (slight yellow) and pyrrole (PY) (brownish) monomers. Upon polymerization of loaded ANI and PY monomers within CFs via oxidative polymerization technique (Wu et al. \u003cspan citationid=\"CR85\" class=\"CitationRef\"\u003e1991\u003c/span\u003e; Moon et al. \u003cspan citationid=\"CR55\" class=\"CitationRef\"\u003e2007\u003c/span\u003e; Kumar Sharma et al. \u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e2015\u003c/span\u003e), as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, a dark black coloration within CFs was observed for both composites. The in-situ polymerization of ANI within CF pieces was carried out in APS/HCl solution (Tang et al. \u003cspan citationid=\"CR79\" class=\"CitationRef\"\u003e2011\u003c/span\u003e). In contrast, in-situ polymerization of PPY within CF pieces was carried out in aqueous FeCl\u003csub\u003e3\u003c/sub\u003e solution (Beneventi et al. \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e2006\u003c/span\u003e). Several studies have reported that the radical coupling mechanism occurs in the chemical polymerization of both ANI and PY (Ballav and Biswas \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e2004\u003c/span\u003e; Ahmed \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e2004\u003c/span\u003e; Tan and Ghandi \u003cspan citationid=\"CR78\" class=\"CitationRef\"\u003e2013\u003c/span\u003e; Grzybowski et al. \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Peng et al. \u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Thus, the visual dark black appearance (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e) of the resultant composite confirmed successful synthesis of conductive polymer within CF matrixes. Furthermore, the in-situ synthesis of PANI and PPY conductive polymers was repeated up to three times in order to enhance the amount of conductive polymer within CF matrices. Therefore, to increase the amount of conductive polymer within CFs matrices, the in-situ synthesis of PANI and PPY conductive polymers within CF pieces was were carried out up to three times, repetitively. For this purpose, the prepared 1PANI@CF and 1PPY@CF pieces were placed in ANI and PY monomers to load more of the related monomers into corresponding CFs by mixing at 250 rpm for 12 h again. Next, the excess amount of monomer from the surface of ANI and PY loaded 1PANI@CF and 1PPY@CF pieces were gently removed with a paper tissue. Then, the ANI and PY loaded 1PANI@CF and 1PPY@CF pieces were placed into initiators solutions, which what is APS:HCl solution for polymerization of ANI, and aqueous FeCl\u003csub\u003e3\u003c/sub\u003e solution for polymerization of PY within 1PANI@CF and 1PPY@CF pieces, respectively. For the third loading/polymerization cycles of ANI and PY within CFs, the same procedure was applied to 2PANI@CF and 2PPY@CF pieces, as mentioned above.\u003c/p\u003e \u003cp\u003eFT-IR spectra of CFs, PANI@CFs, and PPY@CFs were collected to confirm the in-situ synthesis of the conductive polymer in the matrix. Also, the FT-IR spectra after the multiple monomersloading and then in situ conductive polymer synthesis within CFs, for PANI@CFs, and PPY@CFs were recorded and shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. The most noticeable standing out peaks in FT-IR spectra of CFs were broad -OH stretching vibrations at 3287 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, -OH bending at 1655 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and -CH\u003csub\u003e2\u003c/sub\u003e scissoring at 1459 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, C-H bending at 1314 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, asymmetric ring stretching at 1112 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, C-O stretching at 1032 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and beta linkage of cellulose at 853 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). On the other hand, the peaks at 2994 and 2881 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e assigned to -CH stretching from glycerol were also observed (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). The FT-IR spectrum of 1PANI@CF composite exhibited the distinctive peak for PANI at 1580 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e associated with benzenoic\u0026ndash;quinonic nitrogen vibration (John et al. \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2010\u003c/span\u003e; Ahmad et al. \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e2016\u003c/span\u003e) along with CF peaks (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e \u003cb\u003e(a))\u003c/b\u003e. In the FT-IR spectra of 2PANI@CF and 3PANI@CF composites, all of the peaks found for neat CFs almost disappeared, with the exception of the peaks arising from cellulose between 1100\u0026thinsp;\u0026minus;\u0026thinsp;800 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Nevertheless, the intensity of the peak at 1580 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e increased as the number of in situ PANI synthesis increased. The spectra also showed the appearance of additional vibration bands that were characteristics of PANI, including aromatic C\u0026ndash;C peaks at 1478 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, aromatic amine peaks at 1285 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and C\u0026ndash;N\u0026ndash;C peaks at 1146 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (John et al. \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2010\u003c/span\u003e; Ahmad et al. \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Sahiner and Demirci \u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). Besides, the FT-IR spectra of PPY@CFs displayed in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e \u003cb\u003e(b)\u003c/b\u003e revealed the disappearance of almost all peaks observed in the FT-IR spectra of neat CFs, such as the peaks originating from cellulose in the range of 1100\u0026thinsp;\u0026minus;\u0026thinsp;800 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, even after the first synthesis of PPY within CFs. Consequently, there were newly appeared peaks with higher intensity as the number of polymerization cycles increased. These included -C\u0026thinsp;=\u0026thinsp;C peak at 1701 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, fundamental PPY ring vibration at 1539 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, N\u0026ndash;C stretching vibrations at 1288 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and out-of-plane bending of C-H at 976 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, deriving from PPY (Sahiner and Demirci \u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). These spectroscopic changes related to respective conductive polymers confirmed their effective synthesis within the matrix and the increase of their quantity with each synthesis cycle.\u003c/p\u003e \u003cp\u003eFurthermore, the thermal degradation profiles of bare CF, PANI@CF, and PPY@CF are illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e \u003cb\u003e(c)\u003c/b\u003e, and \u003cb\u003e(d)\u003c/b\u003e, respectively. A significant weight loss was observed for CF between 150\u0026ndash;240 \u003csup\u003eo\u003c/sup\u003eC, accounting for an 80.3% reduction, attributed to glycerol decomposition (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Additionally, the observed cumulative weight loss of 92.8% between 270\u0026ndash;315 \u003csup\u003eo\u003c/sup\u003eC was related to the decomposition of cellulose (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). The weight of 1PANI@CF decreased by 12.7% between 165\u0026ndash;195 \u003csup\u003eo\u003c/sup\u003eC (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e\u003cb\u003e(c)\u003c/b\u003e), an indication of a lesser amount of glycerol content in the composite due to the presence of PANI. In addition, the weight loss in the range of 200\u0026ndash;460\u0026deg;C and 465\u0026ndash;650 \u003csup\u003eo\u003c/sup\u003eC, corresponding to 45.3% and 95.3% reduction, could be ascribed to the decomposition of cellulose and PANI, respectively. Similarly, the weight losses in the temperature range of 160\u0026ndash;230\u0026deg;C were 22.7% and 8.4% for 1PPY@CF and 3PPY@CF, respectively. In addition, the respective recorded weight losses between 200\u0026ndash;460\u0026deg;C were 42.2% and 30.9% for 1PPY@CF and 3PPY@CF. The cumulative weight loss at 700 \u003csup\u003eo\u003c/sup\u003eC exceeded 99% for 1PPY@CF and was 94.7% for 3PPY@CF, respectively. These findings indicated that PANI@CF and PPY@CF composites exhibited greater thermal stability compared to CF, as the presence of PANI and PPYs in the CFs cellulose afforded excellent thermal degradation profile due to the interactions between the guest polymers (PANI or PP) and the host, CF (Stejskal et al. \u003cspan citationid=\"CR75\" class=\"CitationRef\"\u003e2005\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAlso, the thermal degradation behavior of CFs and its\u0026rsquo; situ prepared PPY composites were compared, and the corresponding results were illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e \u003cb\u003e(d)\u003c/b\u003e. It was also noted that the in-situ preparation of PPY within CFs caused removal of glycerol from structure pertaining to decrease in weight losses at 160\u0026ndash;230 \u003csup\u003eo\u003c/sup\u003eC range with 22.7, and 8.4% weight losses for 1PPY@CF, and 3PPY@CF respectively. The weight loss in 200\u0026ndash;460\u0026deg;C range was determined as 42.2, and 30.9% for 1PPY@CF, and 3PPY@CF, respectively. The cumulative weight loss at 700 \u003csup\u003eo\u003c/sup\u003eC was \u0026gt;\u0026thinsp;99, and 94.7% for 1PPY@CF, and 3PPY@CF correspondingly. It can be presumed that after three loading/polymerization cycles of PANI and PPY within CFs, the amount of glycerol is decreased due the replacement of it with ANI and/or PY because of the increased amount of PANI and PPY within CF upon their individual polymerizations were observed. Also, it is reasonable to conclude that PANI@CF and PPY@CF composites have higher thermal stability than bare CF, as the presence of PANI and PPYs in the CFs cellulose afford new thermal degradation profiles due to their interactions between the guest (PANI or PP) and the host, CF (Stejskal et al. \u003cspan citationid=\"CR75\" class=\"CitationRef\"\u003e2005\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eThe amounts of PANI and PPY synthesized within CF pieces upon in-situ polymerizations were determined gravimetrically following each loading/polymerization cycle, and the corresponding results are summarized in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. The FT-IR analysis indicated the replacement of glycerol from the CF structure even during the initial monomer loading/polymerization procedure. To quantify the amount of PANI and PPY synthesized with or insitu in CFs, five pieces of CF (1.5x1.5 cm\u003csup\u003e2\u003c/sup\u003e) were washed in 50 mL of water for 24 h, and after drying, their weight was measured as the control. The digital camera images of washed and dried CF and conductive polymer@CF composites are shown in \u003cb\u003eFigure \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e\u003c/b\u003e. It was noticed that the CFs wrinkled, visibly hardened, and became more brittle after washing and drying.\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\u003eThe amount of in-situ synthesized conductive polymers within CFs upon multiple monomer loading/polymerization cycles.\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 \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"2\" rowspan=\"3\"\u003e \u003cp\u003eWeight of bare CF (mg) *\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\" morerows=\"2\" rowspan=\"3\"\u003e \u003cp\u003eCF-based composites\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colspan=\"3\" nameend=\"c5\" namest=\"c3\"\u003e \u003cp\u003eAmount of in situ synthesized conductive polymers within CFs\u003c/p\u003e \u003cp\u003e(mg.g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) / (mmoles)**\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colspan=\"3\" nameend=\"c5\" namest=\"c3\"\u003e \u003cp\u003eNumbers of conductive polymer loading\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e3\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003e23.2\u0026thinsp;\u0026plusmn;\u0026thinsp;1.9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003ePANI\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e176.6\u0026thinsp;\u0026plusmn;\u0026thinsp;10.2 \u003cb\u003e/\u003c/b\u003e 1.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e355.7\u0026thinsp;\u0026plusmn;\u0026thinsp;26.8 / 3.8\u0026thinsp;\u0026plusmn;\u0026thinsp;0.3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e724.8\u0026thinsp;\u0026plusmn;\u0026thinsp;99.7 / 7.8\u0026thinsp;\u0026plusmn;\u0026thinsp;1.1\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003ePPY\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e231.1\u0026thinsp;\u0026plusmn;\u0026thinsp;39.6 / 3.4\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e595.1\u0026thinsp;\u0026plusmn;\u0026thinsp;62.7 / 8.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e833.8\u0026thinsp;\u0026plusmn;\u0026thinsp;25.3 / 12.4\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4\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\u003e* The weight of CFs was measured after washing in water for 24 h.\u003c/p\u003e \u003cp\u003e** mmoles were calculated according to repeating units of related conductive polymers.\u003c/p\u003e \u003cp\u003eThe average weight of five pieces of CF was 93.2\u0026thinsp;\u0026plusmn;\u0026thinsp;8.1 mg, which decreased to 23.2\u0026thinsp;\u0026plusmn;\u0026thinsp;1.9 mg after 24 h of washing in water. This reduction indicated the removal of 75.1\u0026thinsp;\u0026plusmn;\u0026thinsp;2.0% of glycerol from the structure, a finding consistent with the TGA results presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e \u003cb\u003e(b)\u003c/b\u003e. The quantities of PANI in CF after 1, 2, and 3 cycles of monomer loading/polymerization were measured as 176.6\u0026thinsp;\u0026plusmn;\u0026thinsp;10.2, 355.7\u0026thinsp;\u0026plusmn;\u0026thinsp;26.8, and 724.8\u0026thinsp;\u0026plusmn;\u0026thinsp;99.7 mg. g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively, illustrating an increase in polymer content within the CF with each successive cycle. Likewise, the quantities of PPY in 1PPY@CF, 2PPY@CF, and 3PPY@CF were determined to be 231.1\u0026thinsp;\u0026plusmn;\u0026thinsp;39.6, 595.1\u0026thinsp;\u0026plusmn;\u0026thinsp;62.7, and 833.8\u0026thinsp;\u0026plusmn;\u0026thinsp;25.3 mg.g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. This demonstrated that the amount of in situ synthesized PANI increased from 1.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.1 to 7.8\u0026thinsp;\u0026plusmn;\u0026thinsp;1.1 mmoles (based on repeating unit of PANI) through successive monomer loading and polymerization cycles, while the amount of in situ synthesized PPYs within CFs increased from 3.4\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6 to 12.4\u0026thinsp;\u0026plusmn;\u0026thinsp;04 mmoles (based on repeating unit of PPY) .\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec12\" class=\"Section2\"\u003e \u003ch2\u003e3.2 The wettability properties of conductive polymer@CF composites\u003c/h2\u003e \u003cp\u003eThe wetting ability of CFs and conductive polymer@CF composites were assessed through contact angle (CA) measurements. A droplet of 10 \u0026micro;L of DI water was deposited on the samples. As per our previous study, the contact angle of water on plasticized CFs was \u0026lt;\u0026thinsp;15 \u003csup\u003eo\u003c/sup\u003e, while for non-plasticized CF was \u0026gt;\u0026thinsp;80 \u003csup\u003eo\u003c/sup\u003e. The decrease in CA was attributed to the inherent hydrophilicity of glycerol (Rumi et al. \u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). The CA value of 11.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4 \u003csup\u003eo\u003c/sup\u003e for CF was determined in this study after washing and drying whereas the contact angle value was measured as 90.6\u0026thinsp;\u0026plusmn;\u0026thinsp;3.7 \u003csup\u003eo\u003c/sup\u003e before washing and drying and corresponding values compared in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e \u003cb\u003e(a)\u003c/b\u003e. The CA values were determined in two different states. The first state, referred to as \u0026lsquo;as is\u0026rsquo;, involved measuring the contact angles of composites immediately after the completion of the in-situ conductive polymer synthesis process. Water from the sample surface was wiped off before taking the measurement. In the second state, the composites were in their dried forms. Bare CF (\u0026lsquo;as is\u0026rsquo;) was washed and also dried to make a comparison of CA with composites in the second state. The CA of dried CF increased to 90.6\u0026thinsp;\u0026plusmn;\u0026thinsp;3.7 \u003csup\u003eo\u003c/sup\u003e from 11.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4 \u003csup\u003eo\u003c/sup\u003e due to the loss of hydrophilic glycerol. The measured CA values (\u0026lsquo;as is\u0026rsquo; state) for 1PANI@CF, 2PANI@CF, and 3PANI@CF composites were calculated as 42.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6, 39.5\u0026thinsp;\u0026plusmn;\u0026thinsp;1.9, and 26.3\u0026thinsp;\u0026plusmn;\u0026thinsp;2.8 \u003csup\u003eo\u003c/sup\u003e, respectively, which were at least 2-fold higher than bare CF (11.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4 \u003csup\u003eo\u003c/sup\u003e). The CA of PANI@CF composites after washing and drying, increased as well to 86.5\u0026thinsp;\u0026plusmn;\u0026thinsp;1.6, 65.5\u0026thinsp;\u0026plusmn;\u0026thinsp;1.3, and 38.7\u0026thinsp;\u0026plusmn;\u0026thinsp;08 \u003csup\u003eo\u003c/sup\u003e for consecutive cycle of polymerization, although remaining lower than bare CF. The images of water droplets on CF and PANI@CF composites in both states were given in \u003cb\u003eFigure S2\u003c/b\u003e. In both instances, it was observed that wettability of the composites increased with increase of PANI content in the substrate. This phenomenon could be explained by the fact that PANI structures transform into the emeraldine salt during polymerization in the presence of HCl. PANI is relatively hydrophobic in emeraldine base form, and its water CA value is between 94\u0026thinsp;\u0026minus;\u0026thinsp;84 \u003csup\u003eo\u003c/sup\u003e (Liu et al. \u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e1994\u003c/span\u003e; Shishkanova et al. \u003cspan citationid=\"CR73\" class=\"CitationRef\"\u003e2005\u003c/span\u003e). On the other hand, the emeraldine salt form of PANI occurred in the presence of acid such as HCl, HNO\u003csub\u003e3\u003c/sub\u003e, etc. shows lower contact angles (Zhang et al. \u003cspan citationid=\"CR90\" class=\"CitationRef\"\u003e2002\u003c/span\u003e; Blinova et al. \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e2008\u003c/span\u003e). The SFE values for CF in \u0026lsquo;as is\u0026rsquo; form was 71.1\u0026thinsp;\u0026plusmn;\u0026thinsp;0.1 mN/m (CA is 11.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4 \u003csup\u003eo\u003c/sup\u003e), whereas it was 56.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.5, 59.8\u0026thinsp;\u0026plusmn;\u0026thinsp;1.3, 66.2\u0026thinsp;\u0026plusmn;\u0026thinsp;1.4 mN/m for PANI@CF 1PANI@CF, 2PANI@CF, and 3PANI@CF, respectively, as fiven in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e \u003cb\u003e(b)\u003c/b\u003e. On the other hand, the surface free energy (SFE) for washed and dried CF was 34.2\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6 mN/m, while SFE was 35.8\u0026thinsp;\u0026plusmn;\u0026thinsp;0.5, 43.1\u0026thinsp;\u0026plusmn;\u0026thinsp;1.8, 65.4\u0026thinsp;\u0026plusmn;\u0026thinsp;1.1 mN/m for dried PANI@CF 1PANI@CF, 2PANI@CF, and 3PANI@CF, respectively. The calculated SFE values are in agreement compatible with the calculated CA values for each related CF-based structure prepared in this study.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIn contrast, it was found that monomer loading/polymerization cycle had a positive impact on increasing CA of PPY@CF composites as illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e \u003cb\u003e(c)\u003c/b\u003e. The CA values for 1PPY@CF, 2PPY@CF, and 3PPY@CF composites increased to 57.6\u0026thinsp;\u0026plusmn;\u0026thinsp;1.4, 60.7\u0026thinsp;\u0026plusmn;\u0026thinsp;1.2, and 66.8\u0026thinsp;\u0026plusmn;\u0026thinsp;1.0 \u003csup\u003eo\u003c/sup\u003e in the second state from 24.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.2, 25.3\u0026thinsp;\u0026plusmn;\u0026thinsp;1.1, and 42.3\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6 \u003csup\u003eo\u003c/sup\u003e, respectively. The photographs of water droplet on PPY@CF composites are given in \u003cb\u003eFigure S3\u003c/b\u003e. The CA of composites increased with the increased amount of PPY in the matrix. Similarly, a study by Fraser and van Zyl also reported the increase of CA from 35.8\u0026deg; to 48.5 \u0026deg; with an increase of polymerization time from 50 min to 20 h for the bacterial cellulose-PPY composites (Fraser and van Zyl \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). Another study also noted that covering individual cellulose fibers with a continuous PPy coating led to decreased capillary forces, thereby enhancing the contact angle between water and the composite fibers. Additionally, the presence of PPy hindered the formation of hydrogen bonds between the individual fibers when they were in a dry state (Nystr\u0026ouml;m et al. \u003cspan citationid=\"CR58\" class=\"CitationRef\"\u003e2010\u003c/span\u003e). The SFE values for PPY@CF composites were found to decrease with the increasing value of CA after multiple PPY loading/polymerization cycles (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e \u003cb\u003e(d))\u003c/b\u003e. The \u0026lsquo;as is\u0026rsquo; SFE value for 1PPY@CF, 2PPY@CF, and 3PPY@CF composites were calculated as 68.7\u0026thinsp;\u0026plusmn;\u0026thinsp;0.7, 66.3\u0026thinsp;\u0026plusmn;\u0026thinsp;0.5, and 60.4\u0026thinsp;\u0026plusmn;\u0026thinsp;1.1 mN/m, respectively. These values decreased to 8.1\u0026thinsp;\u0026plusmn;\u0026thinsp;0.9, 47.4\u0026thinsp;\u0026plusmn;\u0026thinsp;0.5, and 46.2\u0026thinsp;\u0026plusmn;\u0026thinsp;1.1 mN/m, respectively, in the subsequent state.\u003c/p\u003e \u003cp\u003eIn summary, the in-situ synthesis of conductive polymer within CFs directly affected their wettability properties. The presence of conductive polymers provided tunable hydrophilicity of the composites depending on the specific monomers used and the quantity of polymer present in the substrate. Various studies have documented the ability to manipulate the wetting properties through applied voltages (Xu et al. \u003cspan citationid=\"CR86\" class=\"CitationRef\"\u003e2005\u003c/span\u003e; Liu et al. \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e2010\u003c/span\u003e; Darmanin and Guittard \u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e2014\u003c/span\u003e; Tan et al. \u003cspan citationid=\"CR77\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Pramanik and Suzuki \u003cspan citationid=\"CR61\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Menamparambath \u003cspan citationid=\"CR52\" class=\"CitationRef\"\u003e2024\u003c/span\u003e). The prepared conductive polymer@CF composites could be potentially used not only in sensors but also in providing controlled hydrophilicity/hydrophobicity to render additional functionalities.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec13\" class=\"Section2\"\u003e \u003ch2\u003e3.3 Electrical conductivity comparisons of conductive polymer@CF composites\u003c/h2\u003e \u003cp\u003eCommercial application of conductive polymers presents a number of challenges because of their high cost, poor processability, and lack of repeatability. However, these materials are appealing owing to their unconventional properties, such as the ability for chemical modification, optical capabilities, and potential use in energy and sensor applications. They are considered cutting-edge materials with a variety of potential uses (Nambiar and Yeow \u003cspan citationid=\"CR56\" class=\"CitationRef\"\u003e2011\u003c/span\u003e; Nezakati et al. \u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; K and Rout \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Sharma et al. \u003cspan citationid=\"CR71\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Liu et al. \u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). The unique electrical conductivity of these organic polymers is due to the existence of conjugated bonds and linkages and/or heteroatoms with unshared electron pairs. During polymerization, the oxidation of monomers, either chemically or electrochemically, generates the conjugated backbone of conductive polymers. The conjugation process occurs in two distinct phases: firstly, the monomers undergo oxidation, followed by the polymerization and the oxidation of the polymers. This oxidation creates a space for the incorporation of negatively charged dopants or counter ions, such as chloride (Lota et al. \u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e2004\u003c/span\u003e). The dopant concentration in polymers is usually below one per polymer unit, often ranging from 0.3 to 0.5. This concentration is strongly influenced by the proximity of the polymer units along the polymer chain. In supercapacitor devices, PANI and PPY are commonly utilized as conductive polymers (Suematsu et al. \u003cspan citationid=\"CR76\" class=\"CitationRef\"\u003e2000\u003c/span\u003e). Polarons and bipolarons play a crucial role in realizing the conductivity and electrical conduction along the polymer backbone in the presence of an electric field. The widely recognized conduction process entails the movement of electric charge along the chains of conductive electroactive polymers, as well as the transfer of carriers across chains through hopping. In this study, the electrical conductivities of prepared conductive polymer@CF composites were also studied. The details and the depiction of the experimental arrangement used to test the conductivity of CF, PANI@CF, and PPY@CF composites using I-V curves were conducted in accordance with the literature (Sahiner and Demirci \u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e2016\u003c/span\u003e, \u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). The electrodes of the electrometer were in contact with the CFs, with conductive carbon tapes connected to both the top and bottom sides. The I-V curves were recorded via a computer. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e \u003cb\u003e(a)\u003c/b\u003e and \u003cb\u003e(b)\u003c/b\u003e depict the comparisons of I-V curves of bare CFs with PANI@CFs and PPY@CFs composites, respectively. The conductivities of the bare CF, PANI@CF, and PPY@CF composites were calculated using Eqs.\u0026nbsp;(1) and (2) and are summarized in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e \u003cb\u003e(c)\u003c/b\u003e. The conductivity of bare CFs, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e \u003cb\u003e(c)\u003c/b\u003e, was determined to be 7.0x10\u003csup\u003e\u0026minus;\u0026thinsp;8\u003c/sup\u003e\u0026plusmn;1.0x10\u003csup\u003e\u0026minus;\u0026thinsp;8\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. After in situ synthesis of PANI and PPY within CF, the conductivity values were increased to 3.2x10\u003csup\u003e\u0026minus;\u0026thinsp;6\u003c/sup\u003e\u0026plusmn;9.4x10\u003csup\u003e\u0026minus;\u0026thinsp;7\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 1.3x10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e\u0026plusmn;7.9x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe conductivity of bare CFs improved by roughly 50-fold and 20,000-fold, respectively, following the in-situ synthesis of conductive polymers PANI and PPY in 1st cycles. On the other hand, the conductivity of 2PANI@CF and 2PPY@CF were recorded as 7.6x10\u003csup\u003e\u0026minus;\u0026thinsp;5\u003c/sup\u003e\u0026plusmn;9.3x10\u003csup\u003e\u0026minus;\u0026thinsp;6\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 1.7x10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e\u0026plusmn;7.0x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. The conductivity of 2PANI@CF and 2PPY@CF composites increased by roughly 1.1 K and 24K times, respectively, compared to bare CF, while the enhancement was 24-fold and 1.3-fold for 1PANI@CF and 1PPY@CF composites, respectively. Moreover, the repeated monomer loading/polymerization cycle to CFs 3rd time to attain 3PANI@CF and 3PPY@CF increased the conductivity to 2.3x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e\u0026plusmn;8.1x10\u003csup\u003e\u0026minus;\u0026thinsp;5\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 2.1x10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e\u0026plusmn;5.8x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. The conductivity of 3PANI@CF and 3PPY@CF composites exhibited about 3.3K-fold and 30K-fold increase, respectively in comparison to bare CF. Nevertheless, it represented roughly a 1.2- and 3-fold increase compared to the 2PANI@CF and 2PPY@CF composites, respectively, indicating that the in situ synthesized PANI and PPY were approaching close to their maximum limits, as given in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. The significant improvements in the conductivity of conductive polymer@CF composites unequivocally demonstrated the successful production of conductive polymers within the CFs, and multiple monomer loading/polymerization cycles of ANI and PPY to CFs provided a higher amount of in-situ synthesized conductive polymers with higher conductivity values. The conductivity values for 3PANI@CF and 3PPY@CF composites are comparable to conductive polymer composites with similar architectures reported in different other studies (Alonso et al. \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; Demirci et al. \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Kim et al. \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Parit et al. \u003cspan citationid=\"CR59\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Huang et al. \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Fraser and van Zyl \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). For instance, carboxymethyl cellulose-conductive polymer composite cryogels, CMC-PANI, and CMC-PP, exhibited conductivities of 4.6x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e and 5.0x10\u003csup\u003e\u0026minus;\u0026thinsp;5\u003c/sup\u003e S\u0026middot;cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively (Demirci et al. \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Additionally, bacterial cellulose, methyl cellulose, hydroxypropyl methyl cellulose, and carboxymethyl cellulose PANI composite fabrics displayed conductivities of 199x10\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e, 2.84x10\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e, 2.08x10\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e, and 0.96x10\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e respectively (Kim et al. \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). The cellulose nanofiber-PPY composite had a conductivity of 2x10\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (Parit et al. \u003cspan citationid=\"CR59\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Moreover, bacterial cellulose-PANI blend showed a conductivity of 1.4x10\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (Alonso et al. \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e2018\u003c/span\u003e), while another study reported a remarkably high conductivity of 1.94x10\u003csup\u003e0\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e for bacterial cellulose-PPY composite (Fraser and van Zyl \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). Various formulation of cellulose are reported for conductive material preparation, e.g., the coating of cellulosic paper with PANI/cellulose nanocrystal composites also afforded very high conductivity, 4x10\u003csup\u003e0\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (Huang et al. \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e2021\u003c/span\u003e).\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec14\" class=\"Section2\"\u003e \u003ch2\u003e3.5 Biocompatibilities of conductive polymer@CF composites\u003c/h2\u003e \u003cp\u003eHemocompatibility and biocompatibility of materials are the most essential requirements for for determining their potential use in biomedical applications. Therefore, the hemocompatibility of prepared PANI@CF and PPY@CF composites was investigated via hemolysis and BCI assays. In Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e \u003cb\u003e(a)\u003c/b\u003e, the hemolysis% results for bare CF, PANI@CF, and PPY@CF composites are compared. According to the American Society for Testing and Materials (ASTM), hemolysis below 5% is referred to as non-toxic, up to 10% is regarded as minor, and more than 10% is considered significant (Luna-V\u0026aacute;zquez-G\u0026oacute;mez et al. \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Hemolysis is defined as the rupture or alteration of the red blood cell membrane, leading to the release of hemoglobin (Sowemimo-Coker \u003cspan citationid=\"CR74\" class=\"CitationRef\"\u003e2002\u003c/span\u003e). The hemolysis% values for bare CF were found to be 0.13\u0026thinsp;\u0026plusmn;\u0026thinsp;0.12% at 1 mg/mL concentrations, which indicated that bare CFs are nonhemolytic. However, the hemolysis ratio increased due to the in-situ synthesis of PANI, and at 1 mg/mL concentrations, the 1PANI@CF, 2PANI@CF, and 3PANI@CF composites showed significant hemolysis with values of 37.6\u0026thinsp;\u0026plusmn;\u0026thinsp;2.8, 29.2\u0026thinsp;\u0026plusmn;\u0026thinsp;4.2, and 19.7\u0026thinsp;\u0026plusmn;\u0026thinsp;2.9%, respectively. Conversely, the hemolysis% values of the 1PPY@CF, 2PPY@CF, and 3PPY@CF composites were 3.0\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6%, 5.5\u0026thinsp;\u0026plusmn;\u0026thinsp;0.7, and 2.6\u0026thinsp;\u0026plusmn;\u0026thinsp;0.4, respectively, implying a non-hemolytic nature. As PPY was introduced into an animal's body, no carcinogenic effects, allergies, or hemolysis of red blood cells were reported (Wang et al. \u003cspan citationid=\"CR83\" class=\"CitationRef\"\u003e2004\u003c/span\u003e). It was also reported that PPY-polyvinyl alcohol composites showed great hemocompatibility with non-hemolytic nature (Mezhuev et al. \u003cspan citationid=\"CR53\" class=\"CitationRef\"\u003e2015\u003c/span\u003e). So, it is apparent that PPY-based composites are non-hemolytic materials. Another test that is widely used to evaluate the compatibility of materials with blood is the blood clotting index (BCI). Clotting agents play a crucial role in controlling bleeding, thus making them vital componentss of wound dressing materials. BCI is particularly important in assessing the efficacy of any clotting agents, with lower values indicating superior coagulation effects.The effect of bare CF, PANI@CF, and PPY@CF composites on the blood coagulation process is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e \u003cb\u003e(b).\u003c/b\u003e It was observed that the bare CFs had no effect on coagulation, while PANI@CF and PPY@CF composites exerted a modest impact with 90% BCI. Depending on the specific needs, such as excessive bleeding or the need to prevent blood loss, clotting agents may be necessary to stop bleeding in certain application including surgery or accidents. These agents can also be valuable for wound dressing materials. However, it is often imperative to avoid any disruption to the blood coagulation systems when using materials in biological applications. In general, BCI is around 100% considered no interaction with the blood clothing mechanisms. It was observed that the bare CFs did not affect the blood clotting mechanism with 100.2\u0026thinsp;\u0026plusmn;\u0026thinsp;0.7% BCI value. On the other hand, the prepared PANI@CF and PPY@CF composites exhibit slight effect on blood coagulation mechanism about 90% BCI values.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFurthermore, the cytotoxicity of PANI@CF and PPY@CF composites was compared with neat CF on L929 fibroblast cells and the results are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e \u003cb\u003e(c)\u003c/b\u003e. The cell viability% at 1 mg of CF was determined as 103\u0026thinsp;\u0026plusmn;\u0026thinsp;2%, while the cell viability of 1PANI@CF, 2PANI@CF, and 3PANI@CF composites was determined as 61.2, 52.1, and 53.1%, respectively. The toxicity of PANI@CF composites increased due to the increased PANI content in CFs. However, the results for 1 mg PPY@CF composites showed moderate toxicity on L929 fibroblast cell (L\u0026oacute;pez-Garc\u0026iacute;a et al. \u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). Nevertheless, the cell viability% of 1PPY@CF, 2PPY@CF, and 3PPY@CF composites against L929 fibroblast cells at the same concentration was found to be 81\u0026thinsp;\u0026plusmn;\u0026thinsp;9, 71\u0026thinsp;\u0026plusmn;\u0026thinsp;8, and 70\u0026thinsp;\u0026plusmn;\u0026thinsp;8%, respectively. While 1PPY@CF composites were within the limit of non-toxicity, both 2PPY@CF and 3PPY@CF composites revealed modest toxicity toward L929 fibroblast cells. It is apparent that the types of polymers (PANI vs PPY) have some impact on the cytotoxicity of the composite materials. However, other parameters such as the addition of different oxidizing agents, e.g., whether of chemical or biological origin-, or the amounts of doping agents, or even or type of cell lines, should be taken into consideration. The cytotoxic effects of PANI-based composites on various cell lines vary depending on factors such as PANIs\u0026rsquo;s size, shape, oxidation state, and impurity level (Zare et al. \u003cspan citationid=\"CR88\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). PANI exhibits higher cytotoxicity in its emeraldine salt form compared to its emeraldine base form (Chia et al. \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). However, a mouse embryonic fibroblast cell line (NIH/3T3) or embryonic stem cells (ES R1 (ESc)) did not show any cytotoxicity when the concentration of emeraldine salt was kept below 2.5 \u0026micro;g/mL (Humpol\u0026iacute;ček et al. \u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e2018\u003c/span\u003e). Nevertheless, the cytotoxicity of PANI on mouse embryonic fibroblast cells can be influenced by an acid dopant. Zhang et al. demonstrated that the cytotoxicity increased in the following order: PANI-phosphoric acid\u0026thinsp;\u0026lt;\u0026thinsp;PANI-hydrochloric acid\u0026thinsp;\u0026lt;\u0026thinsp;PANI-sulfuric acid\u0026thinsp;\u0026lt;\u0026thinsp;PANI-methanesulfonic acid\u0026thinsp;\u0026lt;\u0026thinsp;PANI-nitric acid. Even at 20 ppm doses, the most common HCl-doped PANI did not appear to be cytotoxic (Zhang et al. \u003cspan citationid=\"CR89\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). A different investigation indicated that PPY nanoparticles demonstrated non-toxic behavior at a concentration of 100 \u0026micro;g/mL when tested on fibroblast (L929), colorectal adenocarcinoma (HT29), and pancreatic acinar (266\u0026thinsp;\u0026minus;\u0026thinsp;6) cells (Guo et al. \u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). Conversely, PPY particles synthesized via oxidative polymerization in the presence of sodium dodecyl sulfate (SDS) exhibited cytotoxic effects at concentrations exceeding 19.4 \u0026micro;g/mL on primary mouse embryonic fibroblasts (MEF), mouse hepatoma (MH-22A) cells, and human T lymphocyte Jurkat cells (Vaitkuviene et al. \u003cspan citationid=\"CR81\" class=\"CitationRef\"\u003e2013\u003c/span\u003e). Therefore, it is essential to consider various parameters when utilizing conductive polymer-containing composite materials for in vivo biomedical applications.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec15\" class=\"Section2\"\u003e \u003ch2\u003e3.6 Antimicrobial activities of conductive polymer@CF composites\u003c/h2\u003e \u003cp\u003eTwo of the important applications of cellulose-based materials are in packaging (Yaradoddi et al. \u003cspan citationid=\"CR87\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Liu et al. \u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Asim et al. \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e2022\u003c/span\u003e) and wound dressing (Zheng et al. \u003cspan citationid=\"CR91\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Kanikireddy et al. \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Cidreira et al. \u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). Given this, it is crucial for cellulose based materials to possess some level of antimicrobial properties against various microorganisms. Therefore, the antimicrobial effectiveness of the conductive polymer@CF composites was evaluated against gram-negative \u003cem\u003eE. coli\u003c/em\u003e, gram-positive \u003cem\u003eS. aureus\u003c/em\u003e, and a fungus, \u003cem\u003eC. albicans\u003c/em\u003e, and the results are summarized in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\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\u003eAntimicrobial activities of CF-based conductive polymer composites against gram-negative \u003cem\u003eE. coli\u003c/em\u003e, gram-positive \u003cem\u003eS. aureus\u003c/em\u003e, and a fungus, \u003cem\u003eC. albicans\u003c/em\u003e.\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"7\"\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 \u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eMaterials\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colspan=\"2\" nameend=\"c3\" namest=\"c2\"\u003e \u003cp\u003e\u003cem\u003eE. coli\u003c/em\u003e\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colspan=\"2\" nameend=\"c5\" namest=\"c4\"\u003e \u003cp\u003e\u003cem\u003eS. aureus\u003c/em\u003e\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colspan=\"2\" nameend=\"c7\" namest=\"c6\"\u003e \u003cp\u003e\u003cem\u003eC. albicans\u003c/em\u003e\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eMIC (mg/mL)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eMBC (mg/mL)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eMIC (mg/mL)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eMBC (mg/mL)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c6\"\u003e \u003cp\u003eMIC (mg/mL)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c7\"\u003e \u003cp\u003eMBC (mg/mL)\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\u003eCF\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e*N.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003e3PANI@CF\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003e3PANI@CF\u003c/b\u003e\u003csup\u003e\u003cb\u003e+\u003c/b\u003e\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003eN.D.\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003e3PPY@CF\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003e3PPY@CF\u003c/b\u003e\u003csup\u003e\u003cb\u003e+\u003c/b\u003e\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e10\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\u003e*N.D. is not detected.\u003c/p\u003e \u003cp\u003eAs anticipated, bare CF displayed no antimicrobial effect up to a concentration of 10 mg/mL, consistent with prior studies (George and S N \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2015\u003c/span\u003e; Hasanin et al. \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; Abou Hammad et al. \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). Similarly, no antimicrobial activity was observed for the 3PANI@CF composites at the same concentration. However, the 3PPY@CF composites exhibited some antibacterial activity against three microorganisms. Specifically, the MIC value for \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e bacteria was 2.5 mg/mL, with MBC values of 10 mg/mL. Conversely, the MIC and MBC values against \u003cem\u003eC. albicans\u003c/em\u003e were 5 mg/mL and 10 mg/mL, respectively. To assess the potential enhancement of antimicrobial activity following the protonation of amine-containing polymers, the conductive polymer@CF composites were treated with 25 mL of 1M HCl. For the 3PANI@CF\u003csup\u003e+\u003c/sup\u003e composites, the MIC value against \u003cem\u003eE. coli\u003c/em\u003e, \u003cem\u003eS. aureus\u003c/em\u003e bacteria, and \u003cem\u003eC. albicans\u003c/em\u003e fungus was determined to be 10 mg/mL. In contrast, there were no changes observed in the antimicrobial effect of the 3PPY@CF composites after protonation. The MIC value remained at 2.5 mg/mL for \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e bacteria, and 5 mg/mL for \u003cem\u003eC. albicans\u003c/em\u003e, with corresponding MBC values of 10 mg/mL. Accordingly, for 3PPY@CF composites, the MIC value against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e bacteria was found to be 2.5 mg/mL, and the MBC values were found to be 10 mg/mL. On the other hand, MIC, and MBC values for 3PPY@CF composites against \u003cem\u003eC. albicans\u003c/em\u003e were determined as 5 and 10 mg/mL, respectively. These results are comparable with some previously reported in different literature (George and S N \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2015\u003c/span\u003e; Shalini et al. \u003cspan citationid=\"CR70\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Bideau et al. \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Hasanin et al. \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; Abou Hammad et al. \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Du et al. \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Maruthapandi et al. \u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). For instance, PANI/Cell composite displayed slight antimicrobial activity at 10 mg/mL concentrations with 27.7\u0026thinsp;\u0026plusmn;\u0026thinsp;0.5, 32.9\u0026thinsp;\u0026plusmn;\u0026thinsp;0.7, and 39.1\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6% inhibitions against \u003cem\u003eE. coli\u003c/em\u003e, \u003cem\u003eB.subtilis\u003c/em\u003e, and \u003cem\u003eC. albicans\u003c/em\u003e, respectively (Abou Hammad et al. \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). Another study reported MIC values of 2.5 mg/mL and 1.25 mg/mL for cellulose/PANI composites against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e, respectively (Shalini et al. \u003cspan citationid=\"CR70\" class=\"CitationRef\"\u003e2016\u003c/span\u003e). Likewise, a composite composed of PPY (cellulose nanopaper/chitosan/PPY: 1 inch x1 inch) demonstrated a bacterial reduction of 95.59% against \u003cem\u003eE. coli\u003c/em\u003e and 99.28% against \u003cem\u003eS. aureus\u003c/em\u003e (Du et al. \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). It is suggested that the antibacterial efficacy of conductive composites may increase at higher concentrations (e.g.,100 mg) (Bideau et al. \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2016\u003c/span\u003e). The antimicrobial properties of conductive polymer composites can be attributed to either (a) the release of acidic dopant ions from the conducting polymers, which interact with the bacterial cell wall and/or membrane, leading to its destruction and subsequent death, or (b) the electrostatic adhesion between the bacteria and conductive polymers, facilitated by their opposite charges, which results in the rupture of the bacterial cell wall and/or membrane and ultimately causing death (George and S N \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2015\u003c/span\u003e; Bideau et al. \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Abou Hammad et al. \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Maruthapandi et al. \u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e2022\u003c/span\u003e).\u003c/p\u003e \u003c/div\u003e"},{"header":"4. Conclusions","content":"\u003cp\u003eIn this study, it was demonstrated that the synthesis of PANI and PPY within CFs, made from low-quality cotton, through a chemical oxidative polymerization process yields highly versatile conductive polymer@CF composites. The amount of conductive polymers within CF was increased by repeatedly loading ANI and PY monomers into CF structures and then conducting in-situ oxidative polymerization cycles. The resulting conductive polymer-containing composites exhibited excellent thermal stability compared to pure cellulose due to interactions between PANI and PPY chains with cellulose molecules. Multiple cycles of ANI loading/polymerization led to decreased CA values for PANI@CF composites, while multiple PY loading/polymerization cycles resulted in increased CA values for PPY@CF composites. The decrease in CA values of PANI@CF could be attributed to the conversion of PANI structures formed in the previous polymerization process into the emeraldine salt form induced by the presence of HCl. Conversely, the increase in CA of PPY@CF could be ascribed to the heightened amount of in situ synthesized PPY within CFs. The electrical conductivity of the PANI@CF and PPY@CF composites also increased with the multiple cycles of monomer loading/polymerization. The highest electrical conductivity was attained for 3PANI@CF and 3PPY@CF composites and was calculated to be 3.3K and 30K times higher than the conductivity of neat CF, respectively. Additionally, it was found that PANI@CF composites were very hemolytic at 1 mg/mL concentration, resulting in damage to red blood cells. In contrast, PPY@CF composites at the same concentration showed no hemolytic activity and did not cause damage to red blood cells. Moreover, the cytotoxicity of the conductive polymer@CF composites was evaluated on L929 fibroblast cells, demonstrating that at a concentration of 1 mg, the PPY@CF composites exhibited greater biocompatibility compared to PANI@CF composites. In addition, 3PPY@CF composites displayed notable antibacterial properties against both gram-negative and gram-positive bacteria, including \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e, as well as against the fungus \u003cem\u003eC. albicans\u003c/em\u003e.\u003c/p\u003e \u003cp\u003eCellulose, with special attributes of high purity, crystallinity, strong mechanical properties, and biocompatibility, has expanded its usage beyond its traditional application in the food and beverage industry. Electroactive cellulose films hold great potential as adaptable functional materials suitable for many biomedical applications. The results of this study demonstrate the use of cellulose based conductive polymer composites for a wide range of potential applications in biotechnological domains.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e \u003ch2\u003eSupporting Information\u003c/h2\u003e \u003cp\u003eSupporting Information is available from the Springer Library or from the author.\u003c/p\u003e \u003c/p\u003e\u003cp\u003e \u003ch2\u003eConflict of Interest\u003c/h2\u003e \u003cp\u003eThe authors declare no conflict of interest.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eSahin Demirci, Mehtap Sahiner, Shaida S. Rumi, Selin S. Suner: Methodology, validation, investigation, writing- original draft preparation.Noureddine Abidi: Conceptualization, methodology, formal analysis, investigation, Supervision Resources, Writing - review and editingNurettin Sahiner: Conceptualization, Methodology, formal analysis, investigation, Resources, Investigation, Writing - review and editing, Visualization, Supervision, Project administration, Funding acquisition.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThe startup fund through the University of South Florida, Ophthalmology department is greatly appreciated.\u003c/p\u003e\u003ch2\u003eData Availability Statement\u003c/h2\u003e \u003cp\u003eThe data generated is contained within this manuscript and in supplementary materials.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eAbou Hammad AB, Abd El-Aziz ME, Hasanin MS, Kamel S (2019) A novel electromagnetic biodegradable nanocomposite based on cellulose, polyaniline, and cobalt ferrite nanoparticles. 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Front Bioeng Biotechnol 8:. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.3389/fbioe.2020.593768\u003c/span\u003e\u003cspan address=\"10.3389/fbioe.2020.593768\" 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":"cotton derived cellulose films, cellulose-conductive polymer composite, conductive cellulose, antimicrobial cellulose composite","lastPublishedDoi":"10.21203/rs.3.rs-4541295/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4541295/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eDue to the growing interest in biopolymer-based composites in many applications, noticeable devotion has been directed to natural polymer-derived products not only because of their renewable and eco-friendly characteristics but also for their versatility in processing conditions and cost-effectiveness in fabricating the final products. Here, we report the use of cellulose films (CFs) produced from low-quality cotton as a template for in situ synthesis of well-known conductive polymers, e.g., polyaniline (PANI) and polypyrrole (PPY) via oxidative polymerization. Three successive monomer loading/polymerization cycles of aniline (ANI) and pyrrole (PY) within CFs as PANI@CF or PPY@CF were carried out to increase the extent of conductive polymer content. The contact angle (CA) for three times ANI and PPY loaded and polymerized CFs as 3PANI@CF and 3PPY@CF were determined as 26.3\u0026thinsp;\u0026plusmn;\u0026thinsp;2.8\u003csup\u003eo\u003c/sup\u003e and 42.3\u0026thinsp;\u0026plusmn;\u0026thinsp;0.6\u003csup\u003eo\u003c/sup\u003e, respectively. As the electrical conductivity is increased with increased number of conductive polymer synthesis within CF, the higher conductivity values, 3x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e\u0026plusmn;8.1x10\u003csup\u003e\u0026minus;\u0026thinsp;5\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 2.1x10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e\u0026plusmn;5.8x10\u003csup\u003e\u0026minus;\u0026thinsp;4\u003c/sup\u003e S.cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively were measured for 3PANI@CF and 3PPY@CF composites that were approximately 3.3K-fold and 30K-fold higher, respectively, compared to bare CF. It was also found that PANI@CF composites are hemolytic, whereas PPY@CF composites are not at 1 mg/mL concentrations. In the presence of 1 mg of CF-based conductive polymer composites, all PPY@CF composites exhibit better biocompatibility than PANI@CF composites on L929 fibroblast cells with 81\u0026thinsp;\u0026plusmn;\u0026thinsp;9, 71\u0026thinsp;\u0026plusmn;\u0026thinsp;8, and 70\u0026thinsp;\u0026plusmn;\u0026thinsp;8% cell viability for 1PPY@CF, 2PPY@CF, and 3PPY@CF composites, respectively. Moreover, the minimum inhibition concentration (MIC) and minimum bactericidal concentration (MBC) of 3PPY@CF composites for \u003cem\u003eEscherichia coli\u003c/em\u003e ATCC8739, \u003cem\u003eStaphylococcus aureus\u003c/em\u003e ATCC6538 are determined as 2.5 and 5 mg/mL, whereas these values were estimated to 5 and 10 mg/mL for \u003cem\u003eCandida albicans\u003c/em\u003e ATCC10231.\u003c/p\u003e","manuscriptTitle":"The use of low-quality cotton-derived cellulose films as templates for in situ conductive polymer synthesis as promising biomaterials in biomedical applications","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-06-27 11:50:26","doi":"10.21203/rs.3.rs-4541295/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":"cf815977-7fbd-410e-a903-fba824c98adb","owner":[],"postedDate":"June 27th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2024-07-03T00:51:15+00:00","versionOfRecord":[],"versionCreatedAt":"2024-06-27 11:50:26","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-4541295","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4541295","identity":"rs-4541295","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}