ISSN 2308-4057 (Печать),
ISSN 2310-9599 (Онлайн)

Developing composite films from carboxymethyl starch, polyvinyl alcohol, and kaolin for sustainable packaging applications

Аннотация
Health and environmental problems are rising by the day due to an increasing use of synthetic plastics. However, biobased packaging from starch, with its numerous advantages, or its derivatives offers a promising solution to this problem. In this study, we aimed to explore a sustainable approach to developing a bioplastic film from carboxymethyl starch, polyvinyl alcohol, and kaolin to serve as a substitute for synthetic packaging. The study objects included carboxymethyl starch, polyvinyl alcohol, glycerol, and kaolin. All the materials were heated in water to form viscous solutions. The solution was then cast into films using a mold and the water was evaporated through oven-drying. The cast films were characterized via scanning electron microscopy, X-ray diffraction, and thermogravimetric analysis. They were analyzed for their tensile mechanical, barrier, sorption, and biodegradability properties. We also investigated the effects of polyvinyl alcohol and kaolin on the morphology and functional properties of the films. The micro-surface morphology of the carboxymethyl starch/polyvinyl alcohol blend revealed a smooth and homogenous structure, while the film reinforced with kaolin had a more compact structure with zones of particle aggregations. The highest thermal stability was observed in the composite films containing carboxymethyl starch, polyvinyl alcohol, and kaolin. Higher contents of polyvinyl alcohol and kaolin significantly improved the films’ thermal, tensile mechanical, barrier, and sorption properties. The films also demonstrated a substantial rate of biodegradability. The best properties were observed in the films containing 40% of carboxymethyl starch, 60% of polyvinyl alcohol, and 4.5 per hundred resin (phr) of kaolin. The composite films made from carboxymethyl starch, polyvinyl alcohol, and kaolin had good biodegradability, renewability, and improved functional material properties. Therefore, they can be considered a sustainable alternative to the traditional synthetic plastics in packaging applications.
Ключевые слова
Biobased packaging, bioplastics, sustainable, mechanical tensile, barrier properties, biodegradability, composites
СПИСОК ЛИТЕРАТУРЫ
  1. Buryndin VG, Artyemov АV, Savinovskih АV, et al. Biostability of binder-free wood and plant plastics protected with antiseptics. Foods and Raw Materials. 2022;10(1):148–154. https://doi.org/10.21603/2308-4057-2022-1-148-154
  2. Eremeeva NB. Nanoparticles of metals and their compounds in films and coatings: A review. Foods and Raw Materials. 2024;12(1):60–79. https://doi.org/10.21603/2308-4057-2024-1-588
  3. Agarwal S. Major factors affecting the characteristics of starch-based biopolymer films. European Polymer Journal. 2021;160:11078. https://doi.org/10.1016/j.eurpolymj.2021.110788
  4. Tabassum N, Rafique U, Qayyum M, Mohammed AAA, Asif S, et al. Kaolin–polyvinyl alcohol–potato starch composite films for environmentally friendly packaging: Optimization and characterization. Journal of Composite Science. 2024;8(1):29. https://doi.org/10.3390/jcs8010029
  5. Shanmathy M, Mohanta M, Thirugnanam A. Development of biodegradable bioplastic films from Taro starch reinforced with bentonite. Carbohydrate Polymer Technologies and Applications. 2021;2:100173. https://doi.org/10.1016/j.carpta.2021.100173
  6. Gómez-Aldapa CA, Velazquez G, Gutierrez MC, Rangel-Vargas E, Castro-Rosas J, et al. Effect of polyvinyl alcohol on the physicochemical properties of biodegradable starch films. Materials Chemistry and Physics. 2020;239:122–127. https://doi.org/10.1016/j.matchemphys.2019.122027
  7. de Azevedo LC, Rovani S, Santos JJ, Dias DB, Nascimento SS, et al. Biodegradable films derived from corn and potato starch and study effect of silicate extracted from sugarcane waste ash. ACS Applied Polymer Materials. 2020;2(6):2160–2169. https://doi.org/10.1021/acsapm.0c00124
  8. Compart J, Singh A, Fettke J, Apriyanto A. Customizing starch properties: A review of starch modifications and their applications. Polymers. 2023;15(16):3491. https://doi.org/10.3390/polym15163491
  9. Omoike BA, Okieimen FE, Imoisi C, Abubakar MA. Characterization and evaluation of properties of cassava starch/poly(vinyl alcohol) films for food and pharmaceutical packaging applications. Singapore Journal of Scientific Research. 2024;14(1):34–42. https://doi.org/10.3923/sjsr.2024.34.42
  10. Prasad J, Dixit A, Sharma SP, Mwakosya AW, Petkoska AT, et al. Nanoemulsion-based active packaging for food products. Foods and Raw Materials. 2024;12(1):22–36. https://doi.org/10.21603/2308-4057-2024-1-585
  11. Spychaj T, Wilpiszewska K, Zdanowicz M. Medium and high substituted carboxymethyl starch: Synthesis, characterization and application. Starch – Stärke. 2013;65:22–33. https://doi.org/10.1002/star.201200159
  12. Omoike BA, Okieimen FE, Imoisi C. Development of lemongrass oil-based starch/PVA/kaolin films: Antimicrobial properties and biodegradability. Science International. 2025;13(1):1–12. https://doi.org/10.17311/sciintl.2025.01.12
  13. Bangar SP, Whiteside WS, Ashogbon AO, Kumar M. Recent advances in thermoplastic starches for food packaging: A review. Food Packaging and Shelf Life. 2021;30:100743. https://doi.org/10.1016/j.fpsl.2021.100743
  14. Lee S, Kim ST, Pant BR, Song HH, Lee SK, et al. Carboxymethylation of corn starch and characterization using assymetrical flow field-flow fractionation coupled with multiangle light scattering. Journal of Chromatography A. 2010;1217:4623–4628. https://doi.org/10.1016/j.chroma.2010.04.082
  15. Bhattacharyya D, Singhal RS, Kulkarni PR. Physicochemical properties of carboxymethyl starch prepared from corn and waxy amaranth starch. Carbohydrate Polymers. 1995;27:167–169. https://doi.org/10.1016/0144-8617(95)00062-C
  16. Patil S, Bharimalla AK, Mahapatra A, Dhakane-Lad J, Arputharaj A, et al. Effect of polymer blending on mechanical and barrier properties of starch-polyvinyl alcohol based biodegradable composite films. Food Bioscience. 2021;44(Part A):101352. https://doi.org/10.1016/j.fbio.2021.101352
  17. Phattarateera S, Xin L, Amphong C, et al. Comparative studies of starch blends on the properties of PVA films. Carbohydrate Polymer Technologies and Applications. 2023;6:100340. https://doi.org/10.1016/j.carpta.2023.100340
  18. Yurong G, Dapeng L. Preparation and characterization of corn starch/PVA/glycerol composite films incorporated with ε-polylysine as a novel antimicrobial packaging material. e-Polymers. 2020;20(1):154–161. https://doi.org/10.1515/epoly-2020-0019
  19. Idris A, Muntean A, Mesic B, Lestelius M, et al. Oxygen barrier performance of poly(vinyl alcohol) coating films with different induced crystallinity and model predictions. 2021;11(10):1253. https://doi.org/10.3390/coatings11101253
  20. Deng H, Su J, Zhang W, Khan A, Sani MA, et al. A review of starch/polyvinyl alcohol (PVA) blend film: A potential replacement for traditional plastic-based food packaging film. International Journal of Biological Macromolecules. 2024;273(Part 1):132926. https://doi.org/10.1016/j.ijbiomac.2024.132926
  21. Gierszewska M, Jakubowska E, Olewnik-Kruszkowska E. Effect of chemical crosslinking on properties of chitosan montmorillonite composites. Polymer Testing. 2019;77:105872. https://doi.org/10.1016/j.polymertesting.2019.04.019
  22. Rammak T, Boonsuk P, Kaewtatip K. Mechanical and barrier properties of starch blend films enhanced with kaolin for application in food packaging. International Journal of Biological Macromolecules. 2021;192:1013–1020. https://doi.org/10.1016/j.ijbiomac.2021.10.081
  23. Kumari P, Kumari N, Mohan C, et al. Augmenting barrier efficiency in clay‐based starch composite films for enhanced packaging sustainability. Polymers for Advanced Technologies. 2024;35(6):e6458. https://doi.org/10.1002/pat.6458
  24. Labelle MA, Ispas-Szabo P, Vilotte F, et al. Carboxymethyl starch films as enteric coatings: Processing and mechanistic insights. Journal of Pharmaceutical Sciences. 2024;113(3):725–734. https://doi.org/10.1016/j.xphs.2023.09.002
  25. Wilpiszewska K. Hydrophilic films based on starch and carboxymethyl starch. Green Sciences. 2019;21(2):26–30. https://doi.org/10.2478/pjct-2019-0016
  26. Garavand Y, Taheri-Garavand A, Garavand F, Shahbazi F, Khodaei D, et al. Starch-polyvinyl alcohol-based films reinforced with chitosan nanoparticles: Physical, mechanical, structural, thermal and antimicrobial properties. Applied Sciences. 2022;12(3):1111. https://doi.org/10.3390/app12031111
  27. Omoike BA, Okieimen FE, Imoisi C. Design and optimization of eco-friendly biocomposite films for packaging applications using response surface methodology. Tanzania Journal of Science. 2024;50(5):961–974.
  28. Turan D. Water vapor transport properties of polyurethane films for packaging of respiring foods. Food Engineering Reviews. 2021;13:54–65. https://doi.org/10.1007/s12393-019-09205-z
  29. Omoike BA, Okieimen FE, Imoisi C. Water vapour transport properties of cassava starch/poly(vinyl alcohol) films via experimental and fickian methods. Trends in Applied Sciences Research. 2024;19(1):225–232. https://doi.org/10.3923/tasr.2024.225.232
  30. Chaisuwan K, Anurakumphan D, Hemmanee S, Ruamcharoen I, Leelakriangsak M. Soil burial degradation of starchbased films on microbial load and plant growth. Journal of Sustainability Science and Management 2023;18(3):110–124. https://doi.org/10.46754/jssm.2023.03.008
  31. Rydz J, Šišková A, Eckstein AA. Scanning electron microscopy and atomic force microscopy: Topographic and dynamical surface studies of blends, composites, and hybrid functional materials for sustainable future. Advances in Materials Science and Engineering. 2019;2019:681785. https://doi.org/10.1155/2019/6871785
  32. Nath D, Singh F, Das R. X-ray diffraction analysis by Williamson-Hall, Halder-Wagner and size-strain plot methods of CdSe nanoparticles- a comparative study. Materials Chemistry and Physics. 2020;239:122021. https://doi.org/10.1016/j.matchemphys.2019.122021
  33. Yang L, Xie M, Fang J, Zhang T, Wang X, et al. Effect of additives on properties of cross-linked carboxymethyl starch/polyvinyl alcohol composite films. Journal of Applied Polymer Science. 2022;139(4):51546. https://doi.org/10.1002/app.51546
  34. Manimaran M, Norizan MN, Kassim MHM, Adam MR, Norrrahim MNF, et al. Critical assessment of the thermal stability and degradation of chemically functionalized nanocellulose-based polymer nanocomposites. Nanotechnology Reviews. 2024;13(1):20240005. https://doi.org/10.1515/ntrev-2024-0005
  35. Quilez-Molina AI, Meins JFL, Charrier B, Dumon M. Starch-fibers composites, a study of all-polysaccharide foams from microwave foaming to biodegradation. Carbohydrate Polymers. 2024;328:121743. https://doi.org/10.1016/j.carbpol.2023.121743
  36. Luchese CL, Benelli P, Spada JC, Tessaro IC. Impact of the starch source on the physicochemical properties and biodegradability of different starch-based films. Journal of Applied Polymer Science. 2018;135(33):46564. https://doi.org/10.1002/app.46564
  37. Basiak E, Lenart A, Debeaufort F. Effect of starch type on the physico-chemical properties of edible films. International Journal of Biological Macromolecules. 2017;98:348–356. https://doi.org/10.1016/j.ijbiomac.2017.01.122
  38. Tan L, Sun B, Luo W, Liu S, Qiu B, et al. Enhanced mechanical property and water solubility of polyvinyl alcohol film via constructing hydrogen-bond network by adding carboxymethyl chitosan. Journal of Macromolecular Science, Part A. 2023;61(1):31–39. https://doi.org/10.1080/10601325.2023.2283045
  39. Ariffin A, Ariff ZM, Jikan SS. Effects of kaolin and maleic anhydride contents on melt elasticity and flexural behaviour of polypropylene/kaolin and unplasticised poly(vinyl chloride)/kaolin composites. e-Polymers. 2010;10(1):095. https://doi.org/10.1515/epoly.2010.10.1.1069
  40. Essabir H, Raji M, Bouhfid R, Qaiss AE. Hybrid nanocomposites based on graphene and nano-clay: Preparation, characterization, and synergistic effect. In: Qaiss AK, Bouhfid R, Jawaid M, editors. Graphene and Nanoparticles Hybrid Nanocomposites. Singapore: Springer; 2021, pp. 153–181. https://doi.org/10.1007/978-981-33-4988-9_5
  41. Luo Q, Hossen MA, Zeng Y, Dai J, Li S, et al. Gelatin-based composite films and their application in food packaging: A review. Journal of Food Engineering. 2022;313:110762. https://doi.org/10.1016/j.jfoodeng.2021.110762
  42. Dharini V, Selvam SP, Jayaramudu J, Emmanuel RS. Functional properties of clay nanofillers used in the biopolymerbased composite films for active food packaging applications – Review. Applied Clay Science. 2022;226:106555. https://doi.org/10.1016/j.clay.2022.106555
  43. Ma N, Dong W, Qin D, Dang C, Xie S, et al. Green and renewable thermoplastic polyvinyl alcohol/starch blend film fabricated by melt processing. International Journal of Biological Macromolecules. 2024;279(Part 2):134866. https://doi.org/10.1016/j.ijbiomac.2024.134866
  44. Castro JM, Montalbán MG, Martínez-Pérez N, Domene-López D, Pérez JM, et al. Thermoplastic starch/polyvinyl alcohol blend modification by citric acid–glycerol polyesters. International Journal of Biological Macromolecules. 2023;244:125478. https://doi.org/10.1016/j.ijbiomac.2023.125478
  45. Abedi-Firoozjah R, Chabook N, Rostami O, Heydari M, Kolahdouz-Nasiri A, et al. PVA/starch films: An updated review of their preparation, characterization, and diverse applications in the food industry. Polymer Testing. 2023;118:107903. https://doi.org/10.1016/j.polymertesting.2022.107903
  46. Moshood TD, Nawanir G, Mahmud F, Mohamad F, Ahmad MH, et al. Sustainability of biodegradable plastics: New problem or solution to solve the global plastic pollution? Current Research in Green and Sustainable Chemistry. 2022;5:100273. https://doi.org/10.1016/j.orgsc.2022.100273
  47. Zee MV. Methods for evaluating the biodegradability of environmentally degradable polymers. In: Bastioli C. editor. Handbook of Biodegradable Polymers. Berlin, Boston: De Gruyter; 2020, pp. 1–22. https://doi.org/10.1515/9781501511967-001
  48. Mittal A, Garg S, Premi A, Giri AS. Synthesis of polyvinyl alcohol/modified starch-based biodegradable nanocomposite films reinforced with starch nanocrystals for packaging applications. Polymers and Polymer Composites. 2020;29(5):405–416. https://doi.org/10.1177/0967391120922429
  49. Lin YP, Dhib R, Mehrvar M. Recent advances in dynamic modeling and process control of PVA degradation by biological and advanced oxidation processes: A review on trends and advances. Environments. 2021;8(11):116. https://doi.org/10.3390/environments8110116
  50. Lv Z, Meng X, Sun S, Jiang T, Zhang S, et al. Biodegradable carboxymethyl chitosan/polyvinyl alcohol hymexazol-loaded mulch film for soybean root rot control. Agronomy. 2023;13(9):2205. https://doi.org/10.3390/agronomy13092205
  51. Abdullah ZW, Dong Y. Biodegradable and water resistant poly(vinyl) alcohol (PVA)/starch (ST)/glycerol (GL)/halloysite nanotube (HNT) nanocomposite films for sustainable food packaging. Frontiers in Materials. 2019;6:58. https://doi.org/10.3389/fmats.2019.00058
Как цитировать?
Omoike BA, Okieimen FE, Imoisi C. Developing composite films from carboxymethyl starch, polyvinyl alcohol, and kaolin for sustainable packaging applications. Foods and Raw Materials. 2026;14(2):344–356. https://doi.org/10.21603/2308-4057-2026-2-681 
О журнале