Drying-Induced Hornification in Cellulose Nanofiber–PLA Composites Improving Mechanical and Thermal Stability

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Published Jul 31, 2026
https://doi.org/10.55043/jfpc.v5i2.587
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Vol. 5 No. 2 (2026): Journal of Fibers and Polymer Composites

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Sholahuddin Sholahuddin
Universitas Muhammadiyah Yogyakarta
Eka Fitriastuti
Nusantara Scientific Research Center
Dian Yosi Arinawati
Universitas Muhammadiyah Yogyakarta

Abstract

Steam explosion pretreatment is widely used to facilitate the production of cellulose nanofibers (CNFs) from lignocellulosic biomass; however, the influence of pretreatment severity on the performance of CNF-reinforced polylactic acid (PLA) composites remains insufficiently understood. This study investigated the effect of steam explosion pressures of 35 and 40 atm on the mechanical, thermal, and morphological properties of CNF/PLA composites prepared from oil palm empty fruit bunches (EFB). CNFs were produced by steam explosion followed by mechanical fibrillation and incorporated into a PLA matrix at a 1:1 dry weight ratio. The composite prepared using 35 atm exhibited superior mechanical performance, with a tensile strength of 9.22 ± 0.01 MPa and a Young's modulus of 2.26 ± 0.12 GPa. Increasing the pretreatment pressure to 40 atm slightly delayed the onset of thermal degradation and reduced the cold crystallization temperature, suggesting enhanced heterogeneous nucleation during heating. However, the higher pressure also reduced tensile properties and significantly decreased the residual char content, indicating more extensive removal of lignin and possible hornification and partial cellulose depolymerization. These results demonstrate a trade-off between mechanical reinforcement and thermal performance as pretreatment severity increases. Overall, a steam explosion pressure of 35 atm provided the most balanced combination of mechanical and thermal properties, offering useful guidance for optimizing CNF-reinforced PLA biocomposites derived from oil palm biomass.

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Author Biographies

Sholahuddin Sholahuddin, Universitas Muhammadiyah Yogyakarta

Department of Agrotechnology, Faculty of Agriculture, Universitas Muhammadiyah Yogyakarta, Bantul, Indonesia

Eka Fitriastuti, Nusantara Scientific Research Center

Nusantara Scientific Research Center, Bantul, Indonesia

Dian Yosi Arinawati, Universitas Muhammadiyah Yogyakarta

Department of Oral Biology, Faculty of Dentistry, Universitas Muhammadiyah Yogyakarta, Bantul, Indonesia

How to Cite
Sholahuddin, S., Fitriastuti, E., & Arinawati, D. Y. (2026). Drying-Induced Hornification in Cellulose Nanofiber–PLA Composites Improving Mechanical and Thermal Stability. Journal of Fibers and Polymer Composites, 5(2), 177–194. https://doi.org/10.55043/jfpc.v5i2.587

References

  1. Rajendran DS, Venkataraman S, Jha SK, Chakrabarty D, Kumar VV. A review on bio-based polymer polylactic acid potential on sustainable food packaging. Food Sci Biotechnol 2024;33:1759–88. https://doi.org/10.1007/s10068-024-01543-x.
  2. Domenek S, Louaifi A, Guinault A, Baumberger S. Potential of Lignins as Antioxidant Additive in Active Biodegradable Packaging Materials. J Polym Environ 2013;21:692–701. https://doi.org/10.1007/s10924-013-0570-6.
  3. Mosab Kaseem, Zeeshan Ur Rehman SH, Dikici AKS and B. A Review on Synthesis, Properties, and Applications of Polylactic Acid/Silica Composite. Lecture Notes in Mechanical Engineering 2024:703–20. https://doi.org/10.1007/978-981-97-3173-2_49.
  4. Asada C, Sholahuddin, Nakamura Y. Lignin as a Coating and Curing Agent on Biodegradable Epoxy Resins. In: Gutiérrez TJ, editor. Reactive and Functional Polymers Volume One, Springer International Publishing; 2020, p. 195–206. https://doi.org/10.1007/978-3-030-43403-8_9.
  5. Gray D. Nanocellulose: From Nature to High Performance Tailored Material 2013;67:353. https://doi.org/10.1515/hf-2013-0027.
  6. Klemm D, Kramer F, Moritz S, Lindström T, Ankerfors M, Gray D, et al. Nanocelluloses: A New Family of Nature-Based Materials. Angew Chem Int Ed 2011;50:5438–66. https://doi.org/10.1002/anie.201001273.
  7. Fernandes Diniz JMB, Gil MH, Castro J. Hornification—its origin and interpretation in wood pulps. Wood Sci Technol 2004;37:489–94.
  8. Hubbe MA, Rojas OJ, Lucia LA. Green Modification of Surface Characteristics of Cellulosic Materials at the Molecular or Nano Scale: A Review. Bioresources 2015;10.
  9. Asada C, Sholahuddin, Nakamura Y. Biorefinery System of Lignocellulosic Biomass Using Steam Explosion. In: Sand A, Banga S, editors. Cellulose Science and Derivatives, London: intechOpen; 2021, p. 73–98. https://doi.org/10.5772/intechopen.98544.
  10. Sholahuddin S, Arinawati DY, Setiawan CK, Utama NA, Prabasari I, Budiyanto G, et al. Characterization of Cellulose Nanofiber (CNF) from Steam-exploded Palm Oil Kernel Fibers Followed by Supermasscolloider. IOP Conf Ser Earth Environ Sci 2024;1417. https://doi.org/10.1088/1755-1315/1417/1/012038.
  11. Asada C, Honjo K, Nakamura Y. Utilization of Steam-Treated and Milling-Treated Lignin from Moso Bamboo as Curing Agent of Epoxy Resin. Waste Biomass Valorization 2021;12:6261–72. https://doi.org/10.1007/s12649-021-01444-8.
  12. Özdemir B, Nofar M. Effect of solvent type on the dispersion quality of spray-and freeze-dried CNCs in PLA through rheological analysis. Carbohydr Polym 2021;268. https://doi.org/10.1016/j.carbpol.2021.118243.
  13. Shazleen SS, Yasim-Anuar TAT, Ibrahim NA, Hassan MA, Ariffin H. Functionality of cellulose nanofiber as bio-based nucleating agent and nano-reinforcement material to enhance crystallization and mechanical properties of polylactic acid nanocomposite. Polymers (Basel) 2021;13:1–19. https://doi.org/10.3390/polym13030389.
  14. Ding Q, Zeng J, Wang B, Tang D, Chen K, Gao W. Effect of nanocellulose fiber hornification on water fraction characteristics and hydroxyl accessibility during dehydration. Carbohydr Polym 2019;207:44–51. https://doi.org/10.1016/j.carbpol.2018.11.075.
  15. Dufresne A. Nanocellulose: A new ageless bionanomaterial. Materials Today 2013;16:220–7. https://doi.org/10.1016/j.mattod.2013.06.004.
  16. Jonoobi M, Harun J, Mathew AP, Oksman K. Mechanical properties of cellulose nanofiber (CNF) reinforced polylactic acid (PLA) prepared by twin screw extrusion. Compos Sci Technol 2010;70:1742–7. https://doi.org/10.1016/j.compscitech.2010.07.005.
  17. Overend RP, Chornet E, Gascoigne JA. Fractionation of Lignocellulosics by Steam-Aqueous Pretreatments [and Discussion]. Philosophical Transactions of the Royal Society of London Series A, Mathematical and Physical Sciences 1987;321:523–36.
  18. Gea S, Siregar AH, Zaidar E, Harahap M, Indrawan DP, Perangin-Angin YA. Isolation and characterisation of cellulose nanofibre and lignin from oil palm empty fruit bunches. Materials 2020;13. https://doi.org/10.3390/ma13102290.
  19. Spence KL, Venditti RA, Rojas OJ, Habibi Y, Pawlak JJ. A comparative study of energy consumption and physical properties of microfibrillated cellulose produced by different processing methods. Cellulose 2011;18:1097–111. https://doi.org/10.1007/s10570-011-9533-z.
  20. Iyer KA, Torkelson JM. Green composites of polypropylene and eggshell: Effective biofiller size reduction and dispersion by single-step processing with solid-state shear pulverization. Compos Sci Technol 2014;102:152–60. https://doi.org/10.1016/j.compscitech.2014.07.029.
  21. Le Duigou A, Davies P, Baley C. Macroscopic analysis of interfacial properties of flax/PLLA biocomposites. Compos Sci Technol 2010;70:1612–20. https://doi.org/10.1016/j.compscitech.2010.06.001.
  22. Hollingbery LA, Hull TR. The fire retardant effects of huntite in natural mixtures with hydromagnesite. Polym Degrad Stab 2012;97:504–12. https://doi.org/10.1016/j.polymdegradstab.2012.01.024.
  23. Lee KY, Aitomäki Y, Berglund LA, Oksman K, Bismarck A. On the use of nanocellulose as reinforcement in polymer matrix composites. Compos Sci Technol 2014;105:15–27. https://doi.org/10.1016/j.compscitech.2014.08.032.
  24. Bledzki AK, Jaszkiewicz A. Mechanical performance of biocomposites based on PLA and PHBV reinforced with natural fibres - A comparative study to PP. Compos Sci Technol 2010;70:1687–96. https://doi.org/10.1016/j.compscitech.2010.06.005.
  25. Iwatake A, Nogi M, Yano H. Cellulose nanofiber-reinforced polylactic acid. Compos Sci Technol 2008;68:2103–6. https://doi.org/10.1016/j.compscitech.2008.03.006.
  26. Suryanegara L, Nakagaito AN, Yano H. The effect of crystallization of PLA on the thermal and mechanical properties of microfibrillated cellulose-reinforced PLA composites. Compos Sci Technol 2009;69:1187–92. https://doi.org/10.1016/j.compscitech.2009.02.022.
  27. Chen W, Yu H, Liu Y. Preparation of millimeter-long cellulose i nanofibers with diameters of 30-80 nm from bamboo fibers. Carbohydr Polym 2011;86:453–61. https://doi.org/10.1016/j.carbpol.2011.04.061.
  28. Chen W, Yu H, Liu Y, Chen P, Zhang M, Hai Y. Individualization of cellulose nanofibers from wood using high-intensity ultrasonication combined with chemical pretreatments. Carbohydr Polym 2011;83:1804–11. https://doi.org/10.1016/j.carbpol.2010.10.040.
  29. Jofré Barud F, López S, Tapia A, Feresin GE, López ML. Attractant, sexual competitiveness enhancing and toxic activities of the essential oils from Baccharis spartioides and Schinus polygama on Ceratitis capitata Wiedemann. Ind Crops Prod 2014;62:299–304. https://doi.org/10.1016/j.indcrop.2014.08.045.
  30. Wang S, Copeland L. Nature of thermal transitions of native and acid-hydrolysed pea starch: Does gelatinization really happen? Carbohydr Polym 2012;87:1507–14. https://doi.org/10.1016/j.carbpol.2011.09.047.
  31. Grząbka-Zasadzińska A, Klapiszewski Ł, Bula K, Jesionowski T, Borysiak S. Supermolecular structure and nucleation ability of polylactide-based composites with silica/lignin hybrid fillers. J Therm Anal Calorim 2016;126:263–75. https://doi.org/10.1007/s10973-016-5311-3.
  32. Favier V, Canova GR, Cavaillé JY, Chanzy H, Dufresne A, Gauthier C. Nanocomposite materials from latex and cellulose whiskers. Polym Adv Technol 1995;6:351–5. https://doi.org/10.1002/pat.1995.220060514.
  33. Wang Q, Song H, Pan S, Dong N, Wang X, Sun S. Initial pyrolysis mechanism and product formation of cellulose: An Experimental and Density functional theory(DFT) study. Sci Rep 2020;10:1–18. https://doi.org/10.1038/s41598-020-60095-2.
  34. Hilbers TJ, Wang Z, Pecha B, Westerhof RJM, Kersten SRA, Pelaez-Samaniego MR, et al. Cellulose-Lignin interactions during slow and fast pyrolysis. J Anal Appl Pyrolysis 2015;114:197–207. https://doi.org/10.1016/j.jaap.2015.05.020.
  35. Zhu J, Du C. Interaction between lignin and cellulose during the pyrolysis process. Int J Biol Macromol 2024;265:131093. https://doi.org/10.1016/j.ijbiomac.2024.131093.
  36. Majka TM, Al Nakib R, Menceloglu YZ, Pielichowski K. The Influence of Lignin Derivatives on the Thermal Properties and Flammability of PLA+PET Blends. Materials 2025;18:1–33. https://doi.org/10.3390/ma18174181.
  37. Luo Q, Sun Q, Wu L, Yang Z. Structural characterization of an immunoregulatory polysaccharide from the fruiting bodies of Lepista sordida. Carbohydr Polym 2012;88:820–4. https://doi.org/10.1016/j.carbpol.2011.12.043.
  38. Faruk O, Bledzki AK, Fink HP, Sain M. Biocomposites reinforced with natural fibers: 2000-2010. Prog Polym Sci 2012;37:1552–96. https://doi.org/10.1016/j.progpolymsci.2012.04.003