Crystallization Kinetics and Morphological Shifts in Polylactic Acid/Nanocellulose Blends Under Isothermal Melt Conditions

Notice

This is an unedited manuscript accepted for publication and provided as an Article in Press for early access at the author’s request. The article will undergo copyediting, typesetting, and galley proof review before final publication. Please be aware that errors may be identified during production that could affect the content. All legal disclaimers of the journal apply.

Year : 2026 | Volume : 14 | 04 | Page :
By

Kiran Kumar M,

Madhukumar K,

Sasikumar N,

S B G Tilak Babu,

Azeezaa. V,

Santosh Kumar Nathsharma,

  1. Associate Professor, Department of Mechanical Engineering, Sir M Visvesvaraya Institute of Technology, Bangalore, Karnataka, India
  2. Associate Professor, Department of Mechanical Engineering, Sir M Visvesvaraya Institute of Technology, Bangalore, Karnataka, India
  3. Assistant Professor, Department of Physics, Sir M Visvesvaraya Institute of Technology, Bangalore, Karnataka, India
  4. Assistant Professor, Department of Electronics and Communication Engineering, Aditya University, Surampalem, Tamil Nadu, India
  5. Associate Professor, Department of Physics, Rajalakshmi Engineering College, Chennai, Tamil Nadu, India
  6. Lecturer, Department of Chemistry, Stewart Science College, Cuttack, Odisha, India

Abstract

The great potential of polylactic acid as a sustainable biopolymer for packaging, biomedical materials, and additive manufacturing, polylactic acid’s slow crystallization kinetics during melt processing causes it to be poorly crystallized, thermally weak, and mechanically underperforming. Crystallization models of PLA/nanocellulose blends have been limited to isothermal melt crystallization kinetics and the resulting morphological changes. The phenomena discussed in this work are systematically explored by melt compounding of polylactic acid with cellulose nanocrystals at different concentrations (from 1 to 5 wt.%) and subsequent isothermal differential scanning calorimetry, Avrami kinetic modeling, polarized optical microscopy, and scanning electron microscopy. The results show that crystallinity goes up from 30.5% to 43.4%, the half crystallization time decreases from 18.4 min to 6.2 min and the crystallite size becomes smaller and denser while cellulose nanocrystals is added into the mixture at 3 wt.% concentration at 120°C. The following improvements yield better flexural strength and thermal stability than neat polylactic acid and more recent literature. The results will be valuable inputs for optimizing the processing and development of advanced manufacturing applications of polylactic acid-based sustainable composites in industrial processing.

Keywords: Isothermal Melt Crystallization, Polylactic Acid, Biocomposites, Morphological Shifts.

How to cite this article: Kiran Kumar M, Madhukumar K, Sasikumar N, S B G Tilak Babu, Azeezaa. V, Santosh Kumar Nathsharma. Crystallization Kinetics and Morphological Shifts in Polylactic Acid/Nanocellulose Blends Under Isothermal Melt Conditions. Journal of Polymer & Composites. 2026; 14(04):-.
How to cite this URL: Kiran Kumar M, Madhukumar K, Sasikumar N, S B G Tilak Babu, Azeezaa. V, Santosh Kumar Nathsharma. Crystallization Kinetics and Morphological Shifts in Polylactic Acid/Nanocellulose Blends Under Isothermal Melt Conditions. Journal of Polymer & Composites. 2026; 14(04):-. Available from: https://journals.stmjournals.com/jopc/article=2026/view=254886

References

  1. Clarkson CM, El Awad Azrak SM, Schueneman GT, Snyder JF, Youngblood JP. Crystallization kinetics and morphology of small concentrations of cellulose nanofibrils (CNFs) and cellulose nanocrystals (CNCs) melt-compounded into poly(lactic acid) (PLA) with plasticizer. Polymer (Guildf). 2020;187:122101. doi:10.1016/j.polymer.2019.122101.
  2. Dhar P, Bhasney SM, Kumar A, Katiyar V. Acid functionalized cellulose nanocrystals and its effect on mechanical, thermal, crystallization and surface properties of poly(lactic acid) bionanocomposite films: A comprehensive study. Polymer (Guildf). 2016;101:75-92. doi:10.1016/j.polymer.2016.08.028.
  3. Alanalp MB, Ozdemir B, Nofar M, Durmus A. Isothermal and non-isothermal cold crystallization kinetics of polylactide/cellulose nanocrystal (PLA/CNC) nanocomposites. J Therm Anal Calorim. 2022;147(24):14211-14227. doi:10.1007/s10973-022-11598-9.
  4. Shazleen SS, Foong Ng LY, Ibrahim NA, Hassan MA, Ariffin H. Combined effects of cellulose nanofiber nucleation and maleated polylactic acid compatibilization on the crystallization kinetic and mechanical properties of polylactic acid nanocomposite. Polymers (Basel). 2021;13(19):3226. doi:10.3390/polym13193226.
  5. Galera Manzano LM, Ruz Cruz MA, Moo Tun NM, Valadez González A, Mina Hernandez JH. Effect of cellulose and cellulose nanocrystal contents on the biodegradation, under composting conditions, of hierarchical PLA biocomposites. Polymers (Basel). 2021;13(11):1855. doi:10.3390/polym13111855.
  6. Meng W, et al. Mechanical properties and non-isothermal crystallization kinetics of polylactic acid modified by polyacrylic elastomers and cellulose nanocrystals. Polymers (Basel). 2023;15(18):3767. doi:10.3390/polym15183767.
  7. Ahmad ND, Kusmono, Wildan MW, Herianto. Preparation and properties of cellulose nanocrystals-reinforced poly(lactic acid) composite filaments for 3D printing applications. Results Eng. 2023;17:100842. doi:10.1016/j.rineng.2022.100842.
  8. Manickaraj K, et al. Improving mechanical performance of hybrid polymer composites: Incorporating banana stem leaf and jute fibers with tamarind shell powder. BioResources. 2025;20(1):1998-2025. doi:10.15376/biores.20.1.1998-2025.
  9. Yang B, Wan X. Trace sorbitol-modified nano-silica: Towards nano-nucleation for poly(L-lactic acid). Int J Biol Macromol. 2024;274:133236. doi:10.1016/j.ijbiomac.2024.133236.
  10. Rahmanifard M, Matin A, Farizeh T, Khonakdar HA, Hemmati F. Extrusion foaming of biodegradable poly(lactic acid)/nanosilica nanocomposites: Correlations of the phenomena involved in reactive extrusion process-microstructure-foam final properties. Int J Biol Macromol. 2025;319:145609. doi:10.1016/j.ijbiomac.2025.145609.
  11. Agbakoba VC, Mokhena TC, Ferg EE, Hlangothi SP, John MJ. PLA bio-nanocomposites reinforced with cellulose nanofibrils (CNFs) for 3D printing applications. Cellulose. 2023;30(18):11537-11559. doi:10.1007/s10570-023-05549-2.
  12. Ding W, Chu RKM, Mark LH, Park CB, Sain M. Non-isothermal crystallization behaviors of poly(lactic acid)/cellulose nanofiber composites in the presence of CO2. Eur Polym J. 2015;71:231-247. doi:10.1016/j.eurpolymj.2015.07.054.
  13. Pei A, Zhou Q, Berglund LA. Functionalized cellulose nanocrystals as biobased nucleation agents in poly(L-lactide) (PLLA): Crystallization and mechanical property effects. Compos Sci Technol. 2010;70(5):815-821. doi:10.1016/j.compscitech.2010.01.018.
  14. Karimi S, Ghasemi I, Abbassi-Sourki F. A study on the crystallization kinetics of PLLA in the presence of graphene oxide and PEG-grafted graphene oxide: Effects on the nucleation and chain mobility. Compos B Eng. 2019;158:302-310. doi:10.1016/j.compositesb.2018.10.004.
  15. Palanisamy S, et al. Effects of fiber loadings and lengths on mechanical properties of Sansevieria cylindrica fiber reinforced natural rubber biocomposites. Mater Res Express. 2023;10(8):085503. doi:10.1088/2053-1591/acefb0.
  16. Ruz-Cruz MA, Herrera-Franco PJ, Flores-Johnson EA, Moreno-Chulim MV, Galera-Manzano LM, Valadez-González A. Thermal and mechanical properties of PLA-based multiscale cellulosic biocomposites. J Mater Res Technol. 2022;18:485-495. doi:10.1016/j.jmrt.2022.02.072.
  17. Bolat F, Necolau MI, Bîru EI, Zaharia A, Iovu H. Comparative analysis of solvent casting and Pickering emulsion techniques for improving the mechanical properties of surface-modified cellulose nanomaterial-reinforced polylactic acid composites. Polymers (Basel). 2024;16(23):3406. doi:10.3390/polym16233406.
  18. Aigaje E, Riofrio A, Baykara H. Processing, properties, modifications, and environmental impact of nanocellulose/biopolymer composites: A review. Polymers (Basel). 2023;15(5):1219. doi:10.3390/polym15051219.
  19. Palaniappan M, et al. Influence of washing with sodium lauryl sulphate (SLS) surfactant on different properties of ramie fibres. BioResources. 2024;19(2):2609-2625. doi:10.15376/biores.19.2.2609-2625.
  20. Li YD, Fu QQ, Wang M, Zeng JB. Morphology, crystallization and rheological behavior in poly(butylene succinate)/cellulose nanocrystal nanocomposites fabricated by solution coagulation. Carbohydr Polym. 2017;164:75-82. doi:10.1016/j.carbpol.2017.01.089.
  21. Bachtiar D, et al. Effect of alkaline treatment on the thermal and mechanical properties of sugar palm fibre reinforced thermoplastic polyurethane composites. Sci Rep. 2025;15(1):14085. doi:10.1038/s41598-025-99227-x.
  22. Mokhena TC, Sefadi JS, Sadiku ER, John MJ, Mochane MJ, Mtibe A. Thermoplastic processing of PLA/cellulose nanomaterials composites. Polymers (Basel). 2018;10(12):1363. doi:10.3390/polym10121363.
  23. Parhizgar M, Azadfallah M, Kaboorani A, Mastouri A, Frigione M. Development of cellulose nanocrystal (CNC)-reinforced PLA/PMMA nanocomposite coatings for sustainable paper-based packaging. Polymers (Basel). 2026;18(2):175. doi:10.3390/polym18020175.
  24. Kar A, Saikia D, Palanisamy S, Pandiarajan N. Calamus tenuis fiber reinforced epoxy composites: Effect of fiber loading on the tensile, structural, crystalline, thermal and morphological characteristics. J Polym Res. 2024;31(11):323. doi:10.1007/s10965-024-04162-6.
  25. Kar A, Saikia D, Palanisamy S, Pandiarajan N. Effect of fiber loading on the mechanical, morphological, and dynamic mechanical characteristics of Calamus tenuis fiber reinforced epoxy composites. J Vinyl Addit Technol. 2025;31(1):224-240. doi:10.1002/vnl.22167.
  26. Bayat P, Anstey A, Dubé MA, Morse T, Cunningham MF, Meek KM. Effect of carboxylated cellulose nanocrystal acetylation on PLA nanocomposite crystallization behavior. Compos Part C Open Access. 2025;18:100673. doi:10.1016/j.jcomc.2025.100673.
  27. Abrantes S, Magalhães da Silva S, Lima PS, Oliveira JM. Non-isothermal cold crystallization kinetics of leather polymer composites for additive manufacturing. J Therm Anal Calorim. 2025;150(7):5159-5173. doi:10.1007/s10973-025-14105-y.
Ahead of Print Subscription Original Research
Volume 14
04
Received 20/07/2026
Accepted 06/08/2026
Published 07/09/2026
Publication Time 49 Days

Login

My IP

PlumX Metrics