Molecular engineering of nanocellulose-poly(lactic acid) bio-nanocomposite interface by reactive surface grafting from copolymerization

Gaoyuan Ye; Qiwen Yong; Liqiu Hu; Emil Rosqvist; Jouko Peltonen; Yingcheng Hu; Wenyang Xu; Chunlin Xu

doi:10.1016/j.ijbiomac.2025.141371

Molecular engineering of nanocellulose-poly(lactic acid) bio-nanocomposite interface by reactive surface grafting from copolymerization

Gaoyuan Ye
, Qiwen Yong
, Liqiu Hu
, Emil Rosqvist
, Jouko Peltonen
, Yingcheng Hu
, Wenyang Xu
, Chunlin Xu

Research output: Contribution to journal › Article › Scientific › peer-review

4 Citations (Scopus)

45 Downloads (Pure)

Abstract

Poly(lactic acid) (PLA) is a widely reusable polymer, but its practical applications are greatly constrained by low toughness and poor crystallinity. In this study, the modified cellulose nanocrystal (CNC) was designed as a reinforcement through surface copolymerization of caprolactone (CL) and allyl caprolactone (ACL) to enhance the properties of PLA. The surface molecular engineering of reactive core-shell nanofillers (allyl polycaprolactone-grafted CNC, or CNC-g-APCL) effectively improved the interfacial compatibility between PLA and CNC through a straightforward in situ reactive extrusion process. The presence of elastic polycaprolactone (PCL) and allyl polycaprolactone (APCL) rendered good energy dissipation as evidenced by the improved toughness and elongation at break of the PLA/CNC hybrid composites. More importantly, the integrated CNC composite presented an extremely high crystallinity of 45.1%, which is top-ranking among all reported studies on PLA/CNC nanocomposites. In summary, this research introduces an innovative method for designing nanocomposites with improved interfacial compatibility between the matrix and components by grafting copolymerization and reactive extrusion, providing a universal solution to the mechanical and crystalline deficiencies often observed in biodegradable polymers.

Original language	English
Article number	141371
Journal	International Journal of Biological Macromolecules
Volume	306
Issue number	Part 1
DOIs	https://doi.org/10.1016/j.ijbiomac.2025.141371
Publication status	Published - May 2025
MoE publication type	A1 Journal article-refereed

Funding

G. Y. thanks the support of Scientific Research Foundation of Zhejiang A & F University (2023LFR079) and Fundamental Research Funds for the Central Universities (2572020AW46). G. Y. and L. H. would like to acknowledge the financial support from the China Scholarship Council (Student ID 202006600016 for G. Y. and Student ID 201908120107 for L. H.). W. X. appreciates the funding from the Jane and Aatos Erkko Foundation (Project: Healing the wounds with Finnish woods) and Academy of Finland (Funding decision. No. 349109). E. R. wishes to acknowledge the funding from the Jane and Aatos Erkko Foundation (Project: ABC Health). Dr. Hao Zhang is thanked for his help with performing XRD measurements. Mr. Linus Silvander is acknowledged for SEM imaging. Ms. Ellen Sundstr\u00F6m and Mr. Peter Uppstu are thanked for his help on Rheology measurements. Mr. Oskar Backman is acknowledged for his help in 3D printing. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) at \u00C5AU. Parts of the research used Research Council of Finland Research Infrastructure 'Printed Intelligence Infrastructure' (PII-FIRI). G. Y. thanks the support of Scientific Research Foundation of Zhejiang A & F University ( 2023LFR079 ) and Fundamental Research Funds for the Central Universities ( 2572020AW46 ). G. Y. and L. H. would like to acknowledge the financial support from the China Scholarship Council (Student ID 202006600016 for G. Y. and Student ID 201908120107 for L. H.). W. X. appreciates the funding from the Jane and Aatos Erkko Foundation (Project: Healing the wounds with Finnish woods) and Academy of Finland (Funding decision. No. 349109 ). E. R. wishes to acknowledge the funding from the Jane and Aatos Erkko Foundation (Project: ABC Health). Dr. Hao Zhang is thanked for his help with performing XRD measurements. Mr. Linus Silvander is acknowledged for SEM imaging. Ms. Ellen Sundstr\u00F6m and Mr. Peter Uppstu are thanked for his help on Rheology measurements. Mr. Oskar Backman is acknowledged for his help in 3D printing. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) at \u00C5AU.

Keywords

Surface copolymerization
Reactive extrusion
Polylactic acid (PLA)

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1-s2.0-S0141813025019221-mainFinal published version, 6.77 MBLicence: CC BY

Cite this

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title = "Molecular engineering of nanocellulose-poly(lactic acid) bio-nanocomposite interface by reactive surface grafting from copolymerization",

abstract = "Poly(lactic acid) (PLA) is a widely reusable polymer, but its practical applications are greatly constrained by low toughness and poor crystallinity. In this study, the modified cellulose nanocrystal (CNC) was designed as a reinforcement through surface copolymerization of caprolactone (CL) and allyl caprolactone (ACL) to enhance the properties of PLA. The surface molecular engineering of reactive core-shell nanofillers (allyl polycaprolactone-grafted CNC, or CNC-g-APCL) effectively improved the interfacial compatibility between PLA and CNC through a straightforward in situ reactive extrusion process. The presence of elastic polycaprolactone (PCL) and allyl polycaprolactone (APCL) rendered good energy dissipation as evidenced by the improved toughness and elongation at break of the PLA/CNC hybrid composites. More importantly, the integrated CNC composite presented an extremely high crystallinity of 45.1\%, which is top-ranking among all reported studies on PLA/CNC nanocomposites. In summary, this research introduces an innovative method for designing nanocomposites with improved interfacial compatibility between the matrix and components by grafting copolymerization and reactive extrusion, providing a universal solution to the mechanical and crystalline deficiencies often observed in biodegradable polymers.",

keywords = "Surface copolymerization, Reactive extrusion, Polylactic acid (PLA)",

author = "Gaoyuan Ye and Qiwen Yong and Liqiu Hu and Emil Rosqvist and Jouko Peltonen and Yingcheng Hu and Wenyang Xu and Chunlin Xu",

year = "2025",

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doi = "10.1016/j.ijbiomac.2025.141371",

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T1 - Molecular engineering of nanocellulose-poly(lactic acid) bio-nanocomposite interface by reactive surface grafting from copolymerization

AU - Ye, Gaoyuan

AU - Yong, Qiwen

AU - Hu, Liqiu

AU - Rosqvist, Emil

AU - Peltonen, Jouko

AU - Hu, Yingcheng

AU - Xu, Wenyang

AU - Xu, Chunlin

PY - 2025/5

Y1 - 2025/5

N2 - Poly(lactic acid) (PLA) is a widely reusable polymer, but its practical applications are greatly constrained by low toughness and poor crystallinity. In this study, the modified cellulose nanocrystal (CNC) was designed as a reinforcement through surface copolymerization of caprolactone (CL) and allyl caprolactone (ACL) to enhance the properties of PLA. The surface molecular engineering of reactive core-shell nanofillers (allyl polycaprolactone-grafted CNC, or CNC-g-APCL) effectively improved the interfacial compatibility between PLA and CNC through a straightforward in situ reactive extrusion process. The presence of elastic polycaprolactone (PCL) and allyl polycaprolactone (APCL) rendered good energy dissipation as evidenced by the improved toughness and elongation at break of the PLA/CNC hybrid composites. More importantly, the integrated CNC composite presented an extremely high crystallinity of 45.1%, which is top-ranking among all reported studies on PLA/CNC nanocomposites. In summary, this research introduces an innovative method for designing nanocomposites with improved interfacial compatibility between the matrix and components by grafting copolymerization and reactive extrusion, providing a universal solution to the mechanical and crystalline deficiencies often observed in biodegradable polymers.

AB - Poly(lactic acid) (PLA) is a widely reusable polymer, but its practical applications are greatly constrained by low toughness and poor crystallinity. In this study, the modified cellulose nanocrystal (CNC) was designed as a reinforcement through surface copolymerization of caprolactone (CL) and allyl caprolactone (ACL) to enhance the properties of PLA. The surface molecular engineering of reactive core-shell nanofillers (allyl polycaprolactone-grafted CNC, or CNC-g-APCL) effectively improved the interfacial compatibility between PLA and CNC through a straightforward in situ reactive extrusion process. The presence of elastic polycaprolactone (PCL) and allyl polycaprolactone (APCL) rendered good energy dissipation as evidenced by the improved toughness and elongation at break of the PLA/CNC hybrid composites. More importantly, the integrated CNC composite presented an extremely high crystallinity of 45.1%, which is top-ranking among all reported studies on PLA/CNC nanocomposites. In summary, this research introduces an innovative method for designing nanocomposites with improved interfacial compatibility between the matrix and components by grafting copolymerization and reactive extrusion, providing a universal solution to the mechanical and crystalline deficiencies often observed in biodegradable polymers.

KW - Surface copolymerization

KW - Reactive extrusion

KW - Polylactic acid (PLA)

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DO - 10.1016/j.ijbiomac.2025.141371

M3 - Article

SN - 0141-8130

VL - 306

JO - International Journal of Biological Macromolecules

JF - International Journal of Biological Macromolecules

IS - Part 1

M1 - 141371

ER -

Molecular engineering of nanocellulose-poly(lactic acid) bio-nanocomposite interface by reactive surface grafting from copolymerization

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Keywords

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