TY - JOUR
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)
U2 - 10.1016/j.ijbiomac.2025.141371
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 -