Regulating surface molecular structure of cellulose nanocrystals to optimize mechanical reinforcement effect on hydrophobic bio-based polyesters


The classical approach to prepare nanocomposites is often applied to chemical or physical modification of nanofillers to improve interfacial interaction between nanofillers and matrices. However, those methods might disturb the original reinforcement of nanoparticles due to the inhibition and even the absence of association among fillers. Here, we inspected a molecular design strategy using rod-like cellulose nanocrystals (CNCs) as fillers to study whether regulating the surface structure of CNC could allow a better reinforcement effect. Toward that, we prepared four modified CNCs by esterification with mono or binary anhydrides of different lengths of carbon chains. The long hydrocarbon chains were supposed to further improve the interfacial compatibility between CNC and poly(lactic acid) (PLA), and the terminal carboxyl groups should retain the association between nanoparticles. Results from transmittance of visible light for the nanocomposite films revealed homogeneous dispersion and good compatibility between modified nanocrystals and PLA matrix, especially for the long carbon-chain grafting CNCs. With an addition of 4 wt% dodecenyl succinic anhydride-modified CNC, the nanocomposite showed an increase in the tensile strength by ca. 170%. This was ascribed to the improved entanglement of grafting long chains and the potential interaction of terminal carboxyl groups on the CNC surface with the segments of PLA matrix, which enhanced association and compatibility between nanoparticles and matrix. This strategy prepared a biomass alloy of green materials reinforced by natural polymers and promoted the sustainable development of materials with high mechanical properties.

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This research is financially supported by the National Natural Science Foundation of China (51973175 and 51373131), the Project for Chongqing University Innovation Research Group of Chongqing Education Committee (CXQT19008), and the Chongqing Talent Plan for Innovation and Entrepreneurship Demonstration Team (CQYC201903243).

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Correspondence to Lin Gan or Jin Huang.

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Wang, Y., Liao, J., Lu, J. et al. Regulating surface molecular structure of cellulose nanocrystals to optimize mechanical reinforcement effect on hydrophobic bio-based polyesters. Iran Polym J 29, 693–705 (2020).

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  • Poly(lactic acid)
  • Cellulose nanocrystal
  • Surface modification
  • Mechanical reinforcement
  • Filler association