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

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Abstract

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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Acknowledgements

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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Authors and Affiliations

  1. Chongqing Key Laboratory of Soft-Matter Materials Chemistry and Function Manufacturing, School of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, People’s Republic of China

    Yuhuan Wang, Lin Gan & Jin Huang

  2. School of Chemistry, Chemical Engineering and Life Sciences, and School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070, People’s Republic of China

    Jinglu Liao, Zhaoshu Chen, Shanjun Gao & Jin Huang

  3. College of Food Science and Chemical Engineering, Hubei University of Arts and Science, Xiangyang, 441003, People’s Republic of China

    Jun Lu

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  1. Yuhuan Wang
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  2. Jinglu Liao
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Correspondence to Lin Gan or Jin Huang.

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13726_2020_832_MOESM1_ESM.docx

Supplementary file1. Supporting Information. The ratio of reaction materials; DSC and DMA data of Tg, Tm, ΔHm, and crystallinity for PLA and its nanocomposites; the equation about how to calculate the mass mole of hydroxyl groups on CNCs; 13C CP-MAS NMR of the CNC and modified CNCs; XRD patterns of CNC and modified CNCs; DSC spectra of PLA and its nanocomposites (DOCX 7618 kb)

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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). https://doi.org/10.1007/s13726-020-00832-6

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  • DOI: https://doi.org/10.1007/s13726-020-00832-6

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