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Superior Ductile and Barrier PLA/PGA Films by In Situ Constructing a Transversely Isotropic Network and Well-Ordered Crystalline Nanolayers
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    Superior Ductile and Barrier PLA/PGA Films by In Situ Constructing a Transversely Isotropic Network and Well-Ordered Crystalline Nanolayers
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    • Bo Liu
      Bo Liu
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
      More by Bo Liu
    • Pengwu Xu
      Pengwu Xu
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
      More by Pengwu Xu
    • Deyu Niu
      Deyu Niu
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
      More by Deyu Niu
    • Gerrit Gobius du Sart
      Gerrit Gobius du Sart
      TotalEnergies Corbion B. V., Arkelsedijk 46, ACGorinchem 4206, The Netherlands
    • Yaoqi Shi
      Yaoqi Shi
      TotalEnergies Corbion B. V. China, Room 3801, Raffles City, No. 268 Middle Xizang Road, Shanghai 200001, China
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    • Kees Joziasse
      Kees Joziasse
      TotalEnergies Corbion B. V., Arkelsedijk 46, ACGorinchem 4206, The Netherlands
    • Yuxiang Zhou
      Yuxiang Zhou
      TotalEnergies Corbion B. V. China, Room 3801, Raffles City, No. 268 Middle Xizang Road, Shanghai 200001, China
      More by Yuxiang Zhou
    • Ye Ma
      Ye Ma
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
      More by Ye Ma
    • Weijun Yang
      Weijun Yang
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
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    • Xu Zhang
      Xu Zhang
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
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    • Tianxi Liu
      Tianxi Liu
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
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    • Piming Ma*
      Piming Ma
      Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, 1800 Lihu Road, Wuxi 214122, China
      *Email: [email protected]
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    Macromolecules

    Cite this: Macromolecules 2025, XXXX, XXX, XXX-XXX
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    https://doi.org/10.1021/acs.macromol.4c02482
    Published January 9, 2025
    Copyright © 2025 American Chemical Society

    Abstract

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    Simultaneously achieving excellent toughness, transparency, and gas barrier properties is still a challenge for poly(lactic acid) (PLA) films. In this work, we address an effective and scalable strategy based on biaxial stretching to make superior ductile, transparent, and high-barrier PLA films by incorporating polyglycolic acid (PGA) and constructing a transversely isotropic structure in the PLA matrix with numerous nanocrystals and a nanolayer PGA barrier phase. The transversely isotropic structure endowed PLA/PGA films with a robust chain entanglement network, which prevents the formation of densely distributed cohesional entanglement and the physical aging of PLA, allowing the molecular chains of PLA to move sufficiently to exhibit excellent toughness. Consequently, the tensile strength of the PLA/PGA film increased from 67 to 157 MPa while maintaining a high elongation at break (>100%), high transparency (>85%), and high durability, demonstrating excellent comprehensive physical and mechanical properties. Importantly, the in situ constructed nanolayer barrier phase greatly prolongs the diffusion path of gas molecules in the PLA/PGA films, and consequently the oxygen permeability coefficient (PO2) of the PLA/PGA film decreased by almost two orders of magnitude, i.e., from 1.66 × 10–14 to 7.10 × 10–16 cm3·cm/cm2·s·Pa, compared to that of neat PLA, and three orders of magnitude lower than that of the polyethylene film. Therefore, this work contributes a deeper understanding of the structure–property relationship of biaxially oriented PLA-based films and may enable their application in the high-barrier green packaging field.

    Copyright © 2025 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.4c02482.

    • Methods of SEM; TEM; DSC; WAXS; FTIR spectroscopy; DMA; oxygen and water vapor permeability; tensile tests; optical properties; DSC curves; mechanical and barrier properties of BO-PLA films with various stretching ratios; DSC curves and SEM images of BO-PLA/PGA films with varying PGA content; the D and S values; strain–stress curves; visible-light transmittance spectra in the range of 400–800 cm–1 for unstretched PLA/PGA sheets (PDF)

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    Macromolecules

    Cite this: Macromolecules 2025, XXXX, XXX, XXX-XXX
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.4c02482
    Published January 9, 2025
    Copyright © 2025 American Chemical Society

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