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<p>Stereo-complexed poly(lactic acid) (PLA) membranes are highly attractive for sustainable applications, yet achieving a synergy between mechanical strength and superhydrophobicity remains a significant challenge. Herein, a hierarchical crystallization strategy was developed to fabricate high-performance stereo-complexed PLLA/PDLA/ZnO porous composite membranes by integrating methacryloxypropyltrimethoxysilane (MPS)-modified ZnO nanoparticles (NPs). By optimizing the MPS-ZnO content within a 9:1 PLLA/PDLA blending matrix, a remarkable 182% increase in tensile strength (from 2.14 to 6.05&#xa0;MPa) was achieved, while simultaneously attaining stable superhydrophobicity with a water contact angle of 155.4°. Both differential scanning calorimetry (DSC) and X-ray diffraction (XRD) results revealed that MPS-ZnO NPs function as efficient heterogeneous nucleating agents, significantly enhancing stereo-complex (SC) crystallization. Crucially, a “dual-directional traction force” was proposed as a possible mechanism at the molecular level, i.e., the concurrent growth of SC and HC (homo-crystallization) phases induces a confined, oriented crystalline state in the intermediate polymer chains. This unique structure assumption effectively establishes potential correlations in the connection between varying crystalline phases. Furthermore, the composite membranes displayed improved thermal insulation, with thermal conductivity decreasing to 0.055.6&#xa0;W m<sup>−1</sup>&#xa0;K<sup>−1</sup> due to enhanced phonon scattering at the complex hierarchical interfaces. This work provides a versatile approach for designing biodegradable functional membranes with superior structural integrity and tailored surface properties for advanced filtration and insulation.</p> Graphical Abstract <p></p>

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Synergistically robust, superhydrophobic, and stereo-complexed poly(lactic acid)/ZnO porous composite membranes via a hierarchical crystallization strategy

  • 期刊论文

  • 发表日期：

    2026年7月1日

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  • Shengdu Yang,
  • Yuchan Meng,
  • Ding Chen,
  • Xin Sun,
  • Xiaohai Zhao

摘要

Stereo-complexed poly(lactic acid) (PLA) membranes are highly attractive for sustainable applications, yet achieving a synergy between mechanical strength and superhydrophobicity remains a significant challenge. Herein, a hierarchical crystallization strategy was developed to fabricate high-performance stereo-complexed PLLA/PDLA/ZnO porous composite membranes by integrating methacryloxypropyltrimethoxysilane (MPS)-modified ZnO nanoparticles (NPs). By optimizing the MPS-ZnO content within a 9:1 PLLA/PDLA blending matrix, a remarkable 182% increase in tensile strength (from 2.14 to 6.05 MPa) was achieved, while simultaneously attaining stable superhydrophobicity with a water contact angle of 155.4°. Both differential scanning calorimetry (DSC) and X-ray diffraction (XRD) results revealed that MPS-ZnO NPs function as efficient heterogeneous nucleating agents, significantly enhancing stereo-complex (SC) crystallization. Crucially, a “dual-directional traction force” was proposed as a possible mechanism at the molecular level, i.e., the concurrent growth of SC and HC (homo-crystallization) phases induces a confined, oriented crystalline state in the intermediate polymer chains. This unique structure assumption effectively establishes potential correlations in the connection between varying crystalline phases. Furthermore, the composite membranes displayed improved thermal insulation, with thermal conductivity decreasing to 0.055.6 W m−1 K−1 due to enhanced phonon scattering at the complex hierarchical interfaces. This work provides a versatile approach for designing biodegradable functional membranes with superior structural integrity and tailored surface properties for advanced filtration and insulation.

Graphical Abstract