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<p>The inherent trade-off between mechanical robustness and piezoelectricity in flexible poly(vinylidene fluoride) (PVDF) has long limited its practical applications. This work introduces calcium–polyoxometalate sub-nanowires (Ca–POM SNWs) into the PVDF matrix, overcoming this limitation via molecular entanglement and sub-nanoscale interface locking. Within the PVDF matrix, Ca–POM SNWs form a 3D interpenetrating network, enhancing the elastic modulus by 180% and toughness by 619%. During electrospinning, electric field-induced alignment of Ca–POM SNWs creates a periodic architecture that, together with non-covalent interactions, locks PVDF chains into the piezoelectric β-phase, raising its content from 43.6% to 97.9% and the piezoelectric coefficient (<i>d</i><sub>33</sub>) by 195%. This synergy also yields anisotropic fibrous membranes with high modulus and toughness. The concurrent mechanical and piezoelectric reinforcement by SNWs-mediated molecular entanglement and interface locking represents a breakthrough beyond the capability of conventional nanofillers. Integrated as a sensor array in a smart insole and combined with machine learning, the PVDF/Ca–POM composite achieves 100% accuracy in classifying six different human motion states, showing promise for early detection and dynamic monitoring of diabetic foot ulcers. This study establishes a new approach to high-performance piezoelectric composites through sub-nanometer-level interfacial engineering.</p>

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Molecular Entanglement and Interface Locking by Inorganic Sub-nanowires for Concurrent Mechanical and Piezoelectric Reinforcement in Polymer Composites

  • 期刊论文

  • 发表日期：

    2026年3月4日

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  • Yingshuo Xiong,
  • Xin Liu,
  • Dengke Song,
  • Jiangmei Zhao,
  • Wenlong Xu,
  • Zhen Zhang,
  • Hongdi Zhang,
  • Qun Zhang,
  • Meiwen Cao

摘要

The inherent trade-off between mechanical robustness and piezoelectricity in flexible poly(vinylidene fluoride) (PVDF) has long limited its practical applications. This work introduces calcium–polyoxometalate sub-nanowires (Ca–POM SNWs) into the PVDF matrix, overcoming this limitation via molecular entanglement and sub-nanoscale interface locking. Within the PVDF matrix, Ca–POM SNWs form a 3D interpenetrating network, enhancing the elastic modulus by 180% and toughness by 619%. During electrospinning, electric field-induced alignment of Ca–POM SNWs creates a periodic architecture that, together with non-covalent interactions, locks PVDF chains into the piezoelectric β-phase, raising its content from 43.6% to 97.9% and the piezoelectric coefficient (d33) by 195%. This synergy also yields anisotropic fibrous membranes with high modulus and toughness. The concurrent mechanical and piezoelectric reinforcement by SNWs-mediated molecular entanglement and interface locking represents a breakthrough beyond the capability of conventional nanofillers. Integrated as a sensor array in a smart insole and combined with machine learning, the PVDF/Ca–POM composite achieves 100% accuracy in classifying six different human motion states, showing promise for early detection and dynamic monitoring of diabetic foot ulcers. This study establishes a new approach to high-performance piezoelectric composites through sub-nanometer-level interfacial engineering.