<p>Conventional lithium-ion batteries face serious safety challenges including leakage risks, interfacial side reactions, and lithium dendrite growth in liquid electrolytes, while existing solid-state electrolytes still exhibit insufficient capability to suppress dendrites. To address these issues, this study innovatively develops a novel gel polymer electrolyte (L-PEM) based on a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix and low-cost, easily processable micro-sized Li<sub>2</sub>ZrO<sub>3</sub> (LZO) fillers. Microsized LZO offers significant cost and processing advantages over nanomaterials. The direct blending of LZO with commercial PVDF-HFP polymer yields a uniform composite electrolyte through a simple, scalable fabrication process, substantially lowering manufacturing costs. This structure not only provides the electrolyte with excellent mechanical flexibility (remaining intact after bending and puncture tests) but also simultaneously delivers high ionic conductivity (9.01 × 10<sup>−4</sup>&#xa0;S&#xa0;cm<sup>−1</sup> at 30&#xa0;°C) and a high lithium-ion transference number (0.66). This design effectively regulates lithium-ion flux and promotes uniform deposition, thereby fundamentally inhibiting dendrite growth. The assembled cell demonstrates exceptional cycling stability, retaining a high capacity retention of 98.63% after 500 cycles at 0.5&#xa0;C. This work systematically demonstrates the feasibility and mechanism of using low-cost micro-fillers to synergistically enhance the flame retardancy, mechanical strength, and electrochemical performance of electrolytes, providing a new technical pathway and theoretical basis for developing safe, low-cost, and high-performance solid-state batteries.</p>

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Preparation of LZO-doped PVDF-HFP solid polymer electrolyte membranes and their performance in dendrite-free lithium metal batteries

  • Yunchao Nan,
  • Qixin Gai,
  • Hongtao Gao

摘要

Conventional lithium-ion batteries face serious safety challenges including leakage risks, interfacial side reactions, and lithium dendrite growth in liquid electrolytes, while existing solid-state electrolytes still exhibit insufficient capability to suppress dendrites. To address these issues, this study innovatively develops a novel gel polymer electrolyte (L-PEM) based on a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix and low-cost, easily processable micro-sized Li2ZrO3 (LZO) fillers. Microsized LZO offers significant cost and processing advantages over nanomaterials. The direct blending of LZO with commercial PVDF-HFP polymer yields a uniform composite electrolyte through a simple, scalable fabrication process, substantially lowering manufacturing costs. This structure not only provides the electrolyte with excellent mechanical flexibility (remaining intact after bending and puncture tests) but also simultaneously delivers high ionic conductivity (9.01 × 10−4 S cm−1 at 30 °C) and a high lithium-ion transference number (0.66). This design effectively regulates lithium-ion flux and promotes uniform deposition, thereby fundamentally inhibiting dendrite growth. The assembled cell demonstrates exceptional cycling stability, retaining a high capacity retention of 98.63% after 500 cycles at 0.5 C. This work systematically demonstrates the feasibility and mechanism of using low-cost micro-fillers to synergistically enhance the flame retardancy, mechanical strength, and electrochemical performance of electrolytes, providing a new technical pathway and theoretical basis for developing safe, low-cost, and high-performance solid-state batteries.