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<p>Composite solid polymer electrolytes (CSPEs) are ideal candidates for metal batteries, offering flexibility, stability, high ionic conductivity, and compatibility with lithium metal. In this work, we developed a dual polymer-based (PVDF-HFP/PEO)/Li<sub>6.25</sub>La<sub>3</sub>Ga<sub>0.25</sub>Zr<sub>2</sub>O<sub>12</sub> (LLGZO) based CSPE using an easily scalable solution casting method. The integration of dual polymer (PEO in PVDF-HFP matrix) and active ceramics (Ga doped LLZO) demonstrates a good Strategy to balance mechanical strength, ionic conductivity, and electrochemical stability for solid-state Lithium metal batteries. This Synergistic design led to a remarkable enhancement in room-temperature ionic conductivity of 1.08 × 10<sup>–4</sup> S·cm<sup>−1</sup>, the lowest activation energy of 0.304&#xa0;eV, a wide electrochemical Stability window of 5.23&#xa0;V vs. Li/Li⁺, and a high transference number (0.74) at 60&#xa0;°C for 10 wt% LLGZO-coated dual-polymer-based CSPE (LZ10). Additionally, it exhibited lower metal/electrolyte interfacial resistance (52.55Ω) and improved tensile Strength of 2.63&#xa0;MPa. As a consequence, LZ10 enabled an excellent plating/stripping Stability for more than 900&#xa0;h at varying current densities at 60&#xa0;°C, with lower changes in bulk and interfacial resistance during long-term cycling. Moreover, the fabricated solid-state cell (Li/LZ10/LiFePO<sub>4</sub>) delivers superior capacity and cycling stability at various current densities at elevated temperatures. Cells also maintained ~ 84% capacity retention after 50 cycles with an excellent coulombic efficiency of &gt; 98%. Thus, the compiled data suggest that the PVDF-HFP/PEO/LLGZO CSPE is a highly promising candidate for developing metal batteries.</p>

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LLZO incorporated dual polymer-based composite electrolyte for enhanced conductivity and long‑term stability for solid‑state lithium‑metal batteries

  • 期刊论文

  • 发表日期：

    2025年9月25日

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  • Kuntal Ghosh,
  • Mononita Das,
  • Mir Wasim Raja

摘要

Composite solid polymer electrolytes (CSPEs) are ideal candidates for metal batteries, offering flexibility, stability, high ionic conductivity, and compatibility with lithium metal. In this work, we developed a dual polymer-based (PVDF-HFP/PEO)/Li6.25La3Ga0.25Zr2O12 (LLGZO) based CSPE using an easily scalable solution casting method. The integration of dual polymer (PEO in PVDF-HFP matrix) and active ceramics (Ga doped LLZO) demonstrates a good Strategy to balance mechanical strength, ionic conductivity, and electrochemical stability for solid-state Lithium metal batteries. This Synergistic design led to a remarkable enhancement in room-temperature ionic conductivity of 1.08 × 10–4 S·cm−1, the lowest activation energy of 0.304 eV, a wide electrochemical Stability window of 5.23 V vs. Li/Li⁺, and a high transference number (0.74) at 60 °C for 10 wt% LLGZO-coated dual-polymer-based CSPE (LZ10). Additionally, it exhibited lower metal/electrolyte interfacial resistance (52.55Ω) and improved tensile Strength of 2.63 MPa. As a consequence, LZ10 enabled an excellent plating/stripping Stability for more than 900 h at varying current densities at 60 °C, with lower changes in bulk and interfacial resistance during long-term cycling. Moreover, the fabricated solid-state cell (Li/LZ10/LiFePO4) delivers superior capacity and cycling stability at various current densities at elevated temperatures. Cells also maintained ~ 84% capacity retention after 50 cycles with an excellent coulombic efficiency of > 98%. Thus, the compiled data suggest that the PVDF-HFP/PEO/LLGZO CSPE is a highly promising candidate for developing metal batteries.