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<p>Fluoropolymers promise all-solid-state lithium metal batteries (ASLMBs) but suffer from two critical challenges. The first is the trade-off between ionic conductivity (<i>σ</i>) and lithium anode reactions, closely related to high-content residual solvents. The second, usually consciously overlooked, is the fluoropolymer’s inherent instability against alkaline lithium anodes. Here, we propose indium-based metal–organic frameworks (In-MOFs) as a multifunctional promoter to simultaneously address these two challenges, using poly(vinylidene fluoride–hexafluoropropylene) (PVH) as the typical fluoropolymer. In-MOF plays a trio: (1) adsorbing and converting free residual solvents into bonded states to prevent their side reactions with lithium anodes while retaining their advantages on Li<sup>+</sup> transport; (2) forming inorganic-rich solid electrolyte interphase layers to prevent PVH from reacting with lithium anodes and promote uniform lithium deposition without dendrite growth; (3) reducing PVH crystallinity and promoting Li-salt dissociation. Therefore, the resulting PVH/In-MOF (PVH-IM) showcases excellent electrochemical stability against lithium anodes, delivering a 5550&#xa0;h cycling at 0.2&#xa0;mA&#xa0;cm<sup>−2</sup> with a remarkable cumulative lithium deposition capacity of 1110 mAh cm<sup>−2</sup>. It also exhibits an ultrahigh <i>σ</i> of 1.23 × 10<sup>−3</sup> S cm<sup>−1</sup> at 25&#xa0;°C. Moreover, all-solid-state LiFePO<sub>4</sub>|PVH-IM|Li full cells show outstanding rate capability and cyclability (80.0% capacity retention after 280 cycles at 0.5C), demonstrating high potential for practical ASLMBs.</p>

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Indium-MOF as Multifunctional Promoter to Remove Ionic Conductivity and Electrochemical Stability Constraints on Fluoropolymer Electrolytes for All-Solid-State Lithium Metal Battery

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月7日

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  • Xiong Xiong Liu,
  • Long Pan,
  • Haotian Zhang,
  • Cancan Liu,
  • Mufan Cao,
  • Min Gao,
  • Yuan Zhang,
  • Zeyuan Xu,
  • Yaping Wang,
  • ZhengMing Sun

摘要

Fluoropolymers promise all-solid-state lithium metal batteries (ASLMBs) but suffer from two critical challenges. The first is the trade-off between ionic conductivity (σ) and lithium anode reactions, closely related to high-content residual solvents. The second, usually consciously overlooked, is the fluoropolymer’s inherent instability against alkaline lithium anodes. Here, we propose indium-based metal–organic frameworks (In-MOFs) as a multifunctional promoter to simultaneously address these two challenges, using poly(vinylidene fluoride–hexafluoropropylene) (PVH) as the typical fluoropolymer. In-MOF plays a trio: (1) adsorbing and converting free residual solvents into bonded states to prevent their side reactions with lithium anodes while retaining their advantages on Li+ transport; (2) forming inorganic-rich solid electrolyte interphase layers to prevent PVH from reacting with lithium anodes and promote uniform lithium deposition without dendrite growth; (3) reducing PVH crystallinity and promoting Li-salt dissociation. Therefore, the resulting PVH/In-MOF (PVH-IM) showcases excellent electrochemical stability against lithium anodes, delivering a 5550 h cycling at 0.2 mA cm−2 with a remarkable cumulative lithium deposition capacity of 1110 mAh cm−2. It also exhibits an ultrahigh σ of 1.23 × 10−3 S cm−1 at 25 °C. Moreover, all-solid-state LiFePO4|PVH-IM|Li full cells show outstanding rate capability and cyclability (80.0% capacity retention after 280 cycles at 0.5C), demonstrating high potential for practical ASLMBs.