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Vol. 17 (2025)

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

https://doi.org/10.1007/s40820-025-01760-x
Xiong Xiong Liu
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Long Pan
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Haotian Zhang
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Cancan Liu
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Mufan Cao
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Min Gao
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Yuan Zhang
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Zeyuan Xu
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
Yaping Wang
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China
ZhengMing Sun
School of Materials Science and Engineering, Southeast University, Nanjing 211189, People’s Republic of China

Corresponding Author: ZhengMing Sun

zmsun@seu.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 249

Abstract

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.


Highlights:
1 Indium-based metal–organic framework (In-MOF) is proposed as a multifunctional promoter to create poly(vinylidene fluoride–hexafluoropropylene) (PVH)/In-MOF (PVH-IM) composite solid polymer electrolyte, synchronously achieving a high ionic conductivity of 1.23 × 10−3 S cm−1 and excellent electrochemical stability against Li anodes.
2 In-MOF not only can adsorb and convert free residual solvents into bonded states to prevent their side reactions with Li anodes, but also induce inorganic-rich solid electrolyte interphase layers to prevent PVH from reacting with lithium anodes and promote uniform lithium deposition without dendrite growths.
3 The Li|PVH-IM|Li symmetric cells maintain stable cycling for 5550 h at the current density of 0.2 mA cm−2. In addition, all-solid-state LFP|PVH-IM|Li full cells deliver a significant capacity retention of 80.0% at a rate of 0.5C after 280 cycles at 25 °C.

Keywords

Fluoropolymer Solid polymer electrolyte Electrochemical stability In-MOF Solid electrolyte interphase All-solid-state lithium metal battery
Liu, Xiong Xiong, Long Pan, Haotian Zhang, Cancan Liu, Mufan Cao, Min Gao, Yuan Zhang, Zeyuan Xu, Yaping Wang, and ZhengMing Sun. 2025. “Indium-MOF As Multifunctional Promoter to Remove Ionic Conductivity and Electrochemical Stability Constraints on Fluoropolymer Electrolytes for All-Solid-State Lithium Metal Battery”. Nano-Micro Letters 17 (May):249. https://doi.org/10.1007/s40820-025-01760-x.
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