Interfacial Li⁺ Diffusion Booster Accelerated by Enhanced Metal-Organic Framework Sieving and Wettability for High-Voltage Solid-State Lithium Metal Batteries
Date
2025
Authors
Chen, T.
Zhang, Y.
Wang, S.
Li, J.
Lin, H.
Losic, D.
Chen, S.
Wang, J.
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Journal article
Citation
ChemSusChem, 2025; 18(20):e202501351-e202501351
Statement of Responsibility
Tianhua Chen, Yongzheng Zhang, Simeng Wang, Jin Li, Hongzhen Lin, Dusan Losic, Shimou Chen, and Jian Wang
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Abstract
Solid-state lithium metal batteries (SSLMBs) are promising for realizing higher energy density. However, the poor interfacial Li⁺ transport kinetics and Li dendrite growth inhibit SSLMBs, leading to sluggish interfacial ion diffusion and depressive lifespan, which is attributed to high barriers blocked by anions or interface space in solid-state electrolytes. Herein, a flexible solid-state polymer skeleton employed with ionic liquid and metal-organic frameworks (PIM) electrolyte is proposed to strengthen interfacial Li ion exchange by improving the Li⁺ sieving effect and interfacial wettability. Thanks to the immobilization effect of TFSI⁻ anions affected by positive metal atom centers and pore morphology, the PIM electrolyte exhibits exceptional properties, i.e., a high ionic conductivity up to 3.1 mS cm⁻¹ at 60 °C and an improved Li⁺ transference number of 0.65, enabling symmetric cells of Li metal to run steadily for over 1000 h with lower voltage hysteresis (25 mV). Meanwhile, matching with high-voltage electrodes, the solid-state PIM electrolyte exhibits good compatibility and stability toward LiNi₀.₆Co₀.₂Mn₀.₂O₂ and LiFePO₄ electrodes, showing the capacity retentions of 85.5% and 96.5% after 120 and 400 cycles, respectively. This work suggests low interfacial diffusion resistances and high compatibility for make it a promising candidate for future solid-state battery.
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© 2025 The Author(s). ChemSusChem published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.