Fast Isotropic Li-Ion Diffusion in Zeolitic Imidazolate Framework Glass Electrolytes for Batteries电池用沸石咪唑酯框架玻璃电解质中的快速各向同性锂离子扩散

英文 Abstract

All-solid-state lithium batteries require solid electrolytes that combine rapid room-temperature ion transport with mechanical robustness and interfacial compatibility. Zeolitic imidazolate framework (ZIF) glasses, with ZIFs being a sub-set of metal-organic frameworks, offer an attractive yet relatively underexplored platform because they combine an grainboundary-free and amorphous topology with chemically tunable frameworks. Here, we reveal that structural disorder unlocks fast and isotropic lithium diffusion in ZIF glasses. This is realized by using a machine learning interatomic potential to simulate Li+ transport in crystalline and glassy ZIF-4 and ZIF-62. Structural disorder reduces the activation energy for Li+ migration from ~0.35 eV to 0.16 eV and increases the extrapolated room-temperature diffusion coefficient by more than one order of magnitude for ZIF-4 and nearly sevenfold for ZIF-62. Analyses of non-Gaussian dynamics and van Hove correlation functions reveal that Li+ diffusion in crystalline ZIFs occurs via rare, dynamically heterogeneous hopping events among well-defined cages, whereas Li+ diffusion in glassy ZIFs is more homogeneous, continuous, and Fickian-like, benefiting from a wide distribution of coordination geometries and migration barriers. Li+ diffusion in crystalline ZIFs is strongly anisotropic, reflecting that ordered orientations of imidazolate and benzimidazolate rings impose distinct energy barriers along different crystallographic directions. Upon vitrification, these ring orientations become randomized, and hence, the diffusion of Li+ becomes isotropic or near-isotropic. These findings imply that well-designed metal-organic framework glasses are a promising candidate as high-performance solid-state electrolytes.

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中文概述

该内容聚焦规划与仿真，涉及工程化与可信 AI。All-solid-state lithium batteries require solid electrolytes that combine rapid room-temperature ion transport with mechanical robustness and interfacial compatibility. Zeolitic im…… 以上为基于官方材料生成的概述，具体指标和结论请以原始来源为准。

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