Carving Metal–Organic–Framework Glass Based Solid–State Electrolyte Via a Top–Down Strategy for Lithium–Metal Battery

作者：Yang Xiang, Ning Yu, Jian-Bo Li, Huixiang Xu, Shuang Chen, Yufan Xia, Zhen Luo, Li Xu, Zhu Liu, Maowen Xu, Maowen Xu, Yinzhu Jiang, Yinzhu Jiang, Xuan Zhang · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202424288 · 被引用次数：19 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Supercapacitor Materials and Fabrication

Abstract Traditional polymer solid electrolytes (PSEs) suffer from low ions conductivity, poor kinetics and safety concerns. Here, we present a novel porous MOF glass gelled polymer electrolyte (PMG‐GPE) prepared via a top‐down strategy, which features a unique three‐dimensional interconnected graded‐aperture structure for efficient ions transport. Comprehensive analyses, including time‐of‐flight secondary ion mass spectrometry (TOF‐SIMS), Solid‐state 7 Li magic‐angle‐spinning nuclear magnetic resonance (MAS NMR), Molecular Dynamics (MD) simulations, and electrochemical tests, quantify the pore structures, revealing their relationship with ions conductivity that increases and then decreases as macropore proportion rises. The introduced dispersed macropores (17 % fraction) can serve as bridges, connecting adjacent transport units to accelerate ions transport. Taking advantage of the cross‐linked ion‐conductive paths constructed by hierarchical pore structures, the PMG‐GPE achieves a high ions conductivity of 1.9 mS cm −1 . Additionally, the robust mechanical properties of PMG‐GPE effectively suppress dendrite growth and penetration, outperforming crystal MOF‐based electrolytes. The prepared Li symmetric batteries with PMG‐GPE demonstrate a high critical current density of 5.1 mA cm −2 (two times higher than crystal MOF‐electrolytes) and stable cycling for over 6000 hours without short circuits. Furthermore, a Li/PMG‐GPE/LFP half‐cell exhibits exceptional capacity retention of ...