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

作     者：Xiang, Yang Yu, Ning Li, Jianbo Xu, Huixiang Chen, Shuang Xia, Yufan Luo, Zhen Li, Xu Liu, Zhu Xu, Maowen Jiang, Yinzhu Zhang, Xuan 

作者机构：School of Materials Science and Engineering State Key Laboratory of Clean Energy Utilization Zhejiang University Hangzhou310027 China ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University Hangzhou311215 China School of Materials and Energy Southwest University Chongqing400715 China 

出 版 物：《Angewandte Chemie - International Edition》 (Angew. Chem. Int. Ed.)

年 卷 期：2025年第64卷第14期

页      面：e202424288页

核心收录：

学科分类：0808[工学-电气工程] 081704[工学-应用化学] 0809[工学-电子科学与技术（可授工学、理学学位）] 0817[工学-化学工程与技术] 08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：This work was supported by the National Key R&D Program (2022YFB2502000)  Hangzhou Joint Fund of the Zhejiang Provincial Natural Science Foundation of China under Grant No.LHZY24B060002  National Key R&D Program (2023YFB2504000). The authors would like to thank Liang Wang from shiyanjia Lab (www.shiyanjia.com) support of Raman analysis 

主　　题：Magic angle spinning 

摘      要：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 7Li 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 83.12 % after 1400 cycles. These findings highlight the potential of structural design in advancing PSE performance, offering a promising pathway for the commercialization of high-performance solid-state batteries. © 2025 Wiley-VCH GmbH.