南方科技大学赵若团队报道了固体聚合物电解质准金属-有机框架设计，实现与锂金属阳极的超稳定界面。相关研究成果于2024年9月5日发表在《德国应用化学》。

固体聚合物电解质（SPEs）在锂金属电池的发展中至关重要。最近，具有开放金属位点（OMSs）的金属有机框架（MOFs）作为固体填料有望提高SPEs的性能。然而，含有MOFs的OMSs数量非常有限，不到MOFs总数的5%。在考虑产量、成本和加工性时，常用的含MOFs的OMSs不超过10种，造成了很大的局限性。

该文中，研究人员报告了一种简单通用的方法，将无OMS的MOFs转换为富含OMS的准MOFs，用于开发高性能SPEs，并探索了其潜在机制。详细研究了“OMS聚合物”和“OMS离子”的相互作用，以阐明准MOFs对电池性能的作用。

研究发现，作为离子筛的准MOFs可以有效地调节离子迁移，从而促进均匀的Li沉积并实现超稳定的界面。因此，Li对称电池在0.3 mA cm^-2下稳定运行了3000多个小时，而全电池在1.0 C下循环1500次后仍保持了85%的初始容量。最后，使用其他MOFs进行了通用测试，证实了该设计概念的普遍性和有效性。

附：英文原文

Title: Design of Quasi-Metal-Organic Frameworks for Solid Polymer Electrolytes Enabling an Ultra-Stable Interface with Li Metal Anode

Author: Yifan Xu, Zhiyu Chen, Jiaqi Wang, Bai Li, Jiangnan Li, Zijian He, Lei Li, Lei Gao, Songbai Han, Juncao Bian, Jinlong Zhu, Liping Wang, Yusheng Zhao, Qiang Xu, Ruo Zhao

Issue&Volume: 2024-09-05

Abstract: Solid polymer electrolytes (SPEs) are crucial in the development of lithium metal batteries. Recently, metal-organic frameworks (MOFs) with open metal sites (OMSs) have shown promise as solid fillers to improve the performance of SPEs. However, the number of OMS-containing MOFs is quite limited, comprising less than 5% of the total MOFs. When considering yield, cost, and processability, the commonly used OMS-containing MOFs are no more than 10 types, causing great limitations. Herein, we reported a simple and universal methodology that converted OMS-free MOFs to OMS-rich quasi-MOFs for developing high-performance SPEs, and explored the underlying mechanism. The “OMS-polymer” and “OMS-ion” interactions were investigated in detail to elucidate the role of quasi-MOFs on battery performance. It was found that quasi-MOFs, functioning as ion sieves, can effectively regulate ion migration, thus promoting uniform Li deposition and enabling an ultra-stable interface. As a result, the Li symmetric cell stably ran over 3000 h at 0.3 mA cm-2, while the full cell retained 85% of its initial capacity after 1500 cycles at 1.0 C. Finally, universal testing was performed using other MOFs, confirming the generalizability and effectiveness of our design concept.

DOI: 10.1002/anie.202416170

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202416170