Xu Yifan, Chen Zhiyu, Wang Jiaqi, Li Bai, Li Jiangnan, He Zijian, Li Lei, Gao Lei, Han Songbai, Bian Juncao, Zhu Jinlong, Wang Liping, Zhao Yusheng, Xu Qiang, Zhao Ruo
Institute for Advanced Study, Shenzhen University, Shenzhen, 518055, China.
Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Academy for Advanced Interdisciplinary Studies, Southern University of Science and Technology, Shenzhen, 518055, China.
Angew Chem Int Ed Engl. 2025 Jan 21;64(4):e202416170. doi: 10.1002/anie.202416170. Epub 2024 Oct 30.
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, 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.
固态聚合物电解质（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）作为固体填料显示出有望改善SPEs的性能。然而，含OMS的MOFs数量相当有限，占MOFs总数的不到5%。考虑到产率、成本和可加工性，常用的含OMS的MOFs不超过10种，存在很大局限性。在此，我们报道了一种简单通用的方法，将无OMS的MOFs转化为富含OMS的准MOFs以开发高性能SPEs，并探索了其潜在机制。详细研究了“OMS-聚合物”和“OMS-离子”相互作用，以阐明准MOFs对电池性能的作用。发现准MOFs作为离子筛，能有效调节离子迁移，从而促进锂的均匀沉积并形成超稳定界面。结果，锂对称电池在0.3 mA cm下稳定运行超过3000小时，而全电池在1.0 C下循环1500次后仍保留其初始容量的85%。最后，使用其他MOFs进行了通用测试，证实了我们设计概念的通用性和有效性。
