High-Efficiency Lithium-Ion Transport in a Porous Coordination Chain-Based Hydrogen-Bonded Framework

• Published in: Journal of the American Chemical Society 2023-05, Vol.145 (18), p.10149-10158
• Main Authors: Han, Zongsu, Zhang, Runhao, Jiang, Jialong, Chen, Zhonghang, Ni, Youxuan, Xie, Weiwei, Xu, Jun, Zhou, Zhen, Chen, Jun, Cheng, Peng, Shi, Wei
• Format: Article
• Language: English
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.3c00647

Fast and selective Li+ transport in solid plays a key role for the development of high-performance solid-state electrolytes (SSEs) of lithium metal batteries. Porous compounds with tunable Li+ transport pathways are promising SSEs, but the comprehensive performances in terms of Li+ transport kinetics, electrochemical stability window, and interfacial compatibility are difficult to be achieved simultaneously. Herein, we report a porous coordination chain-based hydrogen-bonded framework (NKU-1000) containing arrayed electronegative sites for Li+ transport, exhibiting a superior Li+ conductivity of 1.13 × 10–3 S cm–1, a high Li+ transfer number of 0.87, and a wide electrochemical window of 5.0 V. The assembled solid-state battery with NKU-1000-based SSE shows a high discharge capacity with 94.4% retention after 500 cycles and can work over a wide temperature range without formation of lithium dendrites, which derives from the linear hopping sites that promote a uniformly high-rate Li+ flux and the flexible structure that can buffer the structural variation during Li+ transport.