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

Abstract

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.