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

Zongsu Han; Runhao Zhang; Jialong Jiang; Zhonghang Chen; Youxuan Ni; Weiwei Xie; Jun Xu; Zhen Zhou; Jun Chen; Peng Cheng; Wei Shi

doi:10.1021/jacs.3c00647

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

J Am Chem Soc. 2023 May 10;145(18):10149-10158. doi: 10.1021/jacs.3c00647. Epub 2023 Apr 25.

Authors

Zongsu Han¹, Runhao Zhang¹, Jialong Jiang¹, Zhonghang Chen¹, Youxuan Ni^{1

2}, Weiwei Xie^{1

2}, Jun Xu³, Zhen Zhou⁴, Jun Chen^{1

2}, Peng Cheng^{1

2}, Wei Shi¹

Affiliations

¹ Department of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (MOE) and Frontiers Science Center for New Organic Matter, College of Chemistry, Nankai University, Tianjin 300071, China.
² Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China.
³ School of Materials Science and Engineering & National Institute for Advanced Materials, Center for Rare Earth and Inorganic Functional Materials, Tianjin Key Laboratory for Rare Earth Materials and Applications, Nankai University, Tianjin 300350, China.
⁴ School of Materials Science and Engineering, Institute of New Energy Material Chemistry, Nankai University, Tianjin 300350, China.

PMID: 37120859
DOI: 10.1021/jacs.3c00647

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.