Janus Quasi-Solid Electrolyte Membranes with Asymmetric Porous Structure for High-Performance Lithium-Metal Batteries

Zerui Chen; Wei Zhao; Qian Liu; Yifei Xu; Qinghe Wang; Jinmin Lin; Hao Bin Wu

doi:10.1007/s40820-024-01325-4

Janus Quasi-Solid Electrolyte Membranes with Asymmetric Porous Structure for High-Performance Lithium-Metal Batteries

Nanomicro Lett. 2024 Feb 14;16(1):114. doi: 10.1007/s40820-024-01325-4.

Authors

Zerui Chen¹, Wei Zhao¹, Qian Liu¹, Yifei Xu¹, Qinghe Wang¹, Jinmin Lin¹, Hao Bin Wu²

Affiliations

¹ Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, People's Republic of China.
² Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, People's Republic of China. hbwu@zju.edu.cn.

Abstract

Quasi-solid electrolytes (QSEs) based on nanoporous materials are promising candidates to construct high-performance Li-metal batteries (LMBs). However, simultaneously boosting the ionic conductivity (σ) and lithium-ion transference number (t₊) of liquid electrolyte confined in porous matrix remains challenging. Herein, we report a novel Janus MOFLi/MSLi QSEs with asymmetric porous structure to inherit the benefits of both mesoporous and microporous hosts. This Janus QSE composed of mesoporous silica and microporous MOF exhibits a neat Li⁺ conductivity of 1.5 × 10^-4 S cm^-1 with t₊ of 0.71. A partially de-solvated structure and preference distribution of Li⁺ near the Lewis base O atoms were depicted by MD simulations. Meanwhile, the nanoporous structure enabled efficient ion flux regulation, promoting the homogenous deposition of Li⁺. When incorporated in Li||Cu cells, the MOFLi/MSLi QSEs demonstrated a high Coulombic efficiency of 98.1%, surpassing that of liquid electrolytes (96.3%). Additionally, NCM 622||Li batteries equipped with MOFLi/MSLi QSEs exhibited promising rate performance and could operate stably for over 200 cycles at 1 C. These results highlight the potential of Janus MOFLi/MSLi QSEs as promising candidates for next-generation LMBs.

Keywords: Janus structure; Lithium-metal battery; Mesoporous silicas; Metal–organic frameworks; Quasi-solid electrolytes.