Issue

Vol. 16 (2024)

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

https://doi.org/10.1007/s40820-024-01325-4
Zerui Chen
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
Wei Zhao
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
Qian Liu
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
Yifei Xu
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
Qinghe Wang
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
Jinmin Lin
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
Hao Bin Wu
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

Corresponding Author: Hao Bin Wu

hbwu@zju.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 114

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.


Highlights:
1 Janus quasi-solid electrolyte membranes with asymmetric porous structure were constructed, showing a high σLi+ of 1.5 × 10-4 S cm-1 and a high t+ of 0.71.
2 The solvation structures and ion transport dynamics in nanopores have been deciphered, manifesting a concentrated electrolyte-like structure and regulated transport behaviors.
3 Quasi-solid NCM 622||Li cells have been demonstrated to stably cycle for 200 cycles at 1 C, and pouch cell has shown high tolerance for abuse.

Keywords

Metal–organic frameworks Mesoporous silicas Quasi-solid electrolytes Janus structure Lithium-metal battery
Chen, Zerui, Wei Zhao, Qian Liu, Yifei Xu, Qinghe Wang, Jinmin Lin, and Hao Bin Wu. 2024. “Janus Quasi-Solid Electrolyte Membranes With Asymmetric Porous Structure for High-Performance Lithium-Metal Batteries”. Nano-Micro Letters 16 (February):114. https://doi.org/10.1007/s40820-024-01325-4.
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