Superior electrochemical performance of alkali metal anodes enabled by milder Lewis acidity

Linlin Wang; Jiacheng Zhu; Nan Li; Zhe Zhang; Shiwan Zhang; Yifan Chen; Jianwen Zhang; Yusi Yang; Lulu Tan; Xiaogang Niu; Xuefeng Wang; Xiao Ji; Yujie Zhu

doi:10.1039/D4EE00900B

Superior electrochemical performance of alkali metal anodes enabled by milder Lewis acidity†

Linlin Wang,

‡^a Jiacheng Zhu,‡^b Nan Li,^a Zhe Zhang,^a Shiwan Zhang,^a Yifan Chen,^a Jianwen Zhang,^a Yusi Yang,^a Lulu Tan,^a Xiaogang Niu,^a Xuefeng Wang,

*^b Xiao Ji*^c and Yujie Zhu

*^ad

Author affiliations

* Corresponding authors

^a School of Chemistry, Beihang University, Beijing 100191, China
E-mail: yujiezhu@buaa.edu.cn

^b Institute of Physics, College of Materials Science and Opto-Electronic Technology, Chinese Academy of Sciences, University of Chinese Academy of Sciences, Beijing 100191, China

^c School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China

^d Beijing Advanced Innovation Center for Biomedical Engineering, Beihang University, Beijing 100191, China

Abstract

In the development of electrolytes for high-performance alkali metal batteries, significantly different electrochemical performances were often reported among lithium (Li), sodium (Na), and potassium (K) metals tested in the electrolytes with similar compositions but the underlying mechanism behind these observed discrepancies remains unclear. Here, by adopting a suite of complementary analytical techniques aided with theoretical calculations, we show a close correlation between the Lewis acidity of alkali metal ions and the electrochemical performance of corresponding alkali metals. The lower Lewis acidity of K compared with that of Li and Na endows K with distinctive advantages to easily strip off the reduction-vulnerable solvent and greatly reduces the dissociation degree of K salts to form an anion-rich solvation sheath, resulting in a robust solid electrolyte interphase. These features lead K metal to outperform Li and Na metals in terms of both electrochemical cycling reversibility and calendar aging stability in the present study.

Energy & Environmental Science

Superior electrochemical performance of alkali metal anodes enabled by milder Lewis acidity†

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