Molecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries

Zhuangzhuang Cui, Zhuangzhuang Jia, Digen Ruan, Qingshun Nian, Jiajia Fan, Shunqiang Chen, Zixu He, Dazhuang Wang, Jinyu Jiang, Jun Ma, Xing Ou, Shuhong Jiao, Qingsong Wang () and Xiaodi Ren ()
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Zhuangzhuang Cui: University of Science and Technology of China
Zhuangzhuang Jia: University of Science and Technology of China
Digen Ruan: University of Science and Technology of China
Qingshun Nian: University of Science and Technology of China
Jiajia Fan: University of Science and Technology of China
Shunqiang Chen: University of Science and Technology of China
Zixu He: University of Science and Technology of China
Dazhuang Wang: University of Science and Technology of China
Jinyu Jiang: University of Science and Technology of China
Jun Ma: University of Science and Technology of China
Xing Ou: Central South University
Shuhong Jiao: University of Science and Technology of China
Qingsong Wang: University of Science and Technology of China
Xiaodi Ren: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Constraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially for ether solvents with high Li metal compatibility but low oxidation stability ( 4.4 V) and extensive exothermic reactions between Li metal and reactive anions. Herein, we propose a molecular anchoring approach to restrict the interfacial reactivity of free ether solvents in diluted electrolytes. The hydrogen-bonding interactions from the anchoring solvent effectively suppress excessive ether side reactions and enhances the stability of nickel rich cathodes at 4.7 V, despite the extremely low Li+/ether molar ratio (1:9) and the absence of typical anion-derived interphase. Furthermore, the exothermic processes under thermal abuse conditions are mitigated due to the reduced reactivity of anions, which effectively postpones the battery thermal runaway.

Date: 2024
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DOI: 10.1038/s41467-024-46186-y

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