Nature Communications (Mar 2024)

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,
  • Xiaodi Ren

DOI
https://doi.org/10.1038/s41467-024-46186-y
Journal volume & issue
Vol. 15, no. 1
pp. 1 – 12

Abstract

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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.