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<p>Achieving a reversible four-electron-per-oxygen-molecule oxygen evolution reaction is an essential yet highly challenging task for nonaqueous lithium hydroxide-based Li | |O<sub>2</sub> batteries, as the kinetically sluggish oxygen evolution reaction tends to entangle with competing parasitic reactions, whose origins and mitigating strategies remain largely elusive. Here we construct a highly reversible lithium hydroxide-based Li | |O<sub>2</sub> battery using iron–cobalt–nickel layered double hydroxide catalysts and tetramethylene sulfone-based electrolytes. Lithium hydroxide decomposition toward oxygen evolution involves key reactive oxygen species of surface-bound hydroxyl and hydroxyl radicals, but no singlet oxygen. These hydroxyl species corrode the electrolyte and carbon support, predominantly accounting for charging irreversibility. While oxidation-resistant solvents and electrical conductors are necessary to reduce hydroxyl-induced side reactions, the synergistic interplay of interfacial water solvation and catalytic surface structures hold the key to steering hydroxyl activity toward the desirable oxygen evolution reaction or by-product formation. This work offers insights into achieving long-life lithium hydroxide-based Li | |O<sub>2</sub> batteries.</p>

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Unravelling the key factors governing O2 evolution upon charging a reversible LiOH-based nonaqueous Li | |O2 battery

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年7月9日

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  • Linbin Tang,
  • Zechun Lu,
  • Zongyan Gao,
  • Xuechun Lou,
  • Junjian Li,
  • Yujie Wen,
  • Junchao Chen,
  • Zhexuan Zhu,
  • Shijing Luo,
  • Lina Zhou,
  • Guangfeng Wei,
  • Zuofeng Chen,
  • Hongying Zhao,
  • Tong Li,
  • Luming Peng,
  • Fengting Li,
  • Tao Liu

摘要

Achieving a reversible four-electron-per-oxygen-molecule oxygen evolution reaction is an essential yet highly challenging task for nonaqueous lithium hydroxide-based Li | |O2 batteries, as the kinetically sluggish oxygen evolution reaction tends to entangle with competing parasitic reactions, whose origins and mitigating strategies remain largely elusive. Here we construct a highly reversible lithium hydroxide-based Li | |O2 battery using iron–cobalt–nickel layered double hydroxide catalysts and tetramethylene sulfone-based electrolytes. Lithium hydroxide decomposition toward oxygen evolution involves key reactive oxygen species of surface-bound hydroxyl and hydroxyl radicals, but no singlet oxygen. These hydroxyl species corrode the electrolyte and carbon support, predominantly accounting for charging irreversibility. While oxidation-resistant solvents and electrical conductors are necessary to reduce hydroxyl-induced side reactions, the synergistic interplay of interfacial water solvation and catalytic surface structures hold the key to steering hydroxyl activity toward the desirable oxygen evolution reaction or by-product formation. This work offers insights into achieving long-life lithium hydroxide-based Li | |O2 batteries.