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<p>Electrocatalytic oxygen reduction reaction in seawater represents a sustainable approach for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production, yet industrial-level current densities trigger severe cathodic alkalization and scaling issues, while aggressive acidification of the reaction system compromises catalytic efficiency. Here we show a cationic modification strategy that dynamically modulates the acidic electrified interface to promote both the formation and desorption of the key *OOH intermediate for H<sub>2</sub>O<sub>2</sub> synthesis. Enabled by this strategy, the cationic-modified catalysts achieve &gt;90% efficiency at 500 mA cm<sup>-2</sup> in natural seawater, and even reach 1.125 A cm<sup>-2</sup> in high-salinity electrolytes, with a competitive estimated cost of $0.64 per kilogram of H<sub>2</sub>O<sub>2</sub>. Ab initio molecular dynamics simulations reveal that the introduced cationic modifications effectively counteract O–O bond cleavage induced by both the inherent strong binding of catalytic sites and the potential-induced over-binding effect under highly negative potentials, and thus facilitate *OOH desorption for H<sub>2</sub>O<sub>2</sub> formation. This work highlights dynamic interfacial intermediate stabilization as a strategy that complements conventional static binding-energy tuning, enabling high-current-density H<sub>2</sub>O<sub>2</sub> electrosynthesis in seawater.</p>

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Cation-tuned acidic electrified interface for hydrogen peroxide electrosynthesis with industrial-level current densities in natural seawater

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月20日

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  • Peike Cao,
  • Xuanchen Liu,
  • Yanming Liu,
  • Zihao Zhao,
  • Shuo Chen,
  • Hongtao Yu,
  • Jingguang G. Chen,
  • Xie Quan

摘要

Electrocatalytic oxygen reduction reaction in seawater represents a sustainable approach for hydrogen peroxide (H2O2) production, yet industrial-level current densities trigger severe cathodic alkalization and scaling issues, while aggressive acidification of the reaction system compromises catalytic efficiency. Here we show a cationic modification strategy that dynamically modulates the acidic electrified interface to promote both the formation and desorption of the key *OOH intermediate for H2O2 synthesis. Enabled by this strategy, the cationic-modified catalysts achieve >90% efficiency at 500 mA cm-2 in natural seawater, and even reach 1.125 A cm-2 in high-salinity electrolytes, with a competitive estimated cost of $0.64 per kilogram of H2O2. Ab initio molecular dynamics simulations reveal that the introduced cationic modifications effectively counteract O–O bond cleavage induced by both the inherent strong binding of catalytic sites and the potential-induced over-binding effect under highly negative potentials, and thus facilitate *OOH desorption for H2O2 formation. This work highlights dynamic interfacial intermediate stabilization as a strategy that complements conventional static binding-energy tuning, enabling high-current-density H2O2 electrosynthesis in seawater.