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<p>Electrochemical seawater electrolysis powered by renewable energy is a highly promising route toward sustainable hydrogen production, mitigating both energy shortages and carbon emissions. However, chloride-induced corrosion and competitive chlorine evolution reactions lead to metal site dissolution, severely impairing durability, especially at industrial-level current densities. Here, we report a nitrite-incorporated cobalt-iron layered double hydroxide (CoFe-NO<sub>2</sub><sup>−</sup>-LDH) electrocatalyst that exhibits exceptional activity and stability for seawater splitting. The nitrite anion acts as an electronic pump: it accepts electrons to facilitate the formation of high-valence Fe species essential for initial OER activation, and donates electrons under high potential to suppress oxidative dissolution. Moreover, the negatively charged nitrite generates an electrostatic repulsion field that effectively repels chloride ions, protecting metal active sites from corrosion and segregation. The <i>in situ</i> characterization confirms that nitrite doping weakens the Fe–O covalency, which suppresses lattice oxygen participation and promotes a stable adsorbate-evolving mechanism, consequently leading to significantly enhanced operational stability. When used as an anode, the CoFe-NO<sub>2</sub><sup>−</sup>-LDH catalyst achieves over 1000 h of stable operation at 1000 mA cm<sup>−2</sup> in seawater electrolysis, demonstrating great potential for practical applications.</p>

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Oxygen anion-mediated electron pump suppressed iron segregation in cobalt-iron catalyst boosts ampere-scale seawater electrolysis

  • 期刊论文

  • 发表日期：

    2026年3月20日

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  • Yiwen Chen,
  • Xiaoyan Zhong,
  • Mingxing Zhu,
  • Xiaoxia Chen,
  • Hui Su

摘要

Electrochemical seawater electrolysis powered by renewable energy is a highly promising route toward sustainable hydrogen production, mitigating both energy shortages and carbon emissions. However, chloride-induced corrosion and competitive chlorine evolution reactions lead to metal site dissolution, severely impairing durability, especially at industrial-level current densities. Here, we report a nitrite-incorporated cobalt-iron layered double hydroxide (CoFe-NO2−-LDH) electrocatalyst that exhibits exceptional activity and stability for seawater splitting. The nitrite anion acts as an electronic pump: it accepts electrons to facilitate the formation of high-valence Fe species essential for initial OER activation, and donates electrons under high potential to suppress oxidative dissolution. Moreover, the negatively charged nitrite generates an electrostatic repulsion field that effectively repels chloride ions, protecting metal active sites from corrosion and segregation. The in situ characterization confirms that nitrite doping weakens the Fe–O covalency, which suppresses lattice oxygen participation and promotes a stable adsorbate-evolving mechanism, consequently leading to significantly enhanced operational stability. When used as an anode, the CoFe-NO2−-LDH catalyst achieves over 1000 h of stable operation at 1000 mA cm−2 in seawater electrolysis, demonstrating great potential for practical applications.