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<p>Proton exchange membrane water electrolysis (PEMWE) is a key technology for green hydrogen production, but its widespread deployment is severely constrained by the sluggish kinetics of the anodic oxygen evolution reaction (OER) and the high iridium loading required to achieve practical performance. Herein, we report an interfacial electronic modulation strategy that simultaneously enhance the activity and durability of IrO<sub>2</sub> catalysts by engineering oxygen-deficient tungsten oxide (WO<sub>3−x</sub>) supports. The deliberate generation of abundant oxygen-coordinatively unsaturated tungsten (W<sub>OCU</sub>) sites enables strong electronic coupling at the IrO<sub>2</sub>/WO<sub>3−x</sub> interface, leading to the formation of well-defined Ir-O-W<sub>OCU</sub> motifs. Comprehensive structural and spectroscopic analyses reveal that these motifs drive pronounced electron redistribution from the WO<sub>3−x</sub> support to Ir centers, resulting in a downshift of the Ir d-band center and stabilization of catalytically active Ir<sup>3+</sup> species. Consequently, the IrO<sub>2</sub>@WO<sub>3−x</sub> catalyst exhibits a low overpotential of 324 mV at 10&#xa0;mA cm<sup>− 2</sup> and a high mass activity of 163.3&#xa0;A g<sup>−1</sup><sub>Ir</sub>. More importantly, Ir dissolution is significantly suppressed, endowing the catalyst with enhanced structural stability during prolonged operation. In a practical PEMWE single-cell, the IrO<sub>2</sub>@WO<sub>3−x</sub> anode achieves a low cell voltage of 1.667&#xa0;V at 1&#xa0;A cm<sup>− 2</sup> and stable operation for over 200&#xa0;h with a low iridium loading of 0.2&#xa0;mg cm<sup>− 2</sup>. This work highlights the critical role of oxygen‑coordinatively unsaturated sites in governing interfacial electronic structure and catalytic behavior, and provides a rational design strategy for cost‑effective and durable electrocatalysts for acidic water oxidation.</p> Graphical Abstract <p></p>

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Modulating Interfacial Electron Redistribution via Oxygen-Coordinatively Unsaturated Tungsten Sites for High-Performance Acidic Water Oxidation

  • 期刊论文

  • 发表日期：

    2026年7月18日

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  • Qiang Liu,
  • Fen Yi,
  • Guochun Li,
  • Xuhan Cao,
  • Lili Huang,
  • Liang Li

摘要

Proton exchange membrane water electrolysis (PEMWE) is a key technology for green hydrogen production, but its widespread deployment is severely constrained by the sluggish kinetics of the anodic oxygen evolution reaction (OER) and the high iridium loading required to achieve practical performance. Herein, we report an interfacial electronic modulation strategy that simultaneously enhance the activity and durability of IrO2 catalysts by engineering oxygen-deficient tungsten oxide (WO3−x) supports. The deliberate generation of abundant oxygen-coordinatively unsaturated tungsten (WOCU) sites enables strong electronic coupling at the IrO2/WO3−x interface, leading to the formation of well-defined Ir-O-WOCU motifs. Comprehensive structural and spectroscopic analyses reveal that these motifs drive pronounced electron redistribution from the WO3−x support to Ir centers, resulting in a downshift of the Ir d-band center and stabilization of catalytically active Ir3+ species. Consequently, the IrO2@WO3−x catalyst exhibits a low overpotential of 324 mV at 10 mA cm− 2 and a high mass activity of 163.3 A g−1Ir. More importantly, Ir dissolution is significantly suppressed, endowing the catalyst with enhanced structural stability during prolonged operation. In a practical PEMWE single-cell, the IrO2@WO3−x anode achieves a low cell voltage of 1.667 V at 1 A cm− 2 and stable operation for over 200 h with a low iridium loading of 0.2 mg cm− 2. This work highlights the critical role of oxygen‑coordinatively unsaturated sites in governing interfacial electronic structure and catalytic behavior, and provides a rational design strategy for cost‑effective and durable electrocatalysts for acidic water oxidation.

Graphical Abstract