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<p>Electrochemical advanced oxidation that directly activates O<sub>2</sub> through the oxygen reduction reaction (ORR) to generate hydroxyl radicals (•OH) offers a sustainable strategy for degrading persistent organic pollutants. However, prevailing approaches typically rely on a stepwise process involving the 2e⁻ ORR to produce&#xa0;H<sub>2</sub>O<sub>2</sub> followed by 1e⁻ activation. High barriers associated with intermediate desorption and inter-site transfer consequently limit the •OH yield. Here, we construct a single-active-site architecture in the perovskite oxide Pr<sub>1.0</sub>Sr<sub>1.0</sub>Fe<sub>0.5</sub>Zn<sub>0.25</sub>Mo<sub>0.25</sub>O<sub>4-δ</sub> (PSFZM) that enables a direct three-electron ORR pathway for efficient •OH generation. The Zn<sup>δ</sup>⁺ single active center selectively stabilizes *OOH and *H<sub>2</sub>O<sub>2</sub> through weak orbital interactions, while an adjacent Mo atom polarizes the O atoms of adsorbed H<sub>2</sub>O<sub>2</sub>, promoting cleavage of the peroxide bond at the active site. This strategy avoids intermediate desorption and migration, enabling continuous proton-coupled electron transfer. The catalyst achieves a •OH production rate of 821 μmol h⁻<sup>1</sup> and an O<sub>2</sub> utilization of 37.7%, metrics competitive with previously reported systems. In a membrane-free flow cell that uses gaseous O<sub>2</sub> directly, the •OH generation efficiency reaches 64.7%. By combining atomic-level catalyst design with reactor engineering, this work establishes a scalable platform for sustainable wastewater treatment.</p>

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Single-atom-engineered perovskite enables near-theoretical-rate hydroxyl radical electrogeneration

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月24日

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  • Yaobin Wang,
  • Chaoyue Xie,
  • Ruiqing Zhao,
  • Zhiyuan Su,
  • Hongmei Li,
  • Hang Zhang,
  • Bo Li,
  • Changhui Zhou,
  • Yongyang Chen,
  • Zeyu Du,
  • Jinhua Li,
  • Yunfei Bu,
  • Jing Bai,
  • Baoxue Zhou,
  • Emiliano Cortés,
  • Min Liu

摘要

Electrochemical advanced oxidation that directly activates O2 through the oxygen reduction reaction (ORR) to generate hydroxyl radicals (•OH) offers a sustainable strategy for degrading persistent organic pollutants. However, prevailing approaches typically rely on a stepwise process involving the 2e⁻ ORR to produce H2O2 followed by 1e⁻ activation. High barriers associated with intermediate desorption and inter-site transfer consequently limit the •OH yield. Here, we construct a single-active-site architecture in the perovskite oxide Pr1.0Sr1.0Fe0.5Zn0.25Mo0.25O4-δ (PSFZM) that enables a direct three-electron ORR pathway for efficient •OH generation. The Znδ⁺ single active center selectively stabilizes *OOH and *H2O2 through weak orbital interactions, while an adjacent Mo atom polarizes the O atoms of adsorbed H2O2, promoting cleavage of the peroxide bond at the active site. This strategy avoids intermediate desorption and migration, enabling continuous proton-coupled electron transfer. The catalyst achieves a •OH production rate of 821 μmol h⁻1 and an O2 utilization of 37.7%, metrics competitive with previously reported systems. In a membrane-free flow cell that uses gaseous O2 directly, the •OH generation efficiency reaches 64.7%. By combining atomic-level catalyst design with reactor engineering, this work establishes a scalable platform for sustainable wastewater treatment.