Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification

作者：Sen Lu, Xuechuan Li, Guan Zhang, Shaobin Wang · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-59722-1 · 被引用次数：56 · 研究领域：Electrocatalysts for Energy Conversion、Electrochemical Analysis and Applications、Electronic and Structural Properties of Oxides

Electro-oxidation is a promising green technology for decentralized wastewater purification. However, its efficacy is primarily constrained by the selectivity and efficiency of hydroxyl radical (•OH) generation through one-electron water oxidation. In this study, we elucidate the mechanism of electronic metal-support interactions (EMSI) of Ni single-atoms on antimony-doped tin oxide anode (Ni/ATO) to enhance •OH production and overall water treatment efficiency. We experimentally and theoretically investigate both the structural evolution process and micro-interface mechanisms associated with the EMSI effects induced by Ni single-atoms. The optimized electronic structures in the interfacial catalysts under EMSI conditions and the co-catalytic role of Ni single-atoms synergistically facilitate selective and efficient •OH generation, resulting in over a fivefold increase in its steady-state concentration and tenfold enhancement in pseudo-first-order rate constant of sulfamethoxazole degradation compared to those on bare ATO. With the EMSI, rapid electron transfer channels were established for a marked enhancement in the adsorption, conversion, and dissociation of interfacial H2O molecules. Notably, it is revealed that Ni single-atoms serve as co-catalytic sites, exhibiting a “H-pulling effect” that is crucial for •OH generation. The Ni/ATO anode demonstrates great efficiency in degrading various refractory organic pollutants, and effectively treats real pharmaceutical wastewate...