Sun, Y.Xia, P.Sheng, P.Wang, ChaoYou, J.Deng, Q.He, QuiangSirés Sadornil, IgnacioYe, Z.2024-11-202024-11-081385-8947https://hdl.handle.net/2445/216632Developing cost-effective and durable cathodes with outstanding oxygen mass transport and selective two-electron oxygen reduction reaction (ORR) is crucial for large-scale H2O2 electrosynthesis. Herein, an oxygen vacancy-rich ZnO-modified air-breathing gas-diffusion electrode (ZnO-V/GDE) was fabricated, thus eliminating the cost of aeration while achieving remarkable O2 utilization efficiency and H2O2 selectivity. This novel cathode led to ultrahigh H2O2 yield of 1005.2 mg L−1 with selectivity of 74.6 %, outperforming both the raw and ZnO-modified air-breathing GDEs. Moreover, the practical applicability of ZnO-V/GDE was demonstrated by its high stability and effectiveness when treating micropollutants in wastewater by ZnO-V/GDE-based electro-Fenton process. Mechanistic insights unveiled the key roles of oxygen vacancies, which not only facilitate the O2 transport by creating a superhydrophobic interface and provide binding centers to O2, but also reduce the energy barrier of the rate-determining step (OOH*-to-H2O2), eventually enhancing the ORR performance.1 p.application/pdfengcc-by-nc-nd (c) Elsevier B.V., 2024http://creativecommons.org/licenses/by-nc-nd/4.0/OxigenAigua oxigenadaElectroquímicaOxygenHydrogen peroxideElectrochemistryinfo:eu-repo/semantics/article7518052024-11-20info:eu-repo/semantics/embargoedAccess