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Cobalt oxides, as ideal electrocatalysts for oxygen evolution reaction (OER), have not been extensively applied in PEMWE, due to extremely high voltage and poor stability at large current density, caused by complicated structural variations of cobalt compounds during the OER process. Thus, the authors sought to introduce chromium into a cobalt spinel (Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub>) catalyst to regulate the electronic structure of cobalt, exhibiting a higher oxidation state and increased Co\u2013O covalency with a stable structure. In\u2010depth operando characterizations and theoretical calculations revealed that the activated Co\u2013O covalency and adaptable redox behavior are crucial for facilitating its OER activity. Both turnover frequency and mass activity of Cr\u2010doped Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub> (CoCr) at 1.67\u00a0V (vs RHE) increased by over eight times than those of as\u2010synthesized Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub>. The obtained CoCr catalyst achieved 1500\u00a0mA cm<jats:sup>\u22122<\/jats:sup> at 2.17\u00a0V and exhibited notable durability over extended operation periods \u2013 over 100\u00a0h at 500 mA\u2009cm<jats:sup>\u22122<\/jats:sup> and 500\u00a0h at 100 mA\u2009cm<jats:sup>\u22122<\/jats:sup>, demonstrating promising application in the PEMWE industry.<\/jats:p>","DOI":"10.1002\/advs.202402356","type":"journal-article","created":{"date-parts":[[2024,4,22]],"date-time":"2024-04-22T09:49:22Z","timestamp":1713779362000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["Chromium\u2010Induced High Covalent Co\u2013O Bonds for Efficient Anodic Catalysts in PEM Electrolyzer"],"prefix":"10.1002","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-1398-6135","authenticated-orcid":false,"given":"Qisheng","family":"Yan","sequence":"first","affiliation":[{"name":"State Key Laboratory of Molecular Engineering of 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