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Herein, we report an iridium and lanthanum co\u2010doped manganese\u2010cobalt spinel catalyst, Ir,La\u2010MCO\n                    <jats:sub>\u03b4<\/jats:sub>\n                    , featuring octahedral La\u2013Ir pairs (La\n                    <jats:sub>oct<\/jats:sub>\n                    \u2013Ir\n                    <jats:sub>oct<\/jats:sub>\n                    ) with a theoretical favorable configuration of adjacent bridging and Ir\n                    <jats:italic>z<\/jats:italic>\n                    \u2010axis oxygen vacancies. This low\u2010Ir catalyst Ir,La\u2010MCO\n                    <jats:sub>\u03b4<\/jats:sub>\n                    (0.12\u00a0mg Ir cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ) exhibits an overpotential of merely 220\u00a0mV at 10\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in pH = 1 electrolyte, and demonstrates robust operation for over 1550\u00a0h at 1 A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in a proton exchange membrane (PEM) water electrolyzer. Coupled (quasi)in situ characterizations and operando spectroscopy reveal that the adjacent oxygen vacancies mediate the evolution of oxygen intermediates, enabling water\u2010derived oxygen\u2010hydroxyl coupling with negligible lattice oxygen involvement, via a decoupled proton\u2013electron transfer pathway. This mechanism preserves the structural integrity of the catalyst and yields a calculated reaction free\u2010energy change of merely 0.38\u00a0eV (\n                    <jats:italic>U<\/jats:italic>\n                    = 1.23\u00a0V) for the most unfavorable oxygen\u2010hydroxyl coupling elementary step, thereby endowing Ir,La\u2010MCO\n                    <jats:sub>\u03b4<\/jats:sub>\n                    with exceptional durability. This work provides a valuable mechanistic insight into designing highly stable defective catalysts.\n                  <\/jats:p>","DOI":"10.1002\/adma.75352","type":"journal-article","created":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T07:53:11Z","timestamp":1791618791000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Vacancy\u2010Associated La\u2013Ir Pairs Enable Water\u2010Derived Oxygen\u2010Hydroxyl Coupling for Durable Low\u2010Ir PEM Water Electrolysis"],"prefix":"10.1002","author":[{"given":"Yong","family":"Gao","sequence":"first","affiliation":[{"name":"Centre for Hydrogenergy College of Materials Science and Technology Nanjing University of Aeronautics and Astronautics  Nanjing P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9207-2452","authenticated-orcid":false,"given":"Yinlong","family":"Zhu","sequence":"additional","affiliation":[{"name":"Institute for Frontier Science Nanjing University of Aeronautics and Astronautics  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1851-4803","authenticated-orcid":false,"given":"Zhong\u2010Shuai","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian P. R. 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