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Here, we utilized organic cations to exfoliate bulk PHI and fabricate PHI nanosheets for producing H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    at a rate of 27.35\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    under simulated solar light irradiation, outperforming most of the reported carbon nitride\u2010based catalysts. Importantly, after 36\u00a0h of cyclic accumulation reactions in a self\u2010created spiral flow reactor, the H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    concentration stabilized at 2.7\u00a0wt.%, close to medical sterilization levels. In situ spectroscopic characterizations and density functional theory calculations revealed that the exfoliation results in molecular reconfiguration of the PHI basal planes, forming the active sites to promote charge separation and electron localization. This new structure also creates midgap states, enabling direct H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production via a one\u2010step, two\u2010electron pathway, bypassing the superoxide radical pathway. Theoretical calculations suggest that the localized electronic structure created by the active sites favors the protonation of adsorbed O\n                    <jats:sub>2<\/jats:sub>\n                    and stabilizes the *OOH species, which converts to H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    . This study elucidates and underscores the importance of active\u2010site reconfiguration for efficient photocatalytic oxygen reduction reaction (ORR) pathways.\n                  <\/jats:p>","DOI":"10.1002\/anie.202507415","type":"journal-article","created":{"date-parts":[[2025,5,16]],"date-time":"2025-05-16T03:49:58Z","timestamp":1747367398000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["Defective Poly(heptazine imide) Nanosheets for Efficient One\u2010Step Two\u2010Electron Photocatalytic O\n                    <sub>2<\/sub>\n                    Reduction to Medical\u2010Like H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"64","author":[{"given":"Laiyu","family":"Luo","sequence":"first","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China Heilongjiang University Harbin 150080 P.R. 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