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However, their performance is intrinsically limited by weak spin\u2013orbit coupling (SOC) arising from van der Waals interlayer interactions, thereby suppressing intersystem crossing and triplet\u2010exciton utilization. In this study, we demonstrate that layer\u2010bridging Co single atoms activate triplet excitons in COFs by synergistically enhancing SOC and inducing energy\u2010level splitting via Co\u2500N coordination. This layer\u2010bridging Co coordination markedly promotes singlet\u2010to\u2010triplet conversion, enabling efficient O\n                    <jats:sub>2<\/jats:sub>\n                    activation and substantially boosting the generation of both\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    and O\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2022\u2212<\/jats:sup>\n                    . Consequently, the Co\u2010bridged COF achieves highly efficient photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production and tandem C\u2500N coupling. This work establishes layer\u2010bridging single\u2010atom coordination as a promising strategy for regulating triplet\u2010state reactivity in COFs, offering new opportunities for reactive oxygen species (ROS)\u2010mediated photocatalysis and tandem organic transformations.\n                  <\/jats:p>","DOI":"10.1002\/anie.1580812","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T14:28:16Z","timestamp":1787149696000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Activating Triplet Excitons in COFs via Layer\u2010Bridging Co Single Atoms for Photocatalytic H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Production and Tandem C\u2500N Coupling"],"prefix":"10.1002","volume":"65","author":[{"given":"Guoen","family":"Tang","sequence":"first","affiliation":[{"name":"Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences  Wuhan P. 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