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Here, we present a continuous flow photocatalytic platform that enables the efficient coupling of C\u2500N bonds between methanol and ammonia at ambient temperature and pressure. By synergistically engineering a Pd clusters\u2010decorated TiO\n                    <jats:sub>2<\/jats:sub>\n                    photocatalyst (1Pd\/TiO\n                    <jats:sub>2<\/jats:sub>\n                    ) and a mass transfer\u2010enhanced gas\u2013liquid\u2013solid Taylor flow reactor, the system achieves a remarkable formamide productivity of 256.80\u00a0\u00b5mol h\n                    <jats:sup>\u22121<\/jats:sup>\n                    (6.83\u2010fold enhancement compared to batch reactors) with less than 10% decay in production rate over 50 h of continuous operation, which is remarkably superior to state\u2010of\u2010the\u2010art photocatalytic systems for the synthesis of C\u2500N compounds from C1 small molecules. Distinguishing from the conventional simultaneous bimolecular one\u2010electron oxidation pathway, a mechanistic study has shown that the precisely tailored Pd clusters on TiO\n                    <jats:sub>2<\/jats:sub>\n                    induce charge polarization to drive methanol dehydrogenation toward critical *CH\n                    <jats:sub>2<\/jats:sub>\n                    O intermediates, enabling direct nucleophilic NH\n                    <jats:sub>3<\/jats:sub>\n                    attack for C\u2500N bond formation, thereby circumventing thermodynamic\/kinetic barriers inherent to asynchronous radical generation in prior systems. This work establishes a paradigm for the sustainable, efficient synthesis of formamide via photocatalytic C\u2500N coupling by bridging nanoscale photocatalyst engineering with macroscopic reactor design.\n                  <\/jats:p>","DOI":"10.1002\/anie.202515803","type":"journal-article","created":{"date-parts":[[2025,9,10]],"date-time":"2025-09-10T07:36:29Z","timestamp":1757489789000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Continuous Flow Photocatalysis Boosting C\u2500N Coupling for Sustainable High\u2010Efficiency Formamide Synthesis"],"prefix":"10.1002","volume":"64","author":[{"given":"Junchi","family":"Xu","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale School of Chemistry and Materials Science State Key Laboratory of Precision and Intelligent Chemistry National Synchrotron Radiation Laboratory University of Science and Technology 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