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Alternative feedstock of low\u2010cost methanol is expected to fulfill this breakthrough due to its green and renewable nature; however, the overoxidation of methanol severely inhibits the efficacious formamide synthesis from methanol and ammonia through the conventional catalytic route. Herein, we report the successful development of a direct radical coupling route for converting methanol and ammonia into high\u2010selectivity formamide and hydrogen without extra oxidants under ambient conditions. The optimized Pt\u2010CdS photocatalysts offered an impressive formamide production rate of 1.45\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , as well as an exceptional hole selectivity reaching up to 63.5%. The oxidant\u2010free radical mechanism of high\u2010efficiency formamide generation as revealed by in situ characterizations (e.g., in situ electron paramagnetic resonance and in situ transient absorption spectroscopy), stems from the photogenerated holes oxidizing the methanol to hydroxymethyl radical for subsequently direct C\u2500N coupling with amino radical. This work demonstrates an efficient oxidant\u2010free photoinduced radical coupling strategy with the promise of an acceptable alternative to current technologies for artificial photosynthesis formamide using clean and abundant solar energy.\n                  <\/jats:p>","DOI":"10.1002\/anie.202500747","type":"journal-article","created":{"date-parts":[[2025,3,12]],"date-time":"2025-03-12T01:59:06Z","timestamp":1741744746000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":20,"title":["Artificial Photosynthesis of Formamide via an Oxidant\u2010Free Photoinduced Radical Coupling Route over Pt\u2010CdS"],"prefix":"10.1002","volume":"64","author":[{"given":"Junyu","family":"Gao","sequence":"first","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing 100190 China"},{"name":"Center of Materials Science and 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