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Inspired by the versatile methanol activation on photoexcited solids, we here report a practicable semiconductor\u2010based photocatalytic system for C\u2500H methylation of\n                    <jats:italic>N<\/jats:italic>\n                    \u2010heteroarenes. To be specific, hexagonal cadmium sulfide (\n                    <jats:italic>h<\/jats:italic>\n                    \u2010CdS) was identified to be an ideal platform for visible\u2010light\u2010driven photocatalytic methanol activation, where selective \u2022CH\n                    <jats:sub>2<\/jats:sub>\n                    OH generation undergoing a hole\u2010transfer process without any additional co\u2010catalysts or co\u2010solvent could trigger C\u2500H hydroxymethylation of\n                    <jats:italic>N<\/jats:italic>\n                    \u2010heteroarenes. The following electron transfer between photoexcited\n                    <jats:italic>h<\/jats:italic>\n                    \u2010CdS and hydroxymethylated intermediates could finally lead to the formation of methylated\n                    <jats:italic>N<\/jats:italic>\n                    \u2010heteroarenes. The transformations facilitate the cascade utilization of photoinduced hole and electron, thereby endowing\n                    <jats:italic>h<\/jats:italic>\n                    \u2010CdS with extraordinary photocatalytic performance. Besides, selective generation of hydroxymethylated\/methylated product could be facilely implemented in the presence\/absence of electron scavengers.\n                  <\/jats:p>","DOI":"10.1002\/anie.202507093","type":"journal-article","created":{"date-parts":[[2025,4,11]],"date-time":"2025-04-11T07:51:06Z","timestamp":1744357866000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Visible\u2010Light\u2010Driven Photocatalytic Methanol Activation on Hexagonal CdS for Triggering C\u2500H Methylation"],"prefix":"10.1002","volume":"64","author":[{"given":"Gang","family":"Chen","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei Anhui 230026 P.R. 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