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Herein, we developed a medium\u2010spin Zn\u2013O\u2013Fe(MS) catalyst with tunable Fe(III) spin states, which can efficiently photo\u2010oxidize CH\n                    <jats:sub>4<\/jats:sub>\n                    to ethanol at ambient conditions. The unpaired electrons in d orbitals of Fe sites allow for efficient adsorption of \u2022OH, and the\n                    <jats:italic>e<\/jats:italic>\n                    <jats:sub>g<\/jats:sub>\n                    orbital occupancy enables stabilizing different key carbon\u2010containing intermediates (\u2022OCH\n                    <jats:sub>3<\/jats:sub>\n                    versus \u2022CH\n                    <jats:sub>2<\/jats:sub>\n                    OH). By balancing those two descriptors, the medium\u2010spin Zn\u2013O\u2013Fe(MS) catalyst allows to achieve selective generation of \u2022CH\n                    <jats:sub>2<\/jats:sub>\n                    OH intermediates with a moderate *OH coverage and subsequent coupling of \u2022CH\n                    <jats:sub>3<\/jats:sub>\n                    and \u2022CH\n                    <jats:sub>2<\/jats:sub>\n                    OH to ethanol. With a light intensity of 100 mW\u00b7cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and water as a weak oxidant, the Zn\u2013O\u2013Fe(MS) catalyst exhibited a peak photocatalytic CH\n                    <jats:sub>4<\/jats:sub>\n                    \u2010to\u2010ethanol yield of 372 \u00b5mol\u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00b7h\n                    <jats:sup>\u22121<\/jats:sup>\n                    without the use of photosensitizers or sacrificial reagents, which is \u223c3 times higher than the previously best reported photocatalytic CH\n                    <jats:sub>4<\/jats:sub>\n                    oxidation to ethanol under similar conditions. Our study suggests an attractive potential of converting CH\n                    <jats:sub>4<\/jats:sub>\n                    to multicarbon products by modulating spin states of the catalytic sites.\n                  <\/jats:p>","DOI":"10.1002\/anie.202510241","type":"journal-article","created":{"date-parts":[[2025,6,24]],"date-time":"2025-06-24T22:49:29Z","timestamp":1750805369000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":27,"title":["Switching Photocatalytic Methane Oxidation Toward Ethanol by Tuning Spin States"],"prefix":"10.1002","volume":"64","author":[{"given":"Shuya","family":"Hao","sequence":"first","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Maoyin","family":"Wang","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Leshen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ximeng","family":"Lv","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen","family":"Peng","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuhang","family":"Huang","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pei","family":"Yuan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Fuzhou University  Fuzhou Fujian 350108 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qing","family":"Han","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1803-6955","authenticated-orcid":false,"given":"Gengfeng","family":"Zheng","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai 200438 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