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Using atomic layer deposition, we precisely synthesized Fe sub\u2010nanocatalysts with tunable nuclearity (Fe\n                    <jats:sub>1<\/jats:sub>\n                    \u2013Fe\n                    <jats:sub>4<\/jats:sub>\n                    ) anchored on N,O\u2010co\u2010doped carbon nanorods (NOC). The electronic properties and spin configuration of the Fe sub\u2010nanocatalysts were nuclearity dependent and dominated the H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    activation modes and adsorption strength of active O species on Fe sites toward C\u2212H oxidation. The Fe\n                    <jats:sub>1<\/jats:sub>\n                    \u2010NOC single atom catalyst exhibits state\u2010of\u2010the\u2010art activity for benzene oxidation to phenol, which is ascribed to its unique coordination environment (Fe\n                    <jats:sub>1<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    ) and medium spin state (\n                    <jats:italic>\n                      t\n                      <jats:sub>2g<\/jats:sub>\n                      <jats:sup>4<\/jats:sup>\n                      e\n                      <jats:sub>g<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>\n                      <jats:italic>1<\/jats:italic>\n                    <\/jats:sup>\n                    ); turnover frequencies of 407\u2005h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 25\u2009\u00b0C and 1869\u2005h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 60\u2009\u00b0C were obtained, which is 3.4, 5.7, and 13.6 times higher than those of Fe dimer, trimer, and tetramer catalysts, respectively.\n                  <\/jats:p>","DOI":"10.1002\/anie.202216062","type":"journal-article","created":{"date-parts":[[2022,11,22]],"date-time":"2022-11-22T05:40:43Z","timestamp":1669095643000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Boosting Benzene Oxidation with a Spin\u2010State\u2010Controlled Nuclearity Effect on Iron Sub\u2010Nanocatalysts"],"prefix":"10.1002","volume":"62","author":[{"given":"Fanle","family":"Bu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of 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