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In this reaction, methyl radical (\u22c5CH<jats:sub>3<\/jats:sub>) was deemed a key intermediate that affected the yields and selectivity of the products. However, direct observation of \u22c5CH<jats:sub>3<\/jats:sub> and other intermediates is still challenging. Here, a rectangular photocatalytic reactor coupled with in situ synchrotron radiation photoionization mass spectrometry (SR\u2010PIMS) was developed to detect reactive intermediates within several hundred microseconds during photocatalytic methane oxidation over Ag\u2212ZnO. Gas phase \u22c5CH<jats:sub>3<\/jats:sub> generated by photogenerated holes (O<jats:sup>\u2212<\/jats:sup>) was directly observed, and its formation was demonstrated to be significantly enhanced by coadsorbed oxygen molecules. Methoxy radical (CH<jats:sub>3<\/jats:sub>O\u22c5) and formaldehyde (HCHO) were confirmed to be key C1 intermediates in photocatalytic methane overoxidation to CO<jats:sub>2<\/jats:sub>. The gas\u2010phase self\u2010coupling reaction of \u22c5CH<jats:sub>3<\/jats:sub> contributes to the formation of ethane, which indicates the key role of \u22c5CH<jats:sub>3<\/jats:sub> desorption in the highly selective synthesis of ethane. Based on the observed intermediates, the reaction network initiated from \u22c5CH<jats:sub>3<\/jats:sub> of photocatalytic methane oxidation could be clearly illustrated, which is helpful for studying the photocatalytic methane conversion processes.<\/jats:p>","DOI":"10.1002\/anie.202304352","type":"journal-article","created":{"date-parts":[[2023,5,23]],"date-time":"2023-05-23T14:54:17Z","timestamp":1684853657000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":38,"title":["Illustrating the Fate of Methyl Radical in Photocatalytic Methane Oxidation over Ag\u2212ZnO by in situ Synchrotron Radiation Photoionization Mass Spectrometry"],"prefix":"10.1002","volume":"62","author":[{"given":"Chengyuan","family":"Liu","sequence":"first","affiliation":[{"name":"National Synchrotron Radiation Laboratory University of Science and Technology of China  Hefei, Anhui 230029 P. R. 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