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Herein, mesoporous Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub> (mCo<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub>\u2010350) showed excellent catalytic activity for selective oxidation of aromatic\u2010alkanes, especially for oxidation of ethylbenzene with a conversion of 42\u2009% and selectivity of 90\u2009% for acetophenone at 120\u2009\u00b0C. Notably, mCo<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub> presented a unique catalytic path of direct oxidation of aromatic\u2010alkanes to aromatic ketones rather than the conventional stepwise oxidation to alcohols and then to ketones. Density functional theory calculations revealed that oxygen vacancies in mCo<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub> activate around Co atoms, causing electronic state change from Co<jats:sup>3+<\/jats:sup><jats:sub>(<jats:italic>O<\/jats:italic>h)<\/jats:sub>\u2192Co<jats:sup>2+<\/jats:sup><jats:sub>(<jats:italic>O<\/jats:italic>h)<\/jats:sub>. Co<jats:sup>2+<\/jats:sup><jats:sub>(<jats:italic>O<\/jats:italic>h)<\/jats:sub> has great attraction to ethylbenzene, and weak interaction with O<jats:sub>2<\/jats:sub>, which provide insufficient O<jats:sub>2<\/jats:sub> for gradual oxidation of phenylethanol to acetophenone. Combined with high energy barrier for forming phenylethanol, the direct oxidation path from ethylbenzene to acetophenone is kinetically favorable on mCo<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub>, sharply contrasted to non\u2010selective oxidation of ethylbenzene on commercial Co<jats:sub>3<\/jats:sub>O<jats:sub>4<\/jats:sub>.<\/jats:p>","DOI":"10.1002\/anie.202306261","type":"journal-article","created":{"date-parts":[[2023,5,24]],"date-time":"2023-05-24T08:37:22Z","timestamp":1684917442000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":67,"title":["Efficient Selective Oxidation of Aromatic Alkanes by Double Cobalt Active Sites over Oxygen Vacancy\u2010rich Mesoporous Co<sub>3<\/sub>O<sub>4<\/sub>"],"prefix":"10.1002","volume":"62","author":[{"given":"Yali","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University  Changchun, Jilin 130012 China"},{"name":"Department of Chemical Engineering, School of Petrochemical Engineering &amp; Environment Zhejiang Ocean University  Zhoushan, Zhejiang 316022 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuenan","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University  Changchun, Jilin 130012 China"},{"name":"State Key Laboratory of Fine Chemicals, School of Chemical Engineering Dalian University of Technology  Dalian, Liaoning 116081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Danyang","family":"Feng","sequence":"additional","affiliation":[{"name":"Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Northeast Normal University  Jilin 130024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liangliang","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University  Changchun, Jilin 130012 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry Jilin University  Changchun, Jilin 130012 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaowei","family":"Song","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University  Changchun, Jilin 130012 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6064-9360","authenticated-orcid":false,"given":"Zhen\u2010An","family":"Qiao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University  Changchun, Jilin 130012 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,6,12]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr050523v"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/18417"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja200997a"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.8b00330"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1183602"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature12284"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemmater.8b03624"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-021-03637-6"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abd1085"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c12817"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aax6637"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1215864"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.7b00272"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-021-00725-8"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7GC00469A"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201600455"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.matt.2020.02.002"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5NR03802B"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1039\/b820519a"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-23150-8"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201207920"},{"key":"e_1_2_8_22_1","volume":"30","author":"Huang K.","year":"2018","journal-title":"Adv. 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