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Herein, abundant electron\u2010enriched lattice oxygen species were introduced into CeO<jats:sub>2<\/jats:sub> catalyst by constructing the point defects and crystal\u2010terminated phases in the crystal reconstruction process. Benefitting from the acid\u2010base properties modulated by the electron\u2010enriched lattice oxygen, the optimized CeO<jats:sub>2<\/jats:sub> catalyst exhibited a much higher DMC yield of 22.2 mmol g<jats:sup>\u20101<\/jats:sup> than the reported metal\u2010oxide\u2010based catalysts at the similar conditions. Mechanistic investigations illustrated that the electron\u2010enriched lattice oxygen can provide abundant sites for CO<jats:sub>2<\/jats:sub> adsorption and activation, and was advantageous of the formation of the weakly adsorbed active methoxy species. These were facilitating to the coupling of methoxy and CO<jats:sub>2<\/jats:sub> for the key *CH<jats:sub>3<\/jats:sub>OCOO intermediate formation. More importantly, the weakened adsorption of *CH<jats:sub>3<\/jats:sub>OCOO on the electron\u2010enriched lattice oxygen can switch the rate\u2010determining\u2010step (RDS) of DMC synthesis from *CH<jats:sub>3<\/jats:sub>OCOO formation to *CH<jats:sub>3<\/jats:sub>OCOO dissociation, and lower the corresponding activation barriers, thus giving rise to a high performance. This work provides insights into the underlying reaction mechanism for DMC synthesis from CO<jats:sub>2<\/jats:sub> and methanol and the design of highly efficient catalysts.<\/jats:p>","DOI":"10.1002\/anie.202402053","type":"journal-article","created":{"date-parts":[[2024,3,18]],"date-time":"2024-03-18T03:45:26Z","timestamp":1710733526000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":86,"title":["Dimethyl Carbonate Synthesis from CO<sub>2<\/sub> over CeO<sub>2<\/sub> with Electron\u2010Enriched Lattice Oxygen Species"],"prefix":"10.1002","volume":"63","author":[{"given":"Guoqiang","family":"Hou","sequence":"first","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qi","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Di","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haifeng","family":"Fan","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaidi","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yangyang","family":"Li","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiang\u2010Kui","family":"Gu","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8769-4153","authenticated-orcid":false,"given":"Mingyue","family":"Ding","sequence":"additional","affiliation":[{"name":"School of Power and Mechanical Engineering the Institute of Technological Sciences Wuhan University  Wuhan 430072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,4,8]]},"reference":[{"key":"e_1_2_8_1_1","unstructured":"\u00a0"},{"key":"e_1_2_8_2_2","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00025F"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.5194\/essd-10-2141-2018"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.1c01610"},{"key":"e_1_2_8_5_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.trechm.2023.01.008"},{"key":"e_1_2_8_6_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2017.04.112"},{"key":"e_1_2_8_7_1","unstructured":"\u00a0"},{"key":"e_1_2_8_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/adsu.202200087"},{"key":"e_1_2_8_9_2","doi-asserted-by":"publisher","DOI":"10.1080\/01614940.2019.1696609"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/cs501221q"},{"key":"e_1_2_8_11_1","unstructured":"\u00a0"},{"key":"e_1_2_8_12_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.8b00415"},{"key":"e_1_2_8_13_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202214490"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-019-08697-x"},{"key":"e_1_2_8_15_1","unstructured":"\u00a0"},{"key":"e_1_2_8_16_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.5b00603"},{"key":"e_1_2_8_17_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.7b04198"},{"key":"e_1_2_8_18_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2014.12.013"},{"key":"e_1_2_8_19_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jallcom.2016.10.293"},{"key":"e_1_2_8_20_1","volume":"135","author":"Li W.","year":"2023","journal-title":"Angew. 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