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Herein, based on the concept of a hydrogen bonding trap, we proposed a novel concept to modulate the methane conversion pathway to hinder the overoxidation of target products. Taking boron nitride as a proof\u2010of\u2010concept model, for the first time it is found that the designed N\u2212H bonds can work as a hydrogen bonding trap to attract electrons. Benefitting from this property, the N\u2212H bonds on the BN surface rather than C\u2212H bonds in formaldehyde prefer to cleave, greatly suppressing the continuous dehydrogenation process. More importantly, formaldehyde will combine with the released protons, which leads to a proton rebound process to regenerate methanol. As a result, BN shows a high methane conversion rate (8.5\u2009%) and nearly 100\u2009% product selectivity to oxygenates under atmospheric pressure.<\/jats:p>","DOI":"10.1002\/anie.202302196","type":"journal-article","created":{"date-parts":[[2023,3,9]],"date-time":"2023-03-09T22:26:10Z","timestamp":1678400770000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":35,"title":["Methane Photooxidation with Nearly 100\u2009% Selectivity Towards Oxygenates: Proton Rebound Ensures the Regeneration of Methanol"],"prefix":"10.1002","volume":"62","author":[{"given":"Yuehan","family":"Cao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum University 610500 Chengdu China"},{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wang","family":"Yu","sequence":"additional","affiliation":[{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunqiu","family":"Han","sequence":"additional","affiliation":[{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuantao","family":"Yang","sequence":"additional","affiliation":[{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiqiang","family":"Rao","sequence":"additional","affiliation":[{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Guo","sequence":"additional","affiliation":[{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fan","family":"Dong","sequence":"additional","affiliation":[{"name":"Research Center for Environmental Science and Technology Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China 611731 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruiyang","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9995-0652","authenticated-orcid":false,"given":"Ying","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum University 610500 Chengdu China"},{"name":"School of New Energy and Materials Southwest Petroleum University 610500 Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,3,27]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.7b00236"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1038\/348428a0"},{"key":"e_1_2_7_4_1","unstructured":"\u00a0"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.aav0177"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c04826"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-018-0170-x"},{"key":"e_1_2_7_8_1","unstructured":"\u00a0"},{"key":"e_1_2_7_9_2","doi-asserted-by":"publisher","DOI":"10.1021\/cs500821r"},{"key":"e_1_2_7_10_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201702550"},{"key":"e_1_2_7_10_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201702550"},{"key":"e_1_2_7_11_1","unstructured":"\u00a0"},{"key":"e_1_2_7_12_2","volume-title":"CRC Handbook of Chemistry and Physics, 91st\u2005Edition","author":"Haynes W. 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