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However, the over\u2010oxidation of target products is usually unavoidable due to the easily excessive activation of C\u2212H bond on the sites of supported metal species. Here, we identified the most efficient Zr\u2010oxo nodes of UiO\u201066 metal\u2010organic frameworks (MOFs) catalysts for the selective oxidation of methane with H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub>. These nodes were modified by three types of benzene 1, 4\u2010dicarboxylates (NH<jats:sub>2<\/jats:sub>\u2010BDC, H<jats:sub>2<\/jats:sub>BDC, and NO<jats:sub>2<\/jats:sub>\u2010BDC). Detailed characterizations and DFT calculations revealed that these ligands can effectively tune the electronic properties of Zr\u2010oxo nodes and the H<jats:sub>2<\/jats:sub>BDC ligand led to optimal electronic density of Zr\u2010oxo nodes in UiO\u201066. Thus the UiO\u201066\u2010H catalyst promoted the formation of \u22c5OH species that adsorbed on Zr\u2010oxo nodes, and facilitated the activation of methane with a lower energy barrier and subsequent conversion to hydroxylation oxygenates with 100\u2009% selectivity.<\/jats:p>","DOI":"10.1002\/anie.202205077","type":"journal-article","created":{"date-parts":[[2022,6,30]],"date-time":"2022-06-30T03:53:47Z","timestamp":1656561227000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":75,"title":["Zirconium\u2010oxo Nodes of MOFs with Tunable Electronic Properties Provide Effective \u22c5OH Species for Enhanced Methane Hydroxylation"],"prefix":"10.1002","volume":"61","author":[{"given":"Geqian","family":"Fang","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China"},{"name":"University of Chinese Academy of Sciences 19A Yuquan Road, Shijingshan District Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin\u2010Nian","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Guizhou University Guiyang 550025 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling\u2010Chan","family":"Tian","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Guizhou University Guiyang 550025 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin\u2010Xia","family":"Liang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Guizhou University Guiyang 550025 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1084-7446","authenticated-orcid":false,"given":"Jian","family":"Lin","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lin","family":"Li","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chun","family":"Zhu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Guizhou University Guiyang 550025 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8705-1278","authenticated-orcid":false,"given":"Xiaodong","family":"Wang","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2022,7,27]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2016.05.081"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.9b00223"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1360\/SSC-2020-0191"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.cjche.2021.04.034"},{"key":"e_1_2_7_6_1","unstructured":"\u00a0"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1016\/S0926-860X(99)00160-X"},{"key":"e_1_2_7_8_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.aam9035"},{"key":"e_1_2_7_9_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.cattod.2017.01.023"},{"key":"e_1_2_7_10_1","unstructured":"\u00a0"},{"key":"e_1_2_7_11_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202108069"},{"key":"e_1_2_7_11_3","doi-asserted-by":"crossref","first-page":"202108069","DOI":"10.1002\/ange.202108069","volume":"134","year":"2022","journal-title":"Angew. 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