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Compared with conventional thermocatalytic method, it's more attractive to synthesize PDO via green electrocatalytic technology especially utilizing waste nitrogen oxides gas as nitrogen source. However, there are great challenges in catalyst design for high\u2010efficiency electrosynthetic oxime due to the low electron transport rate and multiple competing reactions. Herein, we propose an interfacial coordination strategy based on metal\u2013organic frameworks (MOF) electrocatalyst for the first time to promote oxime electrosynthesis, by building Zn\u2212O bridges between graphite felt (GF) and zeolitic imidazolate framework (ZIF\u20107\/CGF). Specially, ZIF\u20107\/CGF delivers a Faraday efficiency (FE) of 75.9\u2009% with yield up to 73.1\u2009% for 1\u2010methyl\u20104\u2010piperidone oxime, which is far superior to the catalyst without Zn\u2212O bridges (a FE of 10.7\u2009% and yield of 10.3\u2009%). In\u2010depth mechanism study shows that the introducing Zn\u2212O bridges can promote the electron transfer and induce Zn sites transforming into distorted tetrahedron (Zn\u2010N<jats:sub>3<\/jats:sub>O) coordination mode, which benefits for intermediates adsorption and conversion. The developed strategy presents wide universalities towards various oximes electrosynthesis and adapts to other MOF materials (ZIF\u20108, ZIF\u20104). This work provides new insights for electrosynthetic organic chemicals and upgrading nitrogen cycle through rational design surficial coordinated electrocatalysts.<\/jats:p>","DOI":"10.1002\/anie.202419550","type":"journal-article","created":{"date-parts":[[2025,2,21]],"date-time":"2025-02-21T12:30:16Z","timestamp":1740141016000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":41,"title":["Interfacial Asymmetrically Coordinated Zn\u2212MOF for High\u2010Efficiency Electrosynthetic Oxime"],"prefix":"10.1002","volume":"64","author":[{"given":"Jiawei","family":"Kang","sequence":"first","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM IGCME School of Chemistry Sun Yat-Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peisen","family":"Liao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM IGCME School of Chemistry Sun Yat-Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Runan","family":"Xiang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM IGCME School of Chemistry Sun Yat-Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenpei","family":"Liao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM IGCME School of Chemistry Sun Yat-Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenyu","family":"Yang","sequence":"additional","affiliation":[{"name":"National Synchrotron Radiation Laboratory University of Science and Technology of China  Hefei 230029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shihan","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM IGCME School of Chemistry Sun Yat-Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qinghua","family":"Liu","sequence":"additional","affiliation":[{"name":"National Synchrotron Radiation Laboratory University of Science and Technology of China  Hefei 230029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1233-5591","authenticated-orcid":false,"given":"Guangqin","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM IGCME School of Chemistry Sun Yat-Sen University  Guangzhou 510006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,2,21]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-022-00971-8"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-49167-3"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.abb2559"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-24104-w"},{"key":"e_1_2_7_6_1","unstructured":"\u00a0"},{"key":"e_1_2_7_7_2","unstructured":"S.\u2005K. 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