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Their structures dynamically evolve with applied electrode potentials, allowing the active sites to adjust interactions with intermediates, thereby improving electrocatalytic performance. However, the dynamic changes in these interactions under applied potentials remain poorly understood, hindering the design of more diverse electrocatalytic systems. Herein, we developed a strategy that unitizes electrode potential to control the interactions between active sites and intermediates over oxygen vacancy\u2010modified TiO<jats:sub>2<\/jats:sub> (V<jats:sub>O<\/jats:sub>\u2212TiO<jats:sub>2\u2212x<\/jats:sub>) to enhance NORR performance. By combining state\u2010of\u2010the\u2010art constant inner potential (CIP) DFT calculations with in situ (spectro)electrochemical measurements, we investigated how the electrode potential influences these interactions in NORR. The results clearly demonstrate that applying an external potential alters the spatial symmetry of degenerate orbitals of Ti<jats:sup>3+<\/jats:sup> to facilitate the generation of key intermediates for NO\u2010to\u2010NH<jats:sub>3<\/jats:sub> conversion. Therefore, the V<jats:sub>O<\/jats:sub>\u2212TiO<jats:sub>2\u2212x<\/jats:sub> catalyst exhibited superior NORR performance with a NH<jats:sub>3<\/jats:sub> Faradaic efficiency up to 76.4\u2009% and a high NH<jats:sub>3<\/jats:sub> yield rate of 632.9\u2005\u03bcg\u2009h<jats:sup>\u22121<\/jats:sup>\u2009mg<jats:sub>cat.<\/jats:sub><jats:sup>\u22121<\/jats:sup> under 1.0\u2005vol\u2009% NO atmosphere, which is competitive with those of previously reported works under higher NO concentration (above 10\u2005vol\u2009%). Remarkably, the NORR process achieved a record\u2010breaking NH<jats:sub>3<\/jats:sub> yield of 2292.7\u2005\u03bcg\u2009h<jats:sup>\u22121<\/jats:sup>\u2009mg<jats:sub>cat.<\/jats:sub><jats:sup>\u22121<\/jats:sup> in a membrane electrode assembly (MEA) electrolyzer under the same conditions. This study opens a new avenue for enhancing electrocatalytic activity by adjusting operating conditions, thereby transcending the limitations of material design.<\/jats:p>","DOI":"10.1002\/anie.202420346","type":"journal-article","created":{"date-parts":[[2024,11,20]],"date-time":"2024-11-20T22:13:29Z","timestamp":1732140809000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Enhancing Low\u2010Concentration Electroreduction of NO to NH<sub>3<\/sub> via Potential\u2010Controlled Active Site\u2010Intermediate Interactions"],"prefix":"10.1002","volume":"64","author":[{"given":"Xiaoxi","family":"Guo","sequence":"first","affiliation":[{"name":"Hunan Joint International Research Center for Carbon Dioxide Resource Utilization State Key Laboratory of Powder Metallurgy School of Physics Central South University  410083 Changsha Hunan P.\u2005R. China"},{"name":"School of Materials Science and Engineering Central South University  410083 Changsha Hunan P.\u2005R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tongwei","family":"Wu","sequence":"additional","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  610054 Chengdu Sichuan P.\u2005R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hengfeng","family":"Li","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Central South University  410083 Changsha Hunan P.\u2005R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liyuan","family":"Chai","sequence":"additional","affiliation":[{"name":"School of Metallurgy and Environment Central South University  410083 Changsha Hunan P.\u2005R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9007-4817","authenticated-orcid":false,"given":"Min","family":"Liu","sequence":"additional","affiliation":[{"name":"Hunan Joint International Research Center for Carbon Dioxide Resource Utilization State Key Laboratory of Powder Metallurgy School of Physics Central South University  410083 Changsha Hunan P.\u2005R. China"},{"name":"School of Metallurgy and Environment Central South University  410083 Changsha Hunan P.\u2005R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,12,2]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.9b00202"},{"key":"e_1_2_7_2_1","volume":"36","author":"Wu Z.","year":"2024","journal-title":"Adv. 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