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However, studies on the impact of coordinated\u2010nitrogen species in the active center on the spin state and catalytic activity remain scarce. Herein, two single Ni atom electrocatalysts with distinct pyridinic\u2010N and pyrrolic\u2010N coordination through a rapid Joule\u2010heating method that preserves precursor nitrogen configurations. Magnetic susceptibility measurements reveal that pyridinic\u2010N induces a high\u2010spin state in Ni centers, while pyrrolic\u2010N stabilizes a low\u2010spin configuration. The high\u2010spin Ni\u2013N\n                    <jats:sub>pyridinic<\/jats:sub>\n                    \u2013C demonstrates an exceptional performance in electrocatalytic CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction, achieving 98.8% CO Faradaic efficiency in H\u2010cells and maintaining\u00a0&gt;99% Faradaic efficiency at industrial current densities (\u2265250\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ) across alkaline, neutral, and acidic electrolytes in a gas\u2010diffusion flow cell. A maximum power density of 1.89\u00a0mW\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and excellent charge\u2013discharge cyclability also achieve in zinc\u2013CO\n                    <jats:sub>2<\/jats:sub>\n                    battery, further demonstrating the applicability of Ni\u2013N\n                    <jats:sub>pyridinic<\/jats:sub>\n                    \u2013C. Theoretical calculations demonstrate that the high\u2010spin state enhances d\u2010orbital dispersion, strengthening hybridization with \u03c0* orbital of CO\n                    <jats:sub>2<\/jats:sub>\n                    and stabilizing *COOH intermediates, thereby accelerating CO\n                    <jats:sub>2<\/jats:sub>\n                    activation. This study not only establishes a novel strategy for spin\u2010state engineering through coordination control but also advances scalable electrocatalyst design for efficient carbon cycling.\n                  <\/jats:p>","DOI":"10.1002\/anie.202506845","type":"journal-article","created":{"date-parts":[[2025,6,11]],"date-time":"2025-06-11T22:11:11Z","timestamp":1749679871000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":37,"title":["Modulating Spin State of Ni Single Atomic Center for High\u2010Performance Electrocatalytic Carbon Dioxide Reduction"],"prefix":"10.1002","volume":"64","author":[{"given":"Zhen","family":"Chen","sequence":"first","affiliation":[{"name":"Henan Institute of Advanced Technology, State Key Laboratory of Coking Coal Resources Green Exploitation, and College of Chemistry Zhengzhou University  Zhengzhou 450001 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Key Laboratory of Coking Coal Resources Green Exploitation, and College of Chemistry Zhengzhou University  Zhengzhou 450001 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6728-0559","authenticated-orcid":false,"given":"Shuang\u2010Quan","family":"Zang","sequence":"additional","affiliation":[{"name":"Henan Key Laboratory of Crystalline Molecular Functional Materials, and College of Chemistry Zhengzhou University  Zhengzhou 450001 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