{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,17]],"date-time":"2026-10-17T14:35:08Z","timestamp":1792247708289,"version":"4.4.0"},"reference-count":69,"publisher":"Wiley","issue":"13","license":[{"start":{"date-parts":[[2025,1,27]],"date-time":"2025-01-27T00:00:00Z","timestamp":1737936000000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/onlinelibrary.wiley.com\/termsAndConditions#vor"},{"start":{"date-parts":[[2025,1,27]],"date-time":"2025-01-27T00:00:00Z","timestamp":1737936000000},"content-version":"tdm","delay-in-days":0,"URL":"http:\/\/doi.wiley.com\/10.1002\/tdm_license_1.1"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["52121004"],"award-info":[{"award-number":["52121004"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22376222"],"award-info":[{"award-number":["22376222"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":["onlinelibrary.wiley.com"],"crossmark-restriction":true},"short-container-title":["Angew Chem Int Ed"],"published-print":{"date-parts":[[2025,3,24]]},"abstract":"Abstract<\/jats:title>\n \n Unsaturated Ni single\u2010atom catalysts (SACs), Ni\u2010N\n x<\/jats:sub>\n (\n x<\/jats:italic>\n =1,2,3), have been investigated to break the conventional Ni\u2010N\n 4<\/jats:sub>\n structural limitation and provide more unoccupied 3d orbitals for CO\n 2<\/jats:sub>\n reduction reaction (CO\n 2<\/jats:sub>\n RR) intermediates adsorption, but their intrinsically low structural stability has seriously hindered their applications. Here, we developed a strategy by integrating Ni nanoclusters to stabilize unsaturated Ni\u2010N\n 3<\/jats:sub>\n atomic sites for efficient CO\n 2<\/jats:sub>\n electroreduction to CO at industrial\u2010level current. Density Functional Theory (DFT) calculations revealed that the incorporation of Ni nanocluster effectively stabilizes the unsaturated Ni\u2010N\n 3<\/jats:sub>\n atomic sites and modulates their electronic structure to enhance the adsorption of the key intermediate *COOH during CO\n 2<\/jats:sub>\n RR. Guided by these insights, we prepared an optimal composite catalyst, Ni\n 6<\/jats:sub>\n @Ni\u2010N\n 3<\/jats:sub>\n , which features a Ni\n 6<\/jats:sub>\n N\n 6<\/jats:sub>\n nanocluster surrounded by six Ni\u2010N\n 3<\/jats:sub>\n single atoms sites, through low\u2010temperature pyrolysis. The morphology and coordinative structure of Ni\n 6<\/jats:sub>\n @Ni\u2010N\n 3<\/jats:sub>\n were confirmed by an aberration\u2010corrected transmission electron microscope (AC\u2010TEM) and X\u2010ray absorption spectroscopy (XAS). As a result, Ni\n 6<\/jats:sub>\n @Ni\u2010N\n 3<\/jats:sub>\n demonstrated a remarkably high CO Faradaic efficiency (FE\n CO<\/jats:sub>\n ) of 99.7\u2009% and a turnover frequency (TOF) of 83984.2\u2005h\n \u22121<\/jats:sup>\n at 500\u2005mA\u2009cm\n \u22122<\/jats:sup>\n under \u22121.15\u2005V\n RHE<\/jats:sub>\n , much better than those of Ni\u2010N\n 4<\/jats:sub>\n with a lower FE\n CO<\/jats:sub>\n of 86\u2009% at 100\u2005mA\u2009cm\n \u22122<\/jats:sup>\n and a TOF of 39309.9\u2005h\n \u22121<\/jats:sup>\n under identical potential. XAS analyses of Ni\n 6<\/jats:sub>\n @Ni\u2010N\n 3<\/jats:sub>\n before and after long\u2010term CO\n 2<\/jats:sub>\n RR testing confirmed the excellent stability of its coordinative environment. This work highlights a generalizable approach for stabilizing unsaturated single\u2010atom catalysts, paving the way for their application in high\u2010performance CO\n 2<\/jats:sub>\n RR.\n <\/jats:p>","DOI":"10.1002\/anie.202424552","type":"journal-article","created":{"date-parts":[[2025,1,7]],"date-time":"2025-01-07T22:53:04Z","timestamp":1736290384000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":48,"title":["Nickel Nanocluster\u2010Stabilized Unsaturated Ni\u2013N\n 3<\/sub>\n Atomic Sites for Efficient CO\n 2<\/sub>\n \u2010to\u2010CO Electrolysis at Industrial\u2010Level Current"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-1305-4253","authenticated-orcid":false,"given":"Wuyi","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Metallurgy and Environment Central South University Changsha 410083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8744-1105","authenticated-orcid":false,"given":"Asad","family":"Mehmood","sequence":"additional","affiliation":[{"name":"Division 3.6 \u2013 Electrochemical Energy Materials Bundesanstalt f\u00fcr Materialforschung und -pr\u00fcfung (BAM) 12203 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6272-486X","authenticated-orcid":false,"given":"Ghulam","family":"Ali","sequence":"additional","affiliation":[{"name":"U.S.-Pakistan Center for Advanced Studies in Energy (USPCAS-E) National University of Sciences and Technology (NUST) lslamabad 44000 Pakistan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2693-2546","authenticated-orcid":false,"given":"Hui","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Metallurgy and Environment Central South University Changsha 410083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liyuan","family":"Chai","sequence":"additional","affiliation":[{"name":"School of Metallurgy and Environment Central South University Changsha 410083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7067-6917","authenticated-orcid":false,"given":"Jun","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Metallurgy and Environment Central South University Changsha 410083 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":"School of Metallurgy and Environment Central South University Changsha 410083 China"},{"name":"Hunan Joint International Research Center for Carbon Dioxide Resource Utilization School of Physics Central South University Changsha 410083 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