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Herein, the fabrication of Ni<jats:sub>NP<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>@Ni<jats:sub>SA<\/jats:sub><jats:italic><jats:sub>y<\/jats:sub><\/jats:italic>\u2010NG (<jats:italic>x,y<\/jats:italic>\u00a0= 1, 2, 3; NG = nitrogen\u2010doped graphite) is reported, in which Ni single atom sites (Ni<jats:sub>SA<\/jats:sub>) and Ni nanoparticles (Ni<jats:sub>NP<\/jats:sub>) coexist. These Ni<jats:sub>NP<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>@Ni<jats:sub>SA<\/jats:sub><jats:italic><jats:sub>y<\/jats:sub><\/jats:italic>\u2010NG presented a volcano\u2010like trend for maximum CO Faradaic efficiency (FE<jats:sub>CO<\/jats:sub>) with the highest point at Ni<jats:sub>NP2<\/jats:sub>@Ni<jats:sub>SA2<\/jats:sub>\u2010NG in CO<jats:sub>2<\/jats:sub>RR. Ni<jats:sub>NP2<\/jats:sub>@Ni<jats:sub>SA2<\/jats:sub>\u2010NG exhibited \u224898% of maximum FE<jats:sub>CO<\/jats:sub> and a large current density of \u2212264 mA cm<jats:sup>\u22122<\/jats:sup> at \u22120.98 V (vs. RHE) in the flow cell. In situ experiment and density functional theory (DFT) calculations confirmed that the proper content of Ni<jats:sub>SA<\/jats:sub> and Ni<jats:sub>NP<\/jats:sub> balanced kinetic between proton\u2010feeding and CO<jats:sub>2<\/jats:sub> hydrogenation. The Ni<jats:sub>NP<\/jats:sub> in Ni<jats:sub>NP2<\/jats:sub>@Ni<jats:sub>SA2<\/jats:sub>\u2010NG promoted the formation of H* and reduced the energy barrier of *CO<jats:sub>2<\/jats:sub> hydrogenation to *COOH, and CO desorption can be efficiently facilitated by Ni<jats:sub>SA<\/jats:sub> sites, thereby resulting in enhanced CO<jats:sub>2<\/jats:sub>RR performance.<\/jats:p>","DOI":"10.1002\/smll.202300581","type":"journal-article","created":{"date-parts":[[2023,2,24]],"date-time":"2023-02-24T04:19:56Z","timestamp":1677212396000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":36,"title":["Revealing the Kinetic Balance between Proton\u2010Feeding and Hydrogenation in CO<sub>2<\/sub> Electroreduction"],"prefix":"10.1002","volume":"19","author":[{"given":"Sha","family":"Bai","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Tan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenjun","family":"Ning","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guihao","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhaohui","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianyang","family":"Shen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lirong","family":"Zheng","sequence":"additional","affiliation":[{"name":"Institute of High Energy Physics The Chinese Academy of Sciences  Beijing 100049 P. R. 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