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Herein, we designed highly active metal atom clusters anchored on semiconductor nanosheets, which established heteroatom sites on the interface to steer C\u2212C coupling, realizing air\u2010concentration CO\n                    <jats:sub>2<\/jats:sub>\n                    photoreduction into C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    in pure water. As an example, the Pd nanoclusters loaded on ZnO nanosheets are prepared, demonstrated by the X\u2010ray photoelectron spectroscopy and high\u2010angle annular dark\u2010field image. In situ Fourier transform infrared spectroscopy confirms the C\u2212C coupling step over the Pd\u2010ZnO nanosheets, while quasi in situ X\u2010ray photoelectron spectroscopy illustrates the active sites of Pd and Zn atoms on the Pd\u2010ZnO nanosheets during CO\n                    <jats:sub>2<\/jats:sub>\n                    photoreduction. Density functional theoretical calculations unveil the transition state energy barrier of C\u2212C coupling of CO* and COH* intermediates are only 0.998\u2005eV, hinting the easy C\u2212C coupling to produce C\n                    <jats:sub>2<\/jats:sub>\n                    fuels. Therefore, the Pd\u2010ZnO nanosheets realize C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    photosynthesis by atmospheric\u2010concentration CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction with the formation rate of 1.03\u2005\u03bcmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , while the ZnO nanosheets only acquired the carbon monoxide product.\n                  <\/jats:p>","DOI":"10.1002\/anie.202421353","type":"journal-article","created":{"date-parts":[[2024,11,19]],"date-time":"2024-11-19T22:31:22Z","timestamp":1732055482000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":37,"title":["Interface\u2010Engineering\u2010Induced C\u2212C Coupling for C\n                    <sub>2<\/sub>\n                    H\n                    <sub>4<\/sub>\n                    Photosynthesis from Atmospheric\u2010Concentration CO\n                    <sub>2<\/sub>\n                    Reduction"],"prefix":"10.1002","volume":"64","author":[{"given":"Peijin","family":"Du","sequence":"first","affiliation":[{"name":"Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material Engineering Jiangnan University  Wuxi 214122 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinyu","family":"Ding","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material Engineering Jiangnan University  Wuxi 214122 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengyuan","family":"Liu","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at Microscale National Synchrotron Radiation 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