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However, it remains a grand challenge to achieve a high ethanol yield due to the difficulty in accurate control of CO\n                    <jats:sub>2<\/jats:sub>\n                    activation and C\u2013C coupling under thermocatalytic reaction conditions. Herein, a precise rhodium (Rh) single\u2010cluster catalyst on carbon nitride support (Rh\n                    <jats:sub>SC<\/jats:sub>\n                    \/CN) was designed for CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation to ethanol. The Rh\n                    <jats:sub>SC<\/jats:sub>\n                    \/CN catalyst, with an average Rh\u2013Rh coordination number of 2.06, exhibits a record turnover frequency (TOF\n                    <jats:sub>Rh<\/jats:sub>\n                    ) of 595.2\u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , a high ethanol selectivity of 95.3% and an ethanol yield of 17.5\u00a0mmol g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 240\u00a0\u00b0C and 5.0\u00a0MPa (H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2\u00a0<\/jats:sub>\n                    =\u00a03), surpassing previously reported Rh\u2010based catalysts. Density functional theory calculations, in situ diffuse reflectance infrared Fourier transform spectroscopy, X\u2010ray absorption spectroscopy and H\n                    <jats:sub>2<\/jats:sub>\n                    \/D\n                    <jats:sub>2<\/jats:sub>\n                    isotope exchange probing experiments altogether reveal the reaction mechanism, and show that the synergetic interaction between Rh\u2013Rh and Rh\u2013N sites boosts CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption and asymmetric C\u2013C coupling between CH\n                    <jats:sub>3<\/jats:sub>\n                    * and CO* to form CH\n                    <jats:sub>3<\/jats:sub>\n                    CO*, leading to a high ethanol selectivity. This discovery provides new insights into the design of single\u2010cluster catalysts for simultaneously promoting CO\n                    <jats:sub>2<\/jats:sub>\n                    reactivity and ethanol\u00a0selectivity.\n                  <\/jats:p>","DOI":"10.1002\/anie.202516545","type":"journal-article","created":{"date-parts":[[2025,9,25]],"date-time":"2025-09-25T10:26:38Z","timestamp":1758795998000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Construction of Single\u2010Cluster Rhodium Catalyst for Efficient CO\n                    <sub>2<\/sub>\n                    Hydrogenation to Ethanol"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9360-5150","authenticated-orcid":false,"given":"Hao","family":"Wang","sequence":"first","affiliation":[{"name":"Center for Low\u2010Carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences  Shanghai 201210 P.R. 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