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Here, we report a Z\u2010scheme CuWO\n                    <jats:sub>4<\/jats:sub>\n                    \/poly(heptazine imide) heterojunction featuring asymmetric Cu\n                    <jats:sup>2+<\/jats:sup>\n                    \/Cu\n                    <jats:sup>+<\/jats:sup>\n                    dual sites for CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010ethanol conversion. Site\u2010selective oxygen vacancies in CuWO\n                    <jats:sub>4<\/jats:sub>\n                    trigger generation of structurally identical, charge\u2010asymmetric neighboring Cu sites, which enhance CO\n                    <jats:sub>2<\/jats:sub>\n                    activation and stabilize adjacent *CO intermediates, thereby facilitating C\u2500C bond formation. Meanwhile, an atomically bonded O\u2500W\u2500N heterointerface enables directional Z\u2010scheme charge transfer, supplying photogenerated electrons to the CuWO\n                    <jats:sub>4<\/jats:sub>\n                    surface and stabilizing the asymmetric Cu\n                    <jats:sup>2+<\/jats:sup>\n                    \/Cu\n                    <jats:sup>+<\/jats:sup>\n                    dual sites throughout photocatalysis. Consequently, the optimized photocatalyst achieves an ethanol production rate of 244.5 \u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in pure water without sacrificial reagents. Advanced synchrotron spectroscopies identify the asymmetric Cu\n                    <jats:sup>2+<\/jats:sup>\n                    \/Cu\n                    <jats:sup>+<\/jats:sup>\n                    dual sites and the chemically bonded heterointerface, while operando spectroscopies record the dynamic evolution of active sites and the\n                    <jats:sup>*<\/jats:sup>\n                    CO\u2500\n                    <jats:sup>*<\/jats:sup>\n                    CO coupling pathways upon illumination. Density functional theory calculations reveal that the synergy between asymmetric catalytic centers and the atomically bonded heterointerface promotes the C\u2500C coupling process. This work establishes a strategy for constructing and stabilizing asymmetric catalytic centers through atomic engineering of crystal structure and heterointerface, providing a photocatalyst design paradigm for selective multicarbon solar fuel synthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.3155700","type":"journal-article","created":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T05:49:43Z","timestamp":1791870583000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Z\u2010Scheme CuWO\n                    <sub>4<\/sub>\n                    \/Poly(heptazine imide) Interface Coupled With Asymmetric Cu\n                    <sup>2+<\/sup>\n                    \/Cu\n                    <sup>+<\/sup>\n                    Sites Enables Efficient Photocatalytic CO\n                    <sub>2<\/sub>\n                    \u2010to\u2010Ethanol Conversion"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-5563-4884","authenticated-orcid":false,"given":"Jiaming","family":"Wu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, Frontier Science Center For Smart Materials, PSU\u2010DUT Joint Center For Energy Research, School of Chemical Engineering Dalian University of Technology  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Dong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, Frontier Science Center For Smart Materials, PSU\u2010DUT Joint Center For Energy Research, School of Chemical Engineering Dalian University of Technology  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0467-6684","authenticated-orcid":false,"given":"Keyan","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, Frontier Science Center For Smart Materials, PSU\u2010DUT Joint Center For Energy Research, School of Chemical Engineering Dalian University of Technology  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9736-975X","authenticated-orcid":false,"given":"Lei","family":"Luo","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals, Frontier Science Center For Smart Materials, PSU\u2010DUT Joint Center For Energy Research, School of Chemical Engineering Dalian University of Technology  Dalian 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