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In this study, we develop a de novo coordination\u2010site and geometry engineering strategy to construct high\u2010density proximal Cu SACs for improving CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010C\n                    <jats:sub>2+<\/jats:sub>\n                    electroreduction. Flexible molecular building blocks rich in N\/O coordination motifs assemble into wrinkled 2D networks and further hierarchically organize into a 3D nanoflower framework, where isolated Cu sites with high loading of 14 wt% are anchored via robust N\/O coordination. The structural bending brings adjacent Cu atoms into close proximity (\u223c2.6 \u00c5). Competitive N\/O coordination generates asymmetric and low\u2010coordinated microenvironments, promoting *CO intermediate stabilization and subsequent C\u2500C coupling. The optimized catalyst achieves a C\n                    <jats:sub>2+<\/jats:sub>\n                    Faradaic efficiency of 81.34% at 500 mA\u00b7cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , including 51% ethylene selectivity, with stable operation exceeding 100\u00a0h. This work sheds light on structural dimensional control and microenvironment engineering for promoting cooperative catalysis in single\u2010atom systems, offering new opportunities for efficient multicarbon electrosynthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.9990726","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T13:32:10Z","timestamp":1792071130000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["De Novo Engineering High\u2010Density Proximal Copper Single Atoms for Enhanced C\u2500C Coupling in CO\n                    <sub>2<\/sub>\n                    Electroreduction"],"prefix":"10.1002","author":[{"given":"Qian","family":"Ma","sequence":"first","affiliation":[{"name":"State Key Laboratory of Green and Efficient Development of Phosphorus Resources School of Chemical Engineering and Pharmacy Wuhan Institute of Technology  Wuhan Hubei P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-3082-7884","authenticated-orcid":false,"given":"Fanpeng","family":"Cheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Green and Efficient Development of Phosphorus Resources School of Chemical Engineering and Pharmacy Wuhan Institute of Technology  Wuhan Hubei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingyue","family":"Qiu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Green and Efficient Development of Phosphorus Resources School of Chemical Engineering and Pharmacy Wuhan Institute of Technology  Wuhan Hubei P. R. 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