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Single\u2010atom alloys (SAAs), in which isolated dopants are incorporated into a Cu host, offer an atomic\u2010scale platform to modulate surface chemistry. Here we report a systematic theoretical investigation of 29 Cu\u2010based SAAs, combining grand\u2010canonical density functional theory, surface Pourbaix diagrams, and constant\u2010potential ab initio molecular dynamics with explicit solvation. We uncover a general non\u2010monotonic periodic trend in adsorbate binding strength\u2014strong \u2192 weak \u2192 strong\u2014arising from dopant\u2010induced perturbations of the Cu electronic structure. This universal trend provides a guiding principle: asymmetric active sites, formed by the coexistence of strong\u2010 and weak\u2010binding motifs, enable more favorable *CO\u2013*CO coupling and thereby enhance selectivity toward C\n                    <jats:sub>2\u207a<\/jats:sub>\n                    products. Importantly, we identify net electron transfer from dopant to host as an effective and easily computable descriptor for rapidly screening SAA candidates with low C\u2500C coupling barriers. Guided by this framework, we highlight ScCu, VCu, ZrCu, NbCu, and TaCu as promising SAAs, exhibiting suppressed hydrogen evolution, electrochemical robustness, and efficient C\u2500C bond formation. In particular, NbCu(111) displays a low C\u2500C coupling barrier of 0.87\u00a0eV and a thermodynamically viable pathway to ethanol, confirmed under realistic electrolyte conditions. These findings establish atomic\u2010scale asymmetry as a general design paradigm for advancing SAAs catalysts in CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction.\n                  <\/jats:p>","DOI":"10.1002\/anie.202520426","type":"journal-article","created":{"date-parts":[[2025,11,27]],"date-time":"2025-11-27T06:28:01Z","timestamp":1764224881000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["From Dopant Periodicity to Asymmetric Sites: Steering C\u2500C Coupling in Single\u2010Atom Alloy Catalysts for Electrochemical CO\n                    <sub>2<\/sub>\n                    Reduction"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1520-2847","authenticated-orcid":false,"given":"Tianwei","family":"He","sequence":"first","affiliation":[{"name":"Yunnan Key Laboratory for Micro\/Nano Materials &amp; Technology National Center for International Research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University  Kunming 650091 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rongxing","family":"Sun","sequence":"additional","affiliation":[{"name":"Yunnan Key Laboratory for Micro\/Nano Materials &amp; Technology National Center for International Research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University  Kunming 650091 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ran","family":"Shi","sequence":"additional","affiliation":[{"name":"Yunnan Key Laboratory for Micro\/Nano Materials &amp; Technology National Center for International Research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University  Kunming 650091 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinqi","family":"Chen","sequence":"additional","affiliation":[{"name":"Yunnan Key Laboratory for Micro\/Nano Materials &amp; Technology National Center for International Research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University  Kunming 650091 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tong","family":"Zhou","sequence":"additional","affiliation":[{"name":"Yunnan Key Laboratory for Micro\/Nano Materials &amp; Technology National Center for International Research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University  Kunming 650091 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yun","family":"Han","sequence":"additional","affiliation":[{"name":"Queensland Micro\u2010 and Nanotechnology Centre School of Engineering and Built Environment Griffith University  Nathan Campus QLD 4111 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feng","family":"Liu","sequence":"additional","affiliation":[{"name":"Yunnan Precious Metals Laboratory Co., Ltd  Kunming Yunnan 650106 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Cui","sequence":"additional","affiliation":[{"name":"Yunnan Precious Metals Laboratory Co., Ltd  Kunming Yunnan 650106 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haobo","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingju","family":"Liu","sequence":"additional","affiliation":[{"name":"Yunnan Key Laboratory for Micro\/Nano Materials &amp; Technology National Center for International Research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University  Kunming 650091 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,11,26]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010025\u201008692\u2010x"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010023\u201006321\u2010z"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adn3441"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010024\u201007322\u20102"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010023\u201006917\u20105"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2019.12.015"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1039\/c0ee00071j"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c09079"},{"key":"e_1_2_7_9_1","first-page":"12044","volume":"120","author":"Hannagan R. 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