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Here, we show that pulsed operation does not preserve the as\u2010prepared Cu\u2010Ag catalyst and instead generates a dynamic bimetallic working state in situ. During prolonged electrolysis, the catalyst evolves toward a favorable selectivity profile with significantly increased CO formation, persistent ethylene production, and suppressed hydrogen, methane, and formate pathways. Correlative SEM\/EDS, XPS, ToF\u2010SIMS, ICP\u2010MS, and STEM\u2010EELS show that this behavior arises from Ag\u2010modulated Cu dissolution and redeposition under pulsed conditions. The resulting catalyst develops near\u2010surface Ag enrichment, a topmost catalytically relevant layer containing both Cu and Ag, persistent Cu loss to the electrolyte, and subsurface cavities. Comparison with pure Cu under identical pulsed conditions further shows that Ag redirects the restructuring pathway of Cu toward a distinct Ag\u2010rich yet still Cu\u2010active catalytic state. Under pulsed CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction, Ag therefore acts as a tandem component for CO formation and as a regulator of catalyst evolution.\n                  <\/jats:p>","DOI":"10.1002\/smll.75324","type":"journal-article","created":{"date-parts":[[2026,8,29]],"date-time":"2026-08-29T15:40:06Z","timestamp":1788018006000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Silver\u2010Modulated Copper Dynamics Under Pulsed Tandem Electrochemical CO\n                    <sub>2<\/sub>\n                    Reduction"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-5644-3190","authenticated-orcid":false,"given":"Bla\u017e","family":"Tomc","sequence":"first","affiliation":[{"name":"Department of Materials Chemistry National Institute of Chemistry  Ljubljana Slovenia"},{"name":"University of Nova Gorica  Nova Gorica 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