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While halide species, such as chlorine, promote CO\n                    <jats:sub>2<\/jats:sub>\n                    activation, and silane\u2010based modifiers can regulate charge transfer to enhance C\u2013C dimerization, these effects are typically decoupled when applied separately. Herein, we identify 3\u2010chloropropyltrimethoxysilane (CPTMS) as a molecular modifier that integrates halide functionality and silane anchoring within one scaffold, enabling spatially coupled regulation of CO\n                    <jats:sub>2<\/jats:sub>\n                    RR intermediates at the Cu interface. Introduced via a one\u2010step electrodeposition strategy, the CPTMS\u2010modified Cu catalyst exhibits a 5\u2010fold enhancement in C\n                    <jats:sub>2+<\/jats:sub>\n                    faradaic efficiency, reaching 75% \u00b1 2% compared with 15% \u00b1 4% for unmodified CuO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    at \u22121.5\u00a0V vs. the reverse hydrogen electrode\u00a0with a partial current density of 105\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . In\u2010situ synchrotron\u2010based Fourier transform infrared reveals that the spatially coupled chlorine and silicon functionalities sequentially optimize the CO\n                    <jats:sub>2<\/jats:sub>\n                    RR pathway by promoting CO\n                    <jats:sub>2<\/jats:sub>\n                    activation, *COOH formation, *CO protonation, and subsequent C\u2013C dimerization on Cu active sites achieving enhanced C\n                    <jats:sub>2+<\/jats:sub>\n                    product formation. This work elucidates molecularly integrated halide\u2010silane functionalization\u2010enabled synergistic interfacial control, offering a rational design strategy for advancing selective C\n                    <jats:sub>2+<\/jats:sub>\n                    product formation in CO\n                    <jats:sub>2<\/jats:sub>\n                    RR.\n                  <\/jats:p>","DOI":"10.1002\/advs.76741","type":"journal-article","created":{"date-parts":[[2026,7,24]],"date-time":"2026-07-24T12:28:02Z","timestamp":1784896082000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Chlorine\u2010Functionalized Silane\u2010Modified Copper Electrocatalyst for Enhanced CO\n                    <sub>2<\/sub>\n                    Reduction to Multi\u2010Carbon Products"],"prefix":"10.1002","volume":"13","author":[{"given":"Ying Ying","family":"Ch'ng","sequence":"first","affiliation":[{"name":"School of Chemical Engineering The 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