A Cu-based electrocatalyst (-CuSi) is developed by exsolving ultrathin SiO layer-coated CuO/Cu nanoparticles (<100 nm) on the surface of a conductive intermetallic CuSi parent. This specially designed -CuSi catalyst exhibits high performance for the CO reduction reaction (CORR), which affords an excellent CH faradaic efficiency (FE) of 49.0% with partial current density of over 140.1 mA cm at -1.2 V reversible hydrogen electrode (RHE) in a flow cell, with outstanding stability. The strongly coupled multiphase interfaces among the SiO layer, CuO/Cu species, and substrate contribute to fast interfacial electron transfer for the CORR. Moreover, Raman analysis suggests that the ultrathin SiO layer simultaneously stabilizes the active Cu species and promotes the protonation of *CO to form *CHO, thereby greatly improving overall selectivity and activity of CH production.
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