Abundant (110) Facets on PdCu₃ Alloy Promote Electrochemical Conversion of CO₂ to CO

Electrochemical conversion of CO₂ to high-value chemical fuels offers a promising strategy for managing the global carbon balance but faces huge challenges due to the lack of effective electrocatalysts. Here, we reported PdCu₃ alloy nanoparticles with abundant exposed (110) facets supported on N-doped three-dimensional interconnected carbon frameworks (PdCu₃/NC) as an efficient and durable electrocatalyst for electrochemical CO₂ reduction to CO. The catalyst exhibits extremely high intrinsic CO₂ reduction selectivity for CO production with a Faraday efficiency of nearly 100% at a mild potential of -0.5 V. Moreover, a rechargeable high-performance Zn-CO₂ battery with PdCu₃/NC as a cathode is developed to deliver a record-high energy efficiency of 99.2% at 0.5 mA cm^-2 and rechargeable stability of up to 133 h. Theoretical calculations elucidate that the exposed (110) facet over PdCu₃/NC is the active center for CO₂ activation and rapid formation of the key *COOH intermediate.