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.