Tandem Electroreduction of CO₂ to Programmable Acetate and Syngas via Single-Nickel-Atom-Encapsulated Copper Nanocatalysts

The development of electrocatalysts for converting CO2 to controllable chemicals would meet the strategic requirements, yet remains a great challenge. Herein, a cost-effective tandem catalyst based on Ni single-atom-encapsulated Cu NPs is developed for efficient electroreduction of CO2 (CO2RR) to acetate and syngas in a programmable manner. The operando infrared spectra and density functional theory calculations reveal that the high CO coverage constructed by Ni single atoms could provide favorable conditions for the C–C coupling on the adjacent Cu NPs dominated by the (111) facet and further facilitate the generation of acetate. Moreover, the as-prepared tandem catalyst can also facilitate the formation of syngas (H2/CO) in a wide range from 0.06:1 to 19.5:1 for different application scenarios. Our tandem strategy is expected to contribute to promoting the high single-C2 selectivity liquid fuel output, and facilitating the potential adaption of CO2RR to syngas-mediated thermocatalytic processes for the industrial production.