Abstract

Tandem electrocatalysis is an emerging concept for effective electrochemical CO2 reduction reaction (CO2RR) towards multicarbons (C2+). This decouples the multiple steps of CO2-to-C2+ into two steps of CO2-to-CO and CO-to-C2+ catalyzed by individual catalysts, to improve the Faradic efficiency (FE). However, due to the mass-transport limitation of CO from the generation site to the long-distance consumption site, such a strategy still remains challenge for high-rate production of C2+ products. Herein, we designed CuO/Ni single atoms tandem catalyst, which made the catalytic sites of Ni and Cu for independently catalyzing CO2-to-CO and CO-to-C2+ compactly neighbored, enabling the in-situ generation and rapid consumption of CO. The CuO/Ni SAs tandem catalyst achieved a particularly high partial current density of C2+ products (1220.8 mA/cm2), while still maintained outstanding C2+ products FE (81.4%) and excellent selectivities towards ethylene (FE 54.1%) and ethanol (FE 28.8%), enabling the profitable production of multicarbons by CO2RR.

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