Atomically dispersed copper catalysts for highly selective CO2 reduction

Support substrates play important roles in the catalysis process. Herein, atomically dispersed CuN3 catalysts supported by two different types of zirconia (denoted as CuN3/NC/T-ZrO2 and CuN3/NC/M-ZrO2) have been rationally fabricated to uncover the influence of the support. CuN3/NC/T-ZrO2 exhibits outstanding performance for electrochemical CO2 reduction towards CO at a wide range of potentials (similar to 96%, 0.6-0.8 V vs. RHE) owing to the acidic uncoordinated Zr4+ sites of T-ZrO2, which facilitate CO2 accumulation, and N-doped carbon (NC), which enhances the conductivity of the catalyst. Moreover, density functional theory calculations prove that T-ZrO2 effectively decreases the Gibbs free energy for CO2 to CO conversion. Significantly, this study reports the effects of the substrate on the electrocatalytic CO2RR and provides a promising strategy for tuning catalytic activity and selectivity during the process of converting CO2 into high-value products by controlling the phase of the support for the first time.