Atomically dispersed copper catalysts for highly selective CO2 reduction

Abstract

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 (∼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.