CO 2 electroreduction by AuCu bimetallic clusters: A first principles study

The electrocatalytic CO2 reduction reaction (CO2RR) can convert greenhouse gases into high value-added carbon-based fuels and chemicals, providing a sustainable way to solve the energy and environmental crisis. Currently, AuCu bimetallic alloys are attracting attention because of their potential to customize the catalytic activity. In this work, the stability of Au and AuCu bimetallic clusters are systematically studied by first principles calculation. On this basis, the AuCu cluster catalyst is simulated using the density functional theory (DFT) to detect its catalytic activity for the reduction of CO2 to CH3OH. The calculation results show that the AuCu clusters with symmetry have the best stability. Moreover, the doping of Cu atoms in the Au6 cluster can reduce the reaction barrier to a certain extent, thereby accelerating the reaction. Among them, Au1Cu5 and Au2Cu4 cluster catalysts have the most obvious catalytic effects. In the last step, the energy can be reduced by about 2.688 and 5.404 kcal·mol−1, respectively, which can realize the synergistic catalytic effect of Au and Cu on CO2RR. This work can be helpful for the design and preparation of high-efficiency bimetallic cluster catalysts for CO2RR to CH3OH.