Selective bimetallic sites supported on graphene as a promising catalyst for CO2 Reduction: A first-principles study

Developing efficient and inexpensive electrocatalysts for CO2 reduction reaction (CRR) has been a key scientific issue. Several factors limit the electrocatalyst efficiency of materials, including the relatively high overpotential, low stability and low selectivity for CRR. The use of bimetallic catalyst systems is an efficient approach to improve the catalytic performance. In this study, by using the density functional theory (DFT) calculations, we explore the CRR processes of three different bimetal doped graphenes (M1M2/DG (M1, M2 = Cu, Fe, Ni)). Various reduction reaction pathways of CO2 lead to different products, including CH4, CH3OH, HCOOH and CO. The Eads of different intermediates on different M1M2/DG, the free energy variation and the overpotential of the different M1M2/DG were analyzed. The obtained results confirm the CO2 capture ability of all the studied M1M2/DG systems. The low overpotential of 0.49 V for Cu_Ni/DG is even lower than that of the most outstanding metallic electrocatalyst (Cu (2 1 1)). This work provides useful information for the development of efficient CRR electrocatalysts.