Density Functional Theory Study of Nitrogen-doped Graphene as a High-performance Electrocatalyst for CO2RR

Abstract Metal-free catalysts for the CO2 reduction reaction (CO2RR) is a research hotspot to enhance CO2 utilization as a way to counteract global warming. Nitrogen-doped graphene attracts attention because of the abundance of nitrogen and promising catalytic performance of graphene. In this work, we investigated various N-doped configurations and their corresponding catalytic abilities for CO2RR to ethanol via spin-polarized density functional theory (DFT) computations. The final results indicate that site 43 of binary-N-doped graphene had high CO2RR activity, stable adsorption of reactants, and good activation of CO2. The catalysis process demonstrated features of low free energy barriers in the rising stage and obvious facilitation of the potential-limiting step. Compared with a catalyst-free process, it can effectively improve the reaction activity. The results provide theoretical guidance for the design and preparation of high-performance CO2RR catalysts.