A DFT screening of single transition atoms supported on MoS2 as highly efficient electrocatalysts for the nitrogen reduction reaction

Abstract

The development of low-cost and highly efficient materials for the electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is an attractive and challenging topic in chemistry. In this study, the electrocatalytic performance of a series of transition metal (TM) atoms supported on MoS₂ nanosheets (TM@MoS₂) was systematically investigated using density functional theory (DFT) calculations. It was found that Re supported on MoS₂ (Re@MoS₂) has the best NRR catalytic activity with a limiting potential of −0.43 V, along with high selectivity over the competing hydrogen evolution reaction (HER). Moreover, the ab initio molecular dynamics (AIMD) simulations at 500 K and density of states (DOS) calculations indicated the high thermodynamic stability and excellent electrical conductivity of Re@MoS₂. A linear trend between several parameters of single atom catalysts (SACs) and the adsorption Gibbs free energy change of the NH species (ΔG_*NH) was observed, indicating the later as a simple descriptor for the facilitated screening of novel SACs. These results pave the way for exploring novel, highly efficient electrocatalysts for the electrochemical NRR under ambient conditions.