A DFT Screening of Single Transition Atoms Supported on MoS2 as Highly Efficient Electrocatalysts for Nitrogen Reduction Reaction
The development of low-cost and highly efficient materials for electrocatalytical 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 nanosheet (TM@MoS2) was systematically investigated using density function theory (DFT) calculations. It was found that the Re supported on MoS2 (Re@MoS2) has the best NRR catalytic activity with a limiting potential of –0.43 V, along with the high selectivity over the competing hydrogen evolution reaction (HER). Moreover, the ab initio molecular dynamics simulations (AIMD) at 500 K and density of states (DOS) calculations indicated 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 (∆G*NH) was observed, indicating later as a simple descriptor for the facilitated screening of novel SACs. These results pave the way for exploring the novel, highly efficient electrocatalysts for electrochemical NRR under ambient conditions.