High-Throughput Screening of Nitrogen Reduction Reaction on Single Atom@1T'-MoS2

Abstract

Electrochemical synthesis of ammonia through nitrogen reduction reaction (NRR) is cost-effective and energy-effective compared to the conventional Haber-Bosch process. However, the slow activation kinetics of N2 hindered the development of active and selective catalysts. In this work, we showed that transition metal (TM) single atoms anchored on monolayer molybdenum disulfide (MoS2) with 1T phase could promote its phase transition to 1T' due to broken surface symmetry induced by TM atoms. By combining the high-throughput screening with DFT calculations in transition metals, two TM elements (V, Ti) anchored on 1T'-MoS2 were proved to be promising candidates in N2 fixation. The V and Ti single-atom catalyst exhibits low Gibbs free energy barrier, and Ti single-atom catalyst shows the highest selectivity towards NH3. Moreover, the stability of single-atom TM@1T'-MoS2 was measured with the ab initio molecular dynamics (AIMD) simulations. The density of states (DOS) and surface charge analysis were conducted to reveal the origin of improved activities. Our results pave the way to design more innovative single-atom catalysts for high-performance electrocatalytic NRR.