A DFT screening of single transition atoms supported on MoS2 as highly efficient electrocatalysts for the nitrogen reduction reaction. Issue 18 (22nd April 2020)

• Record Type: Journal Article
• Authors: Zhai, Xingwu; Li, Lei; Liu, Xiaoyue; Li, Yafei; Yang, Jueming; Yang, Dezheng; Zhang, Jinli; Yan, Hongxia; Ge, Guixian
• Is Part Of: Nanoscale. Volume 12:Issue 18(2020)
• Page Start: 10035
• Page End: 10043
• Publication Date: 2020-04-22
• Subjects: Nanoscience -- Periodicals; Nanotechnology -- Periodicals; 620.505
• DOI: 10.1039/d0nr00030b
• Languages: English
• ISSNs: 2040-3364

Abstract

Abstract : Re@MoS2 possesses the best NRR catalytic activity with a limiting potential of −0.43 V among TM@MoS2 systems. 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 (Δ G *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.