Theoretical screening of bis(iminothiolato)metal monolayers as single-atom electrocatalysts for nitrogen reduction

Abstract

Developing efficient catalysts is essential for the electrocatalytic nitrogen reduction reaction (NRR). Two-dimensional metal–organic frameworks (2D MOFs) have emerged as attractive electrocatalysts due to their intrinsic conductivity and structural tunability. Herein, we systematically investigate the NRR catalytic performance of bis(iminothiolato)metal (TMIT, TM = 3d, 4d, and 5d transition metals) monolayers by means of density functional theory. Through a four-step screening strategy considering stability, N2 adsorption, activity, and selectivity, NbIT and MoIT are identified as the most promising NRR catalysts, exhibiting low limiting potentials of −0.27 and −0.30 V and strong suppression of the competing hydrogen evolution reaction (HER). This work highlights NbIT and MoIT as efficient NRR catalysts and offers valuable insights for the rational design of single-atom catalysts.