Theoretical Investigation of Single and Double Transition Metals Anchored on Graphyne Monolayer for Nitrogen Reduction Reaction

Abstract

In contrast to the energy-extensive Haber–Bosch process, green production of ammonia (NH3) at ambient conditions remains as one of the main goals of the 21st century. In this work, we systematically studied single and double transition metal atoms (Fe, Co, Mo, Ru) anchored on graphyne (GY) for nitrogen (N2) reduction by means of density functional theory (DFT). We demonstrated that Ru dimer anchored on two-dimensional (2D) GY exhibits superior catalytic activity for nitrogen reduction via an enzymatic pathway with the maximum free energy change (ΔG) of 0.43 eV. Our findings propose highly reactive catalytic materials for efficient N2 reduction while highlighting the importance of double-atom catalysts for nitrogen reduction reaction (NRR).