Theoretical insights into transition metal clusters supported on graphyne as electrocatalysts for N2–to–NH3 conversion

Abstract

NH3 is not only an important energy intermediates and carbon-free energy carrier, but also essential for various production and life processes. Under ambient conditions, electrocatalytic nitrogen reduction reaction (NRR) is considered to be a very attractive approach, the process converts clean electrical energy into chemical energy, and realizes the efficient use and conversion of renewable energy, which is of great significance in energy and environmental protection. In this study, density functional theory was applied to transition metal clusters supported on graphyne as electrocatalysts (TM3@GY) to realize the NRR process. The effects of cluster types and doping atoms on catalytic performance were systematically studied. Finally, Fe3@BGY was selected as a potential NRR catalytic system with an initial potential of −0.560 V. The reason of the high catalytic activity was revealed through the calculation of electronic properties, which provides a theoretical basis for designing new high-performance cluster catalysts.