Theoretical scanning of bimetallic alloy for designing efficient N2 electroreduction catalyst

Nitrogen reduction conversion into ammonia has received considerable attention and shown application potential in materials science. This work presents the results of theoretical scanning based on comprehensive first principle calculations of bimetallic alloys with the general formula MN, where M and N are transition metals that can be used as electrocatalysts for high-performance N2 reduction. To date, no detailed reaction mechanism has been verified for the production rates in commercial applications. This work of calculations reveals that N2 can be reduced to ammonia (NH3) on palladium-gold (PdAu) and copper-tin (CuSn) bimetallic alloy catalysts with a relatively low limiting potential and activation barrier compared with other bimetallic alloy catalysts. The nitrogen reduction reaction is highly selective and active compared to the competitive hydrogen evolution reaction (HER). This work provides promising guidance for designing efficient single-atom catalysts for the electroreduction of N2. Nickel-cerium (NiCe) bimetallic alloy catalyst was found to have a low activation energy of 0.49 eV during the third hydrogenation step. Scaling relationships were found to exist between the binding energy and limiting potential of NxHy intermediate species in each elementary step on the bimetallic alloy surfaces. This work also provides a promising way to explore and design efficient N2 reduction reaction (NRR) catalysts and identify the reaction mechanism for improving and controlling catalytic performance in practical applications.