High-throughput screening of highly efficient Cu-based dual-atom catalysts to promote nitrate electroreduction for ammonia synthesis: A computational study

Abstract

Nitrate electroreduction to ammonia (NO3ER) holds great promise for producing valuable ammonia and simultaneously solving the nitrate-based environmental concerns, in which searching for highly-efficient catalysts is a crucial issue. Herein, by means of extensive density functional theory (DFT) computations, we explored the potential of a series of Cu-based DACs anchored on two-dimensional boron nitride monolayer with boron vacancy (CuM/BN) as the NO3ER catalysts. Our results revealed that CuMn/BN and CuFe/BN exhibit superior catalytic performance for NO3ER due to their small limiting potentials (-0.27 and -0.32 V) based on a six-step screening strategy. Remarkably, their high NO3ER catalytic activity mainly originates from their optimal binding strength with NO3* intermediate due to their moderate positive charges on the active sites. Our findings not only suggested highly efficient catalysts for advancing sustainable NH3 synthesis, but also proposed a feasible strategy for rapidly screening eligible NO3ER catalysts.