High-Throughput Screening of Efficient Biatom Catalysts Based on Monolayer Carbon Nitride for the Nitric Oxide Reduction Reaction.

Exploring efficient catalysts for the nitric oxide reduction reaction (NORR) toward NH 3 synthesis is becoming increasingly important for tackling both NH 3 synthesis and NO removal problems. Currently, only a few NORR catalysts have been proposed, which are exclusively concentrated on bulk metals or single-atom catalysts. Here, taking monolayer C 2 N as an example, we explore the potential of biatom catalysts (BACs) for direct NO-to-NH 3 conversion by means of high-throughput first-principles calculations. According to a rational five-step screening strategy, a promising BAC of Cr 2 -C 2 N is successfully screened out, exhibiting high stability, activity, and selectivity and a low kinetic barrier for the NORR toward NH 3 synthesis. Importantly, the adsorption energy of N atoms (Δ E *N ) and the Gibbs free energy of NO adsorption (Δ G *NO ) are identified as effective descriptors for efficient NORR catalysts. In addition, through tuning the NO coverage, the NORR on Cr 2 -C 2 N could produce different products of NH 3 and N 2 O, providing the possibility to realize controllable multiproduct BACs. These findings not only suggest the great potential of BACs for direct NO-to-NH 3 conversion but also help in rationally designing high-performance BACs.