Computational screening of two-dimensional conductive metal–organic frameworks as electrocatalysts for the nitric oxide reduction reaction

Abstract

The electrocatalytic reduction of nitric oxide (NORR) is an effective and economical method to eliminate NO by converting it into valuable ammonia (NH₃). However, exploring and screening suitable catalysts with both high activity and selectivity remain a great challenge. Herein, we systematically study the potential of two-dimensional conductive metal–organic frameworks (2D c-MOFs), namely, TM₃(C₆O₆)₂ monolayers (TM = transition metals from group 3 to 11) as single-atom catalysts toward NO-to-NH₃ conversion. Among the 25 candidates, Mo₃(C₆O₆)₂ with high stability, activity, and selectivity was successfully screened out through a four-step screening strategy and high-throughput first principles calculations. In particular, the Gibbs free energy of NO (ΔG_*NO) is applied as an effective descriptor for potential NORR catalysts. This work not only provides an effective strategy to screen out TM₃(C₆O₆)₂ for electrochemical NO-to-NH₃ conversion, but also opens a new avenue for designing high-performance 2D c-MOFs towards the NORR.