Establishing the Principal Descriptor for Electrochemical Urea Production via the Dispersed Dual‐Metals Anchored on the N‐Decorated Graphene

Abstract Urea electrosynthesis under mild conditions starting from the adsorption of inert N 2 molecules has brought out a promising alternative experimentally to conquer its huge energy consumption in industrial Haber‐Bosch process. The most crucial and inevitable reaction is the formation of urea precursor *NCON from *N 2 and CO based on the pre‐selected reaction pathway, together with the following protonated processes. It is significant to comprehend their intrinsic intercorrelation and explore the principal descriptor from massive reaction data. Hereby, the authors study the dispersed dual‐metals (homonuclear MN 3 –MN 3 moiety and heteronuclear MN 3 –M'N 3 moiety) anchored on N‐doped graphene as electrocatalysts to synthesize urea. Based on the screened out 72 stable systems by ab initio molecular dynamics (AIMD) simulations as the database, six significant linear correlations between the computed Gibbs free energy and other important factors are achieved. Most encouragingly, the principal descriptor (Δ E (*NCONH)) is established because 72% low‐performance systems can be filtered out and its effective range (−1.0 eV < Δ E E(*NCONH) < 0.5 eV) is identified by eight optimal systems. This study not only suggests that dispersed dual‐metals via MN 3 moiety can serve as promising active sites for urea production, but also identifies the principal descriptor and its effective range in high‐throughput methods.