Single metal atom anchored on porous boron nitride nanosheet for efficient collaborative urea electrosynthesis: A computational study

Urea electrosynthesis under ambient conditions has been emerging as a sustainable strategy to replace the harsh industrial process, in which the activation of the inert N2 molecule and the then CN coupling still remain the huge challenge due to the lack of advanced electrocatalysts with multiple active sites. Here, by means of density functional theory (DFT) computations, a new family of electrocatalysts with asymmetrical triple active sites was proposed to boost urea production by anchoring single metal atoms on porous boron nitride nanosheet with divacancy (M/p-BN). Through the high-throughput screening, we found that the anchored Fe and Co atoms exhibit satisfied catalytic activity for urea formation with low limiting potentials, moderate kinetic barriers for CN coupling reaction, and excellent suppressing effect on the side reactions, in which Fe/Co and their adjacent two B atoms perform as collaborative adsorption sites. Furthermore, the high activity of the two promising catalysts can be well rationalized by their optimal binding strength with the NCON* species, which is mainly determined by the intrinsic charge distribution on the active sites. This work suggested that the anchoring of a single metal atom can highly activate BN nanosheet to achieve multiple active sites, which opens a new avenue to develop novel and efficient catalysts for other electrocatalytic reactions.