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Abstract Electrocatalytic conversion of nitrates and carbon dioxide to urea under ambient conditions shows promise as a potential substitute for traditional urea synthesis processes characterized by high consumption and pollution. In this study, a straightforward one‐pot method is employed to prepare a highly efficient FeNC‐Fe 1 N 4 electrocatalyst, consisting of atomically dispersed Fe 1 N 4 sites and metallic Fe clusters (FeNC) with particle size of 4–7 nm. The FeNC‐Fe 1 N 4 catalyst exhibits remarkable electrocatalytic activity for urea synthesis from nitrate anion (NO 3 − ) and carbon dioxide (CO 2 ), achieving a urea production rate of 38.2 mmol g cat −1 h −1 at −0.9 V (vs RHE) and a Faradaic efficiency of 66.5% at −0.6 V (vs RHE). Both experimental and theoretical results conclusively demonstrate that metallic Fe clusters and Fe 1 N 4 species provide active sites for the adsorption and activation of NO 3 − and CO 2 , respectively, and the synergistic effect between Fe 1 N 4 and metallic Fe clusters significantly enhances the electrochemical efficiency of urea synthesis. In all, this work contributes to the rational design and comprehensive synthesis of a dual‐active site iron‐based electrocatalyst, facilitating efficient and sustainable urea synthesis.
Li et al. (Wed,) studied this question.