Work

Electrochemical synthesis of urea at cooperative active sites on Mo2C grain boundary

Year: 2025

Type: article

Abstract: The design of multiple types of active sites with cooperative functions on catalyst surface holds great promise for urea synthesis , yet forming these specific sites and ensuring their functionality remain a prominent challenge. Here, we propose two types of Mo 2 C grain boundaries (GBs) that feature intrinsic cooperative active sites, facilitating the coupling of C and N species and achieving efficient urea synthesis. By density-functional theory (DFT) calculations, we verify that positively charged Mo atoms on the GBs exhibit high adsorption and reduction activity for CO 2 , whereas adjacent Mo atoms contribute to the activation of N 2 or NO . The cooperative effects of these active sites enables C-N coupling to proceed spontaneously on the GBs with ultralow limiting potentials (−0.24 ∼ −0.42 V). Furthermore, analysis of the competing hydrogen evolution reaction and nitrogen reduction reaction confirms the high selectivity to generate urea on Mo 2 C GBs. Our work demonstrates GB engineering as a promising strategy for urea generation through the synergistic cooperation between multiple active sites, thus paving the way towards the rational design of effective catalysts for urea electrosynthesis.

Source: Journal of Catalysis

DOI: 10.1016/j.jcat.2025.116139