Urea Synthesis from N₂ and CO₂ over Dual-Atom Catalysts: A High-Throughput Computational Insight

The simultaneous electrocatalytic conversion of N2 and CO2 into value-added urea is a promising approach to utilizing CO2 as a feedstock for the sustainable production of chemicals. Designing cost-effective electrocatalysts for simultaneous activation of N2 and CO2 on distinct active sites is challenging due to the inertness of N2 and the competing reduction of CO2 to other products. To address this, we systematically designed various dual-atom anchored on two-dimensional C2N and found that the presence of dual metal atoms on the C2N generates excess surface-charge density, favoring the activation of CO2 and N2. The screening results demonstrate that ReV@C2N is the optimal candidate for driving the urea synthesis, as it facilitates stable binding of both N2 and CO2. This could be attributed to the presence of dual metal atoms on C2N, which generate excess surface-charge density that favors the activation of CO2 and N2. In addition, we have thoroughly investigated the C–N coupling process. This observation can be explained by the spontaneous coupling of the obtained CO moiety into the activated N–N bond to form NCON, which is driven by the thermodynamic driving force and orbital overlap of the adsorbed N2 and CO.