Urea Synthesis from N<sub>2</sub> and CO<sub>2</sub> over Dual-Atom Catalysts: A High-Throughput Computational Insight
Chaozhen Liu, Feng Gong, Qiang Zhou, Yunlong Xie
Abstract
The simultaneous electrocatalytic conversion of N 2 and CO 2 into value-added urea is a promising approach to utilizing CO 2 as a feedstock for the sustainable production of chemicals. Designing cost-effective electrocatalysts for simultaneous activation of N 2 and CO 2 on distinct active sites is challenging due to the inertness of N 2 and the competing reduction of CO 2 to other products. To address this, we systematically designed various dual-atom anchored on two-dimensional C 2 N and found that the presence of dual metal atoms on the C 2 N generates excess surface-charge density, favoring the activation of CO 2 and N 2 . The screening results demonstrate that ReV@C 2 N is the optimal candidate for driving the urea synthesis, as it facilitates stable binding of both N 2 and CO 2 . This could be attributed to the presence of dual metal atoms on C 2 N, which generate excess surface-charge density that favors the activation of CO 2 and N 2 . 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 N 2 and CO.