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5. Mo₂P Monolayer as a Superior Electrocatalyst for Urea Synthesis from Nitrogen and Carbon Dioxide Fixation: A Computational Study

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   Urea synthesis through the simultaneous electrocatalytic reduction of N₂and CO₂molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production, in which the development of stable, highly efficient, and highly selective catalysts to boost the chemisorption, activation, and coupling of inert N₂and CO₂molecules remains rather challenging. Herein, by means of density functional theory computations, we proposed a new class of two‐dimensional nanomaterials, namely, transition‐metal phosphide monolayers (TM₂P, TM = Ti, Fe, Zr, Mo, and W), as the potential electrocatalysts for urea production. Our results showed that these TM₂P materials exhibit outstanding stability and excellent metallic properties. Interestingly, the Mo₂P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier (0.35 eV) for C–N coupling, low limiting potential (−0.39 V), and significant suppressing effects on the competing side reactions. The outstanding catalytic activity of the Mo₂P monolayer can be ascribed to its optimal adsorption strength with the key *NCON species due to its moderate positive charges on the Mo active sites. Our findings not only propose a novel catalyst with high‐efficiency and high‐selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis. 

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