Design of Fe₂Mo@γ-GDY triatomic catalyst for electrocatalytic urea synthesis of N₂ and CO: a theoretical study

While urea is widely used as a chemical raw material, its precursor ammonia (NH₃) has traditionally to be synthesized under high-temperature/pressure conditions, leading to not only huge energy consumption, but also serious CO₂ emission. Here, we present a groundbreaking catalyst design approach, which optimizes adsorption configurations and reaction pathways by controlling the adsorption energies of each intermediate in the reaction, thus enhancing catalytic performance. Via density functional theory calculations, we designed a triatomic catalyst (i.e., Fe₂Mo@γ-GDY) with a limiting potential of −0.22 V and a C-N coupling energy barrier of 0.34 eV. Notably, the Fe₂Mo@γ-GDY catalyst presents a high selectivity and robust antioxidation capabilities under applied potentials. Our comprehensive analysis elucidates the affecting factors of limiting potential and C-N coupling energy barrier. These insights significantly contribute to the advancement of catalyst design strategies for electrocatalytic urea synthesis, offering a more efficient and eco-friendlier alternative to the traditional methods.