Electrocatalytic nitrogen fixation performance of two-dimensional Metal-Organic Frameworks Cu3(C6O6) and TM/Cu3(C6O6) from first-principle study

Electrochemical nitrogen reduction reaction can convert N2 into NH3 under ambient conditions, which is a friendly method of ammonia synthesis. Many studies have shown that two-dimensional Metal-Organic Framework (2D-MOF) materials have potential applications in the field of catalysis. In this paper, we systematically studied different single-atom catalysts (SACs) TM/Cu3(C6O6) by the density functional theory (DFT), and screened out two suitable candidate catalysts. Fe/Cu3(C6O6) and Co/Cu3(C6O6) catalysts have the excellent catalytic activity with the limiting potentials of −0.92 V and −0.97 V respectively. And it reveals that doping transition metal atoms can effectively improve the catalytic activity of Cu3(C6O6). Interestingly, we analyzed the electronic band structures and the density of state (DOS) of the catalysts, the results show that they have metallic properties and have good electrical conductivity. Therefore, Fe/Cu3(C6O6) and Co/Cu3(C6O6) are promising catalysts for NRR. Our study provides a new idea for the design of high-efficiency nitrogen reduction catalysts.