Abstract:
To evaluate the electrocatalytic performance of single-layer C
2N with single Cu and double Cu atoms, this paper systematically explores the electrocatalytic properties of Cu@C
2N and Cu
2@C
2N by using first-principles method based on density functional theory. Compared to loaded single Cu atom catalysts, dual atom doping increases the adsorption strength of O
2 and oxygen-containing intermediates on Cu atoms by changing their adsorption configurations, significantly enhancing the electrocatalytic activity of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The ORR and OER overpotentials of the Cu
2@C
2N can reach 0.46 and 0.38 V, respectively, which is comparable to that of precious metal catalysts and is a promising candidate material to replace precious metal electrocatalysts. The calculation of electronic state density shows that the Cu atom loaded at the Fermi energy level introduces a higher electronic state density while effectively reducing the band gap width, and Cu
2@C
2N has a smaller band gap than Cu@C
2N, which is beneficial for it to obtain higher carrier concentration and conductivity, thus achieving better electrocatalytic activity.