S site doped-pyrite by single atom for efficiently catalyzing N2 electrochemical reduction

The green electrochemical conversion of N2 to ammonia with low energy consumption has been attractive, but a great challenge remains to find cost-effective and long-term stable catalysts. In this study, we systematically evaluated by DFT the potential of N2 reduction to ammonia catalyzed on pyrite surface doped by different atoms, and we found that ten types of metals/metalloid (Al, Co, Tc, Ru, Mo, Rh, Re, Os, Ir, and As) -doping pyrite surface, with a structure FeMxS2-X@FeS2 (M: the doping atoms), can catalyze N2 reduction under ambient conditions, among which the FeCoxS2-X@FeS2 may be the best catalyst. The results of the electroreduction of N2 to ammonia showed that onto the surface of FeCoxS2-X@FeS2 that was synthesized by a two-step hydrothermal method, the N2 reduction was catalyzed specifically and steadily, with a high NH3 yield rate of 33.5 μg h−1 mg–1cat and Faraday efficiency of 13.6% at − 0.6 V.