▎ 摘　　要

Ammonia is an indispensable component for the development of human society due to its widespread applications and because it is an excellent source of energy. Chemists are looking for a viable catalyst for the activation of N-2 molecule to subsequently synthesize ammonia. In this theoretical work, we have used [Co(N-2)((PNP)-P-R)] (R = tBu, (PNP)-P-tBu = 2,5-bis(di-tert-butylphosphinomethyl)pyrrolide) complex and ruthenium coordinated by nitrogen-doped graphene (NDG) as catalysts. To limit the competitive binding of N-2 and H-2 to the metal centre, we have utilized the concept of Frustrated Lewis Pair [AH](+)[BH](-) (FLP-H-2), which can act as a co-catalyst. It can be utilized to functionalize the coordinated N-2 into NH3 and hydrazine. According to the calculated thermodynamic and kinetic barriers, we have observed that the [Co(N-2)((PNP)-P-R)] and ruthenium coordinated by NDG can be used as catalysts to activate N-2. The alternative addition of H+ and H- to metal coordinated N-2 molecule using the FLP-H-2 source is proposed in the catalytic cycle to generate NH3 and NH2NH2. The current investigation also reveals some thermodynamically feasible hexa- and penta-coordinated metal-hydride bond formation.