▎ 摘　　要

Chemists have long been pursuing the aim of synthesising practically viable low temperature catalysts with high stability, activity and selectivity towards the generation of ammonia under less expensive reaction conditions by using H-2 and N-2. In this regard, we have used molybdenum bound nitrogen-doped graphene as a catalyst in the present computational investigation. We developed a new concept of the Frustrated Lewis Pair [AH](+)[BH](-) (FLP-H-2), which can be used as a source of hydrogen to functionalise the coordinated dinitrogen into ammonia. Furthermore, the utilisation of FLP-H-2 can prevent the competition in binding of N-2 and H-2 with Mo centre and enable the product formation. Our computed thermodynamic and kinetic barriers clearly reveal that the molybdenum bound nitrogen-doped graphene can be used as a catalyst to activate and functionalise the dinitrogen. In the proposed catalytic cycle, H+ and H- can be added in an alternate manner using the FLP-H-2 source to yield NH3 and NH2NH2. Some thermodynamically viable penta-coordinated [M]-H intermediates have also been identified in the current study.