Fe, Mo-co-doped graphene for electrocatalytic N-2-to-NH3 conversion: A DFT investigation

The "cage" like nitmgenase active center structure inspired us to design a "roll-to-roll" Mo-Fe bimetal doped double vacancies graphene (MoFeS4/GR) nitrogen fixation catalyst. By DFT calculations, we studied the nitrogen fixation activity of MoFeS4/GR and the roles played by Mo and Fe in bimetallic catalysts. The calculation results show that the Mo atom is the real active site in MoFeS4/GR. When the nitrogen fixation reaction is carried out on Mo via the enzymatic mechanism, the energy change of the potential determining step is 0.33 eV, and it has good selectivity. In addition, we believe that charge is the main factor affecting the catalyst's nitrogen fixation activity. The role of Mo atoms in the catalyst is to provide electrons, and the role of Fe atoms is to transport electrons.