A new methodology is proposed and tested by Density Functional Theory (DFT) calculations to reduce N-2 to NH3 and N2H4 using H-2 in the presence of [Mo{(NHCH2CH2)(3)N}] and organic co-catalysts under mild experimental conditions. The calculated Gibbs free energies of the fundamental reactions to form various intermediates and transition state molecules suggest that the proposed catalytic cycle is viable to produce NH3 and N2H4, however NH3 formation is more feasible than N2H4. Formation of six coordinate [Mo]-H intermediates have also been predicted. The direct contact of H-2 with [N-2-Mo{(NHCH2CH2)(3)N}] catalyst can be avoided by using organic co-catalysts to prevent the competition in binding between N-2 and H-2 with [Mo{(NHCH2CH2)(3)N}] catalyst. (C) 2013 Elsevier B.V. All rights reserved.