Nitrogen Reduction Reaction Catalyzed by Diatomic Metals Supported by N-Doped Graphite

In this article, for the transition metal-nitrogen ligand Mn-M@N-6-C (M = Ag, Bi, Cd, Co, Cr, Cu, Fe, Hf, Ir, Mo, Nb, Ni, Os, Pd, Pt, Re, Rh, Ru, Sc, Ta, Tc, V, Y, Zn, Zr, Ti, W), by comparing the amount of change in the length of the N-N triple-bond, and calculating the adsorption energy of N-2 and the change of charge around N-2, it is shown that the activation effect of Sc, Ti, Y, Nb-Mn@N-6-C on the single-atomic layer of graphite substrate is relatively good. The calculation of structural stability shows that the Mn-M@N-6-C (M = Sc, Ti, Y) load is relatively stable when it is on the single-atomic layer of the graphite substrate. Through calculations, a series of data such as the adsorption free energy and reaction path are obtained, and the final results show that the preferred reaction mechanism of NRR is the alternating path on Mn-Ti@N-6-C, and the reaction limit potential is only 0.16 eV, Mn-Ti@N-6-C and has good NRR activity. In addition, the vertical path on Mn-Y@N-6-C has a reaction limit potential of 0.39 eV. Mn-Y@N-6-C also has good NRR catalyzing activity.

Automated summary

In this article, the activation effect of Mn-M@N-6-C (M = Ag, Bi, Cd, Co, Cr, Cu, Fe, Hf, Ir, Mo, Nb, Ni, Os, Pd, Pt, Re, Rh, Ru, Sc, Ta, Tc, V, Y, Zn, Zr, Ti, W) on the single-atomic layer of graphite substrate is investigated. The results show that Sc, Ti, Y, Nb-Mn@N-6-C exhibit relatively good activation effect. The preferred reaction mechanism for NRR is found to be the alternating path on Mn-Ti@N-6-C and Mn-Ti@N-6-C demonstrates good NRR activity.