DFT based study of transition metal nano-clusters for electrochemical NH3 production

Jakob Geelmuyden Howalt, Thomas Bligaard, Jan Rossmeisl, Tejs Vegge

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Abstract

Theoretical studies of the possibility of producing ammonia electrochemically at ambient temperature and pressure without direct N2 dissociation are presented. Density functional theory calculations were used in combination with the computational standard hydrogen electrode to calculate the free energy profile for the reduction of N2 admolecules and N adatoms on transition metal nanoclusters in contact with an acidic electrolyte. The work has established linear scaling relations for the dissociative reaction intermediates NH, NH2, and NH3. In addition, linear scaling relations for the associative reaction intermediates N2H, N2H2, and N2H3 have been determined. Furthermore, correlations between the adsorption energies of N, N2, and H have been established. These scaling relations and the free energy corrections are used to establish volcanoes describing the onset potential for electrochemical ammonia production. The competing hydrogen evolution reaction has also been analyzed for comparison.
Original languageEnglish
JournalPhysical Chemistry Chemical Physics
Volume15
Pages (from-to)7785-7795
ISSN1463-9076
DOIs
Publication statusPublished - 2013

Bibliographical note

Published as Gold Open Access as part of the RSC’s Gold for Gold initiative.

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