Jump to main content
Jump to site search

Issue 3, 2012
Previous Article Next Article

A theoretical evaluation of possible transition metal electro-catalysts for N2 reduction

Author affiliations

Abstract

Theoretical studies of the possibility of forming ammonia electrochemically at ambient temperature and pressure 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 several close-packed and stepped transition metal surfaces in contact with an acidic electrolyte. Trends in the catalytic activity were calculated for a range of transition metal surfaces and applied potentials under the assumption that the activation energy barrier scales with the free energy difference in each elementary step. The most active surfaces, on top of the volcano diagrams, are Mo, Fe, Rh, and Ru, but hydrogen gas formation will be a competing reaction reducing the faradaic efficiency for ammonia production. Since the early transition metal surfaces such as Sc, Y, Ti, and Zr bind N-adatoms more strongly than H-adatoms, a significant production of ammonia compared with hydrogen gas can be expected on those metal electrodes when a bias of − 1 V to − 1.5 V vs. SHE is applied. Defect-free surfaces of the early transition metals are catalytically more active than their stepped counterparts.

Graphical abstract: A theoretical evaluation of possible transition metal electro-catalysts for N2 reduction

Back to tab navigation

Supplementary files

Publication details

The article was received on 12 Jul 2011, accepted on 09 Nov 2011 and first published on 07 Dec 2011


Article type: Paper
DOI: 10.1039/C1CP22271F
Phys. Chem. Chem. Phys., 2012,14, 1235-1245

  •   Request permissions

    A theoretical evaluation of possible transition metal electro-catalysts for N2 reduction

    E. Skúlason, T. Bligaard, S. Gudmundsdóttir, F. Studt, J. Rossmeisl, F. Abild-Pedersen, T. Vegge, H. Jónsson and J. K. Nørskov, Phys. Chem. Chem. Phys., 2012, 14, 1235
    DOI: 10.1039/C1CP22271F

Search articles by author

Spotlight

Advertisements