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Volumn 111, Issue 33, 2007, Pages 12425-12433

Hydrogen oxidation reaction on Pt in acidic media: Adsorption isotherm and activation free energies

Author keywords

[No Author keywords available]

Indexed keywords

ADSORPTION; ADSORPTION ISOTHERMS; DENSITY FUNCTIONAL THEORY; FREE ENERGY; OXIDATION; REACTION KINETICS;

EID: 34548550898     PISSN: 19327447     EISSN: 19327455     Source Type: Journal    
DOI: 10.1021/jp073400i     Document Type: Article
Times cited : (54)

References (39)
  • 1
    • 34548558387 scopus 로고    scopus 로고
    • Breiter, M. W. Reaction mechanisms of the H2 oxidation/evolution reaction. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; 2 Electrocatalysis, Chapter 25, p 361.
    • Breiter, M. W. Reaction mechanisms of the H2 oxidation/evolution reaction. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; Vol. 2 Electrocatalysis, Chapter 25, p 361.
  • 2
    • 34548571622 scopus 로고    scopus 로고
    • Markovic, N. M. The hydrogen electrode reaction and the electrooxidation of CO and H2/CO mixtures on well-characterized Pt and Pt-bimetallic surfaces. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; 2 Electrocatalysis, Chapter 26, p 368.
    • Markovic, N. M. The hydrogen electrode reaction and the electrooxidation of CO and H2/CO mixtures on well-characterized Pt and Pt-bimetallic surfaces. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; Vol. 2 Electrocatalysis, Chapter 26, p 368.
  • 3
    • 34548574413 scopus 로고    scopus 로고
    • Gattre, M.; MacDougall, B. Reaction mechanisms of the O2 reduction/evolution reaction. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; 2 Electrocatalysis, Chapter 30, p 443.
    • Gattre, M.; MacDougall, B. Reaction mechanisms of the O2 reduction/evolution reaction. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; Vol. 2 Electrocatalysis, Chapter 30, p 443.
  • 4
    • 0000762566 scopus 로고
    • Electrode Kinetics
    • Bockris, J. O. M, Ed, Scientific Publications: London, Chapter 4, p
    • Bockris, J. O. M. Electrode Kinetics. In Modern Aspects of Electrochemistry; Bockris, J. O. M., Ed.; Scientific Publications: London, 1954; Chapter 4, p 180.
    • (1954) Modern Aspects of Electrochemistry , pp. 180
    • Bockris, J.O.M.1
  • 16
    • 34548576613 scopus 로고    scopus 로고
    • Trasatti, S. Adsorption - Volcano curve. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; 2 Electrocatalysis, Chapter 10, p 88.
    • Trasatti, S. Adsorption - Volcano curve. In Handbook of Fuel Cells; Vielstich, W., Lamm, A., Gasteiger, H. A., Eds.; Wiley: New York, 2003; Vol. 2 Electrocatalysis, Chapter 10, p 88.
  • 28
    • 34548566654 scopus 로고    scopus 로고
    • The DFT calculations within the DMol3 code used the generalized gradient approximation with the spin-restricted PW91 functional. The Kohn-Sham one-electron equations were solved on a basic set of double numerical plus d functions (comparable to a Gaussian 6-31G(d, with kinetic energies below 5.0 Å, and semi-core pseudo-potentials described the ionic cores. The Pt(111) surface was modeled by a four-layer slab, separated by an 11 Å thick vacuum. H adsorptions on a bare Pt(111) and the H pre-adsorbed Pt(111) were included in a 2′1 super-cell. In all cases, H and the first two Pt layers were allowed to relax, while the Pt atoms in the bottom two layers were fixed at the substrate's lattice position. The differential adsorption energy of H on Pt(111) was expressed as ΔEH, E[(i, 1)H/Pt(111, 1/2E(H2, E[iH/Pt111, where i is the number of H atoms pre-adsorbed per unit cell. In addition, for each optimized structure, a Mulliken
    • 2) - E[iH/Pt(111)], where "i" is the number of H atoms pre-adsorbed per unit cell. In addition, for each optimized structure, a Mulliken population analysis was carried out to estimate the partial charge on each atom and examine qualitative trends in charge redistribution.


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