Details
| Original language | English |
|---|---|
| Article number | e25407 |
| Journal | International Journal of Quantum Chemistry |
| Volume | 117 |
| Issue number | 17 |
| Early online date | 30 May 2017 |
| Publication status | Published - 5 Sept 2017 |
Abstract
The dynamics and kinetics of the dissociation of hydrogen over the hexagonal close packed platinum (Pt(111)) surface are investigated using Car–Parrinello molecular dynamics and static density functional theory calculations of the potential energy surfaces. The calculations model the reference energy-resolved molecular beam experiments, considering the degrees of freedom of the catalytic surface. Two-dimensional potential energy surfaces above the main sites on Pt(111) are determined. Combined with Car–Parrinello trajectories, they confirm the dissociative adsorption of H2 as the only adsorption pathway on this surface at H2 incindence energies above 5 kJ/mol. A direct determination of energy-resolved sticking coefficients from molecular dynamics is also performed, showing an excellent agreement with the experimental data at incidence energies in the 5–30 kJ/mol range. Application of dispersion corrections does not lead to an improvement in the prediction of the H2 sticking coefficient. The adsorption reaction rate obtained from the calculated sticking coefficients is consistent with experimentally derived literature values.
Keywords
- AIMD, Car–Parrinello, density functional theory, hydrogen adsorption, platinum
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Atomic and Molecular Physics, and Optics
- Physics and Astronomy(all)
- Condensed Matter Physics
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: International Journal of Quantum Chemistry, Vol. 117, No. 17, e25407, 05.09.2017.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - On the dynamics of H2 adsorption on the Pt(111) surface
AU - Kraus, Peter
AU - Frank, Irmgard
N1 - Publisher Copyright: © 2017 Wiley Periodicals, Inc.
PY - 2017/9/5
Y1 - 2017/9/5
N2 - The dynamics and kinetics of the dissociation of hydrogen over the hexagonal close packed platinum (Pt(111)) surface are investigated using Car–Parrinello molecular dynamics and static density functional theory calculations of the potential energy surfaces. The calculations model the reference energy-resolved molecular beam experiments, considering the degrees of freedom of the catalytic surface. Two-dimensional potential energy surfaces above the main sites on Pt(111) are determined. Combined with Car–Parrinello trajectories, they confirm the dissociative adsorption of H2 as the only adsorption pathway on this surface at H2 incindence energies above 5 kJ/mol. A direct determination of energy-resolved sticking coefficients from molecular dynamics is also performed, showing an excellent agreement with the experimental data at incidence energies in the 5–30 kJ/mol range. Application of dispersion corrections does not lead to an improvement in the prediction of the H2 sticking coefficient. The adsorption reaction rate obtained from the calculated sticking coefficients is consistent with experimentally derived literature values.
AB - The dynamics and kinetics of the dissociation of hydrogen over the hexagonal close packed platinum (Pt(111)) surface are investigated using Car–Parrinello molecular dynamics and static density functional theory calculations of the potential energy surfaces. The calculations model the reference energy-resolved molecular beam experiments, considering the degrees of freedom of the catalytic surface. Two-dimensional potential energy surfaces above the main sites on Pt(111) are determined. Combined with Car–Parrinello trajectories, they confirm the dissociative adsorption of H2 as the only adsorption pathway on this surface at H2 incindence energies above 5 kJ/mol. A direct determination of energy-resolved sticking coefficients from molecular dynamics is also performed, showing an excellent agreement with the experimental data at incidence energies in the 5–30 kJ/mol range. Application of dispersion corrections does not lead to an improvement in the prediction of the H2 sticking coefficient. The adsorption reaction rate obtained from the calculated sticking coefficients is consistent with experimentally derived literature values.
KW - AIMD
KW - Car–Parrinello
KW - density functional theory
KW - hydrogen adsorption
KW - platinum
UR - http://www.scopus.com/inward/record.url?scp=85019679074&partnerID=8YFLogxK
U2 - 10.1002/qua.25407
DO - 10.1002/qua.25407
M3 - Article
AN - SCOPUS:85019679074
VL - 117
JO - International Journal of Quantum Chemistry
JF - International Journal of Quantum Chemistry
SN - 0020-7608
IS - 17
M1 - e25407
ER -