On the dynamics of H2 adsorption on the Pt(111) surface. Issue 17 (30th May 2017)

• Record Type: Journal Article
• Authors: Kraus, Peter; Frank, Irmgard
• Is Part Of: International journal of quantum chemistry. Volume 117:Issue 17(2017)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2017-05-30
• Subjects: AIMD -- Car–Parrinello -- density functional theory -- hydrogen adsorption -- platinum; Quantum chemistry -- Periodicals; 541.28
• DOI: 10.1002/qua.25407
• Languages: English
• ISSNs: 0020-7608

Abstract

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. Abstract : The dynamics and kinetics of the dissociation of hydrogen over the Pt(111) surface are investigated using Car–Parrinello molecular dynamics, including dispersion corrections. The adsorption pathways are investigated on the main sites on the surface. A direct determination of energy‐resolved sticking coefficients from the calculated trajectories shows an excellent agreement with the experimental data at incidence energies in the 5–30 kJ/mol range.