Vibrational and structural properties of OH adsorbed on Pt(111)

Bedürftig, Kolja; Völkening, Stephan; Wang, Yuemin; Wintterlin, Joost; Jacobi, K.; Ertl, G.

doi:10.1063/1.480472

Cited by 155 publications

(168 citation statements)

References 25 publications

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“…This configuration is similar to an on-top OH state observed by STM and HREELS on Pt͑111͒. 42 On that surface, the OH species were seen to hydrogen bond in six-membered rings.…”

Section: B Adsorption Of Molecules and Radicalssupporting

confidence: 51%

Atomic and molecular adsorption on Rh(111)

Mavrikakis¹,

Rempel

Greeley³

et al. 2002

The Journal of Chemical Physics

202

161

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A systematic study of the chemisorption of both atomic ͑H, O, N, S, C͒, molecular (N 2 , CO, NO), and radical (CH 3 , OH) species on Rh͑111͒ has been performed. Self-consistent, periodic, density functional theory ͑DFT-GGA͒ calculations, using both PW91 and RPBE functionals, have been employed to determine preferred binding sites, detailed chemisorption structures, binding energies, and the effects of surface relaxation for each one of the considered species at a surface coverage of 0.25 ML. The thermochemical results indicate the following order in the binding energies from the least to the most strongly bound: N 2 ϽCH 3 ϽCOϽNOϽHϽOHϽOϽNϽSϽC. A preference for threefold sites for the atomic adsorbates is observed. Molecular adsorbates, in contrast, favor top sites with the exceptions of NO ͑hcp͒ and OH ͑fcc or bridge tilted͒. Surface relaxation leads to insignificant changes in binding energies but to considerable changes in the spacing between surface rhodium atoms, particularly for on-top adsorption where the rhodium atom directly below the adsorbate is lifted above the plane of the surface. RPBE binding energies are found to be in remarkable agreement with the available experimental values. All atomic adsorbates, except for H, have a significant diffusion barrier ͓between 0.4 and 0.6 eV ͑RPBE͔͒ on Rh͑111͒. Atomic H and molecular/radical adsorbates appear to be much more mobile on Rh͑111͒, with an estimated diffusion barrier between 0.1 and 0.2 eV ͑RPBE͒. Finally, the thermochemistry for dissociation of CO, NO, and N 2 on Rh͑111͒ has been examined. In all three cases, decomposition is found to be thermodynamically preferable to desorption.

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“…This configuration is similar to an on-top OH state observed by STM and HREELS on Pt͑111͒. 42 On that surface, the OH species were seen to hydrogen bond in six-membered rings.…”

Section: B Adsorption Of Molecules and Radicalssupporting

confidence: 51%

Atomic and molecular adsorption on Rh(111)

Mavrikakis¹,

Rempel

Greeley³

et al. 2002

The Journal of Chemical Physics

202

161

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“…The sample was cleaned by sputtering-annealing cycles as described elsewhere. 4 The chemical cleanliness was checked by HREELS. Gas purities were 99.999% for H 2 and 99.7% for D 2 .…”

Section: Methodsmentioning

confidence: 99%

Vibrational states of a H monolayer on the Pt(111) surface

et al. 2003

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We present high-resolution electron energy-loss data and theoretical modeling for the vibrational properties of an atomic monolayer of H ͑D͒ on the Pt͑111͒ surface. Experimentally we find three loss peaks, in contrast with two peaks visible in the low-coverage case. A three-dimensional adiabatic potential-energy surface at full coverage of hydrogen is obtained through first-principles calculations. When the zero-point energy effects are included, the minimum energy adsorption site is found to be the fcc site just as in the low-coverage case. Vibrational band states for motion in this potential-energy surface are computed and the excited states associated with the observed loss peaks identified.

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“…The coadsorption of hydrogen and oxygen is a textbook case, being the first step in the catalytic formation of water [2,3,4,5,6,7,8,9]. Oxygen molecules adsorb intact on the Pd(111) surface forming ordered (2×2) islands at low temperature but when the temperature is increased to 120 K thermal dissociation can be observed to occur on the time scale of minutes, and at 160 K all the molecules have dissociated, forming a (2×2) ordered phase [10,11].…”

Section: Introductionmentioning

confidence: 99%

Interactions of oxygen and hydrogen on Pd(111) surface

et al. 2008

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The coadsorption and interactions of oxygen and hydrogen on Pd(111) was studied by scanning tunneling microscopy and density functional theory calculations. In the absence of hydrogen oxygen forms a (2×2) ordered structure. Coadsorption of hydrogen leads to a structural transformation from the (2×2) to a (√3×√3)R30 o structure. In addition to this transformation, hydrogen enhances the mobility of oxygen. To explain these observations, the interaction of oxygen and hydrogen on Pd(111) was studied within the density functional theory. In agreement with the experiment the calculations find a total energy minimum for the oxygen (2×2) structure. The interaction between H and O atoms was found to be repulsive and short ranged, leading to a compression of the O islands from (2×2) to (√3×√3)R30 o ordered structure at high H coverage. The computed energy barriers for the oxygen diffusion were found to be reduced due to the coadsorption of hydrogen, in agreement with the experimentally observed enhancement of oxygen mobility. The calculations also support the finding that at low temperatures the water formation reaction does not occur on Pd(111).

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Vibrational and structural properties of OH adsorbed on Pt(111)

Cited by 155 publications

References 25 publications

Atomic and molecular adsorption on Rh(111)

Atomic and molecular adsorption on Rh(111)

Vibrational states of a H monolayer on the Pt(111) surface

Interactions of oxygen and hydrogen on Pd(111) surface

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