Adsorption and reaction of gaseous H(D) atoms with D(H) adatoms on Pt(111) and Sn/Pt(111) surface alloys

Harald Busse, Michael R. Voss, Dmitri Jerdev, Bruce E. Koel, Mark T. Paffett

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

The reaction of gas phase H(D) atoms with adsorbed D(H) atoms on Pt(111) and two different Sn/Pt(111) surface alloys was studied by temperature programmed desorption (TPD). The incident H(D) atoms were produced by thermal dissociation in a Pt tube source operated at 1300 K. The alloy surfaces were prepared in situ by vapor deposition of Sn onto a Pt(111) single crystal to form the (2 × 2) and (√3 × √3)R30°-Sn/Pt(111) surfaces, which have a well-defined structure and composition with relative Sn surface concentrations of 0.25 and 0.33, respectively. A kinetic barrier eliminates dissociative H2(D2) chemisorption on both of these surface alloys, but abstraction reactions of incident H(D) atoms with preadsorbed H or D adatoms occur at 110 K on Pt(111) and both Pt-Sn alloys. This is well below the temperatures for thermal recombination on these surfaces, indicating that the reactions proceed by a direct or pseudo-direct reaction mechanism. Values for the H→D abstraction cross-section, σR, on Pt(111) and the (2 × 2) and (√3 × √3)R30°-Sn/Pt(111) surface alloys were determined to be 0.21, 0.93, and 1.7 Å2, respectively. The corresponding D→H abstraction cross-sections for the two alloys were determined to be 0.8, and 1.5 Å2, respectively. The values of σR for both H→D and D→H reactions increase with ΘSn and indicate a significant structural sensitivity for H abstraction reactions. There is no significant kinetic isotope effect on either alloy surface, however there is evidence that incident H atoms are slightly more efficient in abstracting adsorbed D atoms than vice versa.

Original languageEnglish (US)
Pages (from-to)133-143
Number of pages11
JournalSurface Science
Volume490
Issue number1-2
DOIs
StatePublished - Sep 1 2001
Externally publishedYes

Fingerprint

Adatoms
adatoms
Adsorption
Atoms
adsorption
atoms
thermal dissociation
Vapor deposition
Kinetics
cross sections
kinetics
Temperature programmed desorption
Chemisorption
Isotopes
isotope effect
chemisorption
Gases
desorption
Single crystals
vapor deposition

All Science Journal Classification (ASJC) codes

  • Condensed Matter Physics
  • Materials Chemistry
  • Surfaces, Coatings and Films
  • Surfaces and Interfaces

Cite this

Busse, Harald ; Voss, Michael R. ; Jerdev, Dmitri ; Koel, Bruce E. ; Paffett, Mark T. / Adsorption and reaction of gaseous H(D) atoms with D(H) adatoms on Pt(111) and Sn/Pt(111) surface alloys. In: Surface Science. 2001 ; Vol. 490, No. 1-2. pp. 133-143.
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abstract = "The reaction of gas phase H(D) atoms with adsorbed D(H) atoms on Pt(111) and two different Sn/Pt(111) surface alloys was studied by temperature programmed desorption (TPD). The incident H(D) atoms were produced by thermal dissociation in a Pt tube source operated at 1300 K. The alloy surfaces were prepared in situ by vapor deposition of Sn onto a Pt(111) single crystal to form the (2 × 2) and (√3 × √3)R30°-Sn/Pt(111) surfaces, which have a well-defined structure and composition with relative Sn surface concentrations of 0.25 and 0.33, respectively. A kinetic barrier eliminates dissociative H2(D2) chemisorption on both of these surface alloys, but abstraction reactions of incident H(D) atoms with preadsorbed H or D adatoms occur at 110 K on Pt(111) and both Pt-Sn alloys. This is well below the temperatures for thermal recombination on these surfaces, indicating that the reactions proceed by a direct or pseudo-direct reaction mechanism. Values for the H→D abstraction cross-section, σR, on Pt(111) and the (2 × 2) and (√3 × √3)R30°-Sn/Pt(111) surface alloys were determined to be 0.21, 0.93, and 1.7 {\AA}2, respectively. The corresponding D→H abstraction cross-sections for the two alloys were determined to be 0.8, and 1.5 {\AA}2, respectively. The values of σR for both H→D and D→H reactions increase with ΘSn and indicate a significant structural sensitivity for H abstraction reactions. There is no significant kinetic isotope effect on either alloy surface, however there is evidence that incident H atoms are slightly more efficient in abstracting adsorbed D atoms than vice versa.",
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Adsorption and reaction of gaseous H(D) atoms with D(H) adatoms on Pt(111) and Sn/Pt(111) surface alloys. / Busse, Harald; Voss, Michael R.; Jerdev, Dmitri; Koel, Bruce E.; Paffett, Mark T.

In: Surface Science, Vol. 490, No. 1-2, 01.09.2001, p. 133-143.

Research output: Contribution to journalArticle

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AU - Busse, Harald

AU - Voss, Michael R.

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AB - The reaction of gas phase H(D) atoms with adsorbed D(H) atoms on Pt(111) and two different Sn/Pt(111) surface alloys was studied by temperature programmed desorption (TPD). The incident H(D) atoms were produced by thermal dissociation in a Pt tube source operated at 1300 K. The alloy surfaces were prepared in situ by vapor deposition of Sn onto a Pt(111) single crystal to form the (2 × 2) and (√3 × √3)R30°-Sn/Pt(111) surfaces, which have a well-defined structure and composition with relative Sn surface concentrations of 0.25 and 0.33, respectively. A kinetic barrier eliminates dissociative H2(D2) chemisorption on both of these surface alloys, but abstraction reactions of incident H(D) atoms with preadsorbed H or D adatoms occur at 110 K on Pt(111) and both Pt-Sn alloys. This is well below the temperatures for thermal recombination on these surfaces, indicating that the reactions proceed by a direct or pseudo-direct reaction mechanism. Values for the H→D abstraction cross-section, σR, on Pt(111) and the (2 × 2) and (√3 × √3)R30°-Sn/Pt(111) surface alloys were determined to be 0.21, 0.93, and 1.7 Å2, respectively. The corresponding D→H abstraction cross-sections for the two alloys were determined to be 0.8, and 1.5 Å2, respectively. The values of σR for both H→D and D→H reactions increase with ΘSn and indicate a significant structural sensitivity for H abstraction reactions. There is no significant kinetic isotope effect on either alloy surface, however there is evidence that incident H atoms are slightly more efficient in abstracting adsorbed D atoms than vice versa.

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