DOI: 10.1063/1.471395. Modification of Ni(111) reactivity toward CH4, CO, and D2 by two-dimensional alloying

Modification of Ni(111) reactivity toward CH4, CO, and D2 by two-dimensional alloying

10.1063/1.471395

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

Alloying Au into the outermost atomic layer of Ni(111) significantly alters the physical and chemical properties of the surface. The reactivity is investigated by the use of seeded supersonic molecular beams of CH4 and it is found that the nobleness of Au reduces the overall reactivity toward CH4. This is accounted for in an ensemble model resolving the sticking probability on Ni atoms having different nearest neighbor surroundings. Although a mean field description of site distributions is found to be a very good approximation it is improved by using experimentally determined ensemble statistics from STM images. The strong influence of the vibrational temperature on the sticking coefficients of CH4 vs translational energy on the pure Ni(111) is also demonstrated. Desorption energies of CO and D2 is observed to decrease approximately 25–30 kJ/mole as the coverage of Au is increased from 0.0 to 0.7 ML. In TPD spectra of deuterium saturated surface alloys a new clearly resolved desorption state is observed at 180–220 K with maximum intensity around θAu=0.3–0.4 ML. This state is clearly related to chemisorption sites involving both Au and Ni. A site model based on mean field statistics adequately accounts for the appearance of this state. The effect of Au is also evident in the TPD spectra of CO saturated Au/Ni(111) surface alloys where the saturation coverage decreases and new structure develops.

Bibliography

Holmblad, P. M., Larsen, J. H., & Chorkendorff, I. (1996). Modification of Ni(111) reactivity toward CH4, CO, and D2 by two-dimensional alloying. The Journal of Chemical Physics, 104(18), 7289â7295.

Authors 3

P. M. Holmblad (first)
J. Hvolbæk Larsen (additional)
I. Chorkendorff (additional)

References 28 Referenced 99

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{'key': '2024021106472297700_r2'}
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Dates

Type	When
Created	23 years, 1 month ago (July 26, 2002, 8:32 a.m.)
Deposited	1 year, 6 months ago (Feb. 11, 2024, 1:47 a.m.)
Indexed	2 months ago (June 27, 2025, 4:03 p.m.)
Issued	29 years, 3 months ago (May 8, 1996)
Published	29 years, 3 months ago (May 8, 1996)
Published Print	29 years, 3 months ago (May 8, 1996)

Funders 0

None

BibTeX

@article{Holmblad_1996, title={Modification of Ni(111) reactivity toward CH4, CO, and D2 by two-dimensional alloying}, volume={104}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.471395}, DOI={10.1063/1.471395}, number={18}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Holmblad, P. M. and Larsen, J. Hvolbæk and Chorkendorff, I.}, year={1996}, month=may, pages={7289–7295} }

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