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Title: Elucidation of temperature-programmed desorption of high-coverage hydrogen on Pt(211), Pt(221), Pt(533) and Pt(553) based on density functional theory calculations

Abstract

In this article we compute high-coverage hydrogen adsorption energies and geometries on the stepped platinum surfaces Pt(211) and Pt(533) which contain a (100)-step type and the Pt(221) and Pt(553) surface with a (111) step edge. We discuss these results in relation to ultra-high-vacuum temperature programmed desorption (TPD) data to elucidate the origin of the desorption features. Our results indicated that on surfaces with a (100)-step type, two distinct ranges of adsorption energy for the step and terrace are observed, which mirrors the TPD spectra for which we find a clear separation of the desorption peaks. For the (111) step type, the TPD spectra show much less separation of the step and terrace features, which we assign to the low individual adsorption energies for H atoms on this step edge. In conclusion, from our results, we obtain a much clearer understanding of the surface–hydrogen bonding at high coverages and the origin of the different TPD features present for the two step types studied.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Leiden Univ. (Netherlands)
  2. Univ. of Iceland, Reykjavík (Iceland); Univ. of Otago, Dunedin (New Zealand)
  3. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Univ. of Iceland, Reykjavík (Iceland)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1569298
Alternate Identifier(s):
OSTI ID: 1544583; OSTI ID: 1560675
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Published Article
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 21; Journal Issue: 31; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kolb, Manuel J., Garden, Anna L., Badan, Cansin, Garrido Torres, José A., Skúlason, Egill, Juurlink, Ludo B. F., Jónsson, Hannes, and Koper, Marc T. M. Elucidation of temperature-programmed desorption of high-coverage hydrogen on Pt(211), Pt(221), Pt(533) and Pt(553) based on density functional theory calculations. United States: N. p., 2019. Web. doi:10.1039/c9cp02330e.
Kolb, Manuel J., Garden, Anna L., Badan, Cansin, Garrido Torres, José A., Skúlason, Egill, Juurlink, Ludo B. F., Jónsson, Hannes, & Koper, Marc T. M. Elucidation of temperature-programmed desorption of high-coverage hydrogen on Pt(211), Pt(221), Pt(533) and Pt(553) based on density functional theory calculations. United States. doi:10.1039/c9cp02330e.
Kolb, Manuel J., Garden, Anna L., Badan, Cansin, Garrido Torres, José A., Skúlason, Egill, Juurlink, Ludo B. F., Jónsson, Hannes, and Koper, Marc T. M. Tue . "Elucidation of temperature-programmed desorption of high-coverage hydrogen on Pt(211), Pt(221), Pt(533) and Pt(553) based on density functional theory calculations". United States. doi:10.1039/c9cp02330e.
@article{osti_1569298,
title = {Elucidation of temperature-programmed desorption of high-coverage hydrogen on Pt(211), Pt(221), Pt(533) and Pt(553) based on density functional theory calculations},
author = {Kolb, Manuel J. and Garden, Anna L. and Badan, Cansin and Garrido Torres, José A. and Skúlason, Egill and Juurlink, Ludo B. F. and Jónsson, Hannes and Koper, Marc T. M.},
abstractNote = {In this article we compute high-coverage hydrogen adsorption energies and geometries on the stepped platinum surfaces Pt(211) and Pt(533) which contain a (100)-step type and the Pt(221) and Pt(553) surface with a (111) step edge. We discuss these results in relation to ultra-high-vacuum temperature programmed desorption (TPD) data to elucidate the origin of the desorption features. Our results indicated that on surfaces with a (100)-step type, two distinct ranges of adsorption energy for the step and terrace are observed, which mirrors the TPD spectra for which we find a clear separation of the desorption peaks. For the (111) step type, the TPD spectra show much less separation of the step and terrace features, which we assign to the low individual adsorption energies for H atoms on this step edge. In conclusion, from our results, we obtain a much clearer understanding of the surface–hydrogen bonding at high coverages and the origin of the different TPD features present for the two step types studied.},
doi = {10.1039/c9cp02330e},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 31,
volume = 21,
place = {United States},
year = {2019},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/c9cp02330e

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