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Title: Pd3Ag(111) as a Model System for Hydrogen Separation Membranes: Combined Effects of CO Adsorption and Surface Termination on the Activation of Molecular Hydrogen

Abstract

Abstract The co-adsorption of hydrogen and carbon monoxide on Pd 3 Ag(111) alloy surfaces has been studied as a model system for Pd-Ag alloys in membrane and catalysis applications using periodic density functional theory calculations (PW91-GGA). We explored the effects of Pd–Ag surface composition, since segregation of silver towards and away from the surface has been suggested to explain the experimentally observed changes in H 2 activation, CO inhibition and reactivity. We found that CO pre-adsorbed on the surface weakens the adsorption of H on Pd 3 Ag(111) alloy surfaces irrespective of whether the surface termination corresponds to the bulk Pd 3 Ag composition, or is purely Pd-terminated. A higher coverage of H with CO present is obtained for the Pd-terminated surface; this surface also exhibits a larger range of chemical potentials for co-adsorbed hydrogen and CO. The barrier for H 2 activation increases with increasing CO coverage, but the surface composition has the largest impact on H 2 activation at intermediate CO coverage. The results imply that Pd-based membranes with typically ~ 23 wt% Ag are less prone to CO poisoning if the surface becomes Pd-terminated.

Authors:
ORCiD logo; ; ORCiD logo; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1619451
Grant/Contract Number:  
FG02-05ER15731; AC02-05CH11231
Resource Type:
Published Article
Journal Name:
Topics in Catalysis
Additional Journal Information:
Journal Name: Topics in Catalysis Journal Volume: 63 Journal Issue: 7-8; Journal ID: ISSN 1022-5528
Publisher:
Springer Science + Business Media
Country of Publication:
United States
Language:
English

Citation Formats

Svenum, Ingeborg-Helene, Herron, Jeffrey A., Mavrikakis, Manos, and Venvik, Hilde J. Pd3Ag(111) as a Model System for Hydrogen Separation Membranes: Combined Effects of CO Adsorption and Surface Termination on the Activation of Molecular Hydrogen. United States: N. p., 2020. Web. doi:10.1007/s11244-020-01246-7.
Svenum, Ingeborg-Helene, Herron, Jeffrey A., Mavrikakis, Manos, & Venvik, Hilde J. Pd3Ag(111) as a Model System for Hydrogen Separation Membranes: Combined Effects of CO Adsorption and Surface Termination on the Activation of Molecular Hydrogen. United States. doi:https://doi.org/10.1007/s11244-020-01246-7
Svenum, Ingeborg-Helene, Herron, Jeffrey A., Mavrikakis, Manos, and Venvik, Hilde J. Mon . "Pd3Ag(111) as a Model System for Hydrogen Separation Membranes: Combined Effects of CO Adsorption and Surface Termination on the Activation of Molecular Hydrogen". United States. doi:https://doi.org/10.1007/s11244-020-01246-7.
@article{osti_1619451,
title = {Pd3Ag(111) as a Model System for Hydrogen Separation Membranes: Combined Effects of CO Adsorption and Surface Termination on the Activation of Molecular Hydrogen},
author = {Svenum, Ingeborg-Helene and Herron, Jeffrey A. and Mavrikakis, Manos and Venvik, Hilde J.},
abstractNote = {Abstract The co-adsorption of hydrogen and carbon monoxide on Pd 3 Ag(111) alloy surfaces has been studied as a model system for Pd-Ag alloys in membrane and catalysis applications using periodic density functional theory calculations (PW91-GGA). We explored the effects of Pd–Ag surface composition, since segregation of silver towards and away from the surface has been suggested to explain the experimentally observed changes in H 2 activation, CO inhibition and reactivity. We found that CO pre-adsorbed on the surface weakens the adsorption of H on Pd 3 Ag(111) alloy surfaces irrespective of whether the surface termination corresponds to the bulk Pd 3 Ag composition, or is purely Pd-terminated. A higher coverage of H with CO present is obtained for the Pd-terminated surface; this surface also exhibits a larger range of chemical potentials for co-adsorbed hydrogen and CO. The barrier for H 2 activation increases with increasing CO coverage, but the surface composition has the largest impact on H 2 activation at intermediate CO coverage. The results imply that Pd-based membranes with typically ~ 23 wt% Ag are less prone to CO poisoning if the surface becomes Pd-terminated.},
doi = {10.1007/s11244-020-01246-7},
journal = {Topics in Catalysis},
number = 7-8,
volume = 63,
place = {United States},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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DOI: https://doi.org/10.1007/s11244-020-01246-7

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Cited by: 1 work
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