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Understanding the I...
Understanding the Intrinsic Surface Reactivity of Single-Layer and Multilayer PdO(101) on Pd(100)
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- Mehar, Vikram (författare)
- University of Florida,Florida Museum Natural History,Department of Chemical Engineering, University of Florida, Gainesville, 32611, FL, United States
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- Kim, Minkyu (författare)
- Ohio State University,William G. Lowrie Chemical and Biomolecular Engineering, Ohio State University, Columbus, 43210, OH, United States
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- Shipilin, Mikhail (författare)
- Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Division of Synchrotron Radiation Research, Lund University, Lund, SE-22100, Sweden
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- van den Bossche, Maxime, 1989 (författare)
- Chalmers University of Technology,Department of Physics and Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg, SE-412 96, Sweden
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- Gustafson, Johan (författare)
- Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Division of Synchrotron Radiation Research, Lund University, Lund, SE-22100, Sweden
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- Merte, Lindsay Richard (författare)
- Malmö universitet,Malmö University,Institutionen för materialvetenskap och tillämpad matematik (MTM)
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- Hejral, Uta, 1984 (författare)
- Lund University,Lunds universitet,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Division of Synchrotron Radiation Research, Lund University, Lund, SE-22100, Sweden
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- Grönbeck, Henrik, 1966 (författare)
- Chalmers University of Technology,Department of Physics and Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg, SE-412 96, Sweden
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- Lundgren, Edvin (författare)
- Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Synkrotronljusfysik,Fysiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Synchrotron Radiation Research,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Division of Synchrotron Radiation Research, Lund University, Lund, SE-22100, Sweden
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- Asthagiri, A. (författare)
- Ohio State University,William G. Lowrie Chemical and Biomolecular Engineering, Ohio State University, Columbus, 43210, OH, United States
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- Weaver, Jason F. (författare)
- University of Florida,Florida Museum Natural History,Department of Chemical Engineering, University of Florida, Gainesville, 32611, FL, United States
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(creator_code:org_t)
- 2018-08-03
- 2018
- Engelska.
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Ingår i: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 8:9, s. 8553-8567
- Relaterad länk:
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https://www.osti.gov...
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http://dx.doi.org/10...
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https://research.cha...
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https://research.cha...
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https://doi.org/10.1...
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https://research.cha...
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https://lup.lub.lu.s...
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https://urn.kb.se/re...
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Abstract
Ämnesord
Stäng
- We investigated the intrinsic reactivity of CO on single-layer and multilayer PdO(101) grown on Pd(100) using temperature-programmed reaction spectroscopy (TPRS) and reflection absorption infrared spectroscopy (RAIRS) experiments, as well as density functional theory (DFT) calculations. We find that CO binds more strongly on multilayer than single-layer PdO(101) (∼119 kJ/mol vs 43 kJ/mol), and that CO oxidizes negligibly on single-layer PdO(101), whereas nearly 90% of a saturated layer of CO oxidizes on multilayer PdO(101) during TPRS experiments. RAIRS further shows that CO molecules adsorb on both bridge-Pdcusand atop-Pdcussites (coordinatively unsaturated Pd sites) of single-layer PdO(101)/Pd(100), while CO binds exclusively on atop-Pdcussites of multilayer PdO(101). The DFT calculations reproduce the much stronger binding of CO on multilayer PdO(101), as well as the observed binding site preferences, and reveal that the stronger binding is entirely responsible for the higher CO oxidation activity of multilayer PdO(101)/Pd(100). We show that the O atom below the Pdcussite, present only on multilayer PdO(101), modifies the electronic states of the Pdcusatom in a way that enhances the CO-Pdcusbonding. Lastly, we show that a precursor-mediated kinetic model, with energetics determined from the present study, predicts that the intrinsic CO oxidation rates achieved on both single-layer and multilayer PdO(101)/Pd(100) can be expected to exceed the gaseous CO diffusion rate to the surface during steady-state CO oxidation at elevated pressures, even though the intrinsic reaction rates are 4-5 orders of magnitude lower on single-layer PdO(101)/Pd(100) than on multilayer PdO(101)/Pd(100).
Ämnesord
- NATURVETENSKAP -- Kemi -- Oorganisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)
- NATURVETENSKAP -- Kemi -- Teoretisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Theoretical Chemistry (hsv//eng)
- NATURVETENSKAP -- Fysik -- Den kondenserade materiens fysik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Condensed Matter Physics (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
- TEKNIK OCH TEKNOLOGIER -- Materialteknik (hsv//swe)
- ENGINEERING AND TECHNOLOGY -- Materials Engineering (hsv//eng)
Nyckelord
- CO oxidation
- RAIRS
- surface oxide
- infrared spectroscopy
- Pd(100)
- DFT
- PdO
- palladium
- CO oxidation
- DFT
- infrared spectroscopy
- palladium
- Pd(100)
- PdO
- RAIRS
- surface oxide
Publikations- och innehållstyp
- art (ämneskategori)
- ref (ämneskategori)
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- Av författaren/redakt...
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Mehar, Vikram
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Kim, Minkyu
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Shipilin, Mikhai ...
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van den Bossche, ...
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Gustafson, Johan
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Merte, Lindsay R ...
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visa fler...
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Hejral, Uta, 198 ...
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Grönbeck, Henrik ...
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Lundgren, Edvin
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Asthagiri, A.
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Weaver, Jason F.
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- Om ämnet
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- NATURVETENSKAP
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NATURVETENSKAP
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och Kemi
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och Oorganisk kemi
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- NATURVETENSKAP
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NATURVETENSKAP
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och Kemi
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och Teoretisk kemi
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- NATURVETENSKAP
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NATURVETENSKAP
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och Fysik
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och Den kondenserade ...
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- NATURVETENSKAP
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NATURVETENSKAP
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och Kemi
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och Fysikalisk kemi
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- TEKNIK OCH TEKNOLOGIER
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TEKNIK OCH TEKNO ...
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och Materialteknik
- Artiklar i publikationen
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ACS Catalysis
- Av lärosätet
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Chalmers tekniska högskola
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Lunds universitet
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Malmö universitet