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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 (author)
- University of Florida,Florida Museum Natural History
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- Kim, Minkyu (author)
- Ohio State University
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- Shipilin, Mikhail (author)
- 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
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- van den Bossche, Maxime, 1989 (author)
- Chalmers University of Technology
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- Gustafson, Johan (author)
- 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
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- Merte, Lindsay Richard (author)
- Malmö universitet,Malmö University,Institutionen för materialvetenskap och tillämpad matematik (MTM)
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- Hejral, Uta, 1984 (author)
- 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
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- Grönbeck, Henrik, 1966 (author)
- Chalmers University of Technology
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- Lundgren, Edvin (author)
- 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
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- Asthagiri, A. (author)
- Ohio State University
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- Weaver, Jason F. (author)
- University of Florida,Florida Museum Natural History
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(creator_code:org_t)
- 2018-08-03
- 2018
- English.
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In: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 8:9, s. 8553-8567
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Abstract
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- 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).
Subject headings
- 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)
Keyword
- CO oxidation
- RAIRS
- surface oxide
- infrared spectroscopy
- Pd(100)
- DFT
- PdO
- palladium
- CO oxidation
- DFT
- infrared spectroscopy
- palladium
- Pd(100)
- PdO
- RAIRS
- surface oxide
Publication and Content Type
- art (subject category)
- ref (subject category)
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- By the author/editor
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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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show more...
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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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show less...
- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Inorganic Chemis ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Theoretical Chem ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Physical Science ...
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and Condensed Matter ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Physical Chemist ...
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- ENGINEERING AND TECHNOLOGY
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ENGINEERING AND ...
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and Materials Engine ...
- Articles in the publication
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ACS Catalysis
- By the university
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Chalmers University of Technology
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Lund University
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Malmö University