Oxidation and reduction of Pd(100) and aerosol-deposited Pd nanoparticles

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Oxidation and reduction of Pd(100) and aerosol-deposited Pd nanoparticles

Westerström, Rasmus (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

Messing, Maria (author): Lund University,Lunds universitet,Fasta tillståndets fysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Synkrotronljusfysik,Solid State Physics,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Synchrotron Radiation Research,Faculty of Engineering, LTH

Blomberg, Sara (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

Hellman, Anders, 1974 (author): Chalmers tekniska högskola,Chalmers University of Technology

Grönbeck, Henrik, 1966 (author): Chalmers tekniska högskola,Chalmers University of Technology

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

Martin, Natalia (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

Balmes, O. (author)

van Rijn, R. (author)

Andersen, Jesper N (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

Deppert, Knut (author): Lund University,Lunds universitet,Fasta tillståndets fysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Solid State Physics,Department of Physics,Departments at LTH,Faculty of Engineering, LTH

Bluhm, H. (author)

Liu, Z. (author)

Grass, M. E. (author)

Havecker, M. (author)

Lundgren, Edvin (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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2011
2011
English.
In: Physical Review B - Condensed Matter and Materials Physics. - 2469-9950 .- 2469-9969 .- 1098-0121. ; 83:11

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Journal article (peer-reviewed)

Abstract Subject headings

Using in situ high-pressure x-ray photoelectron spectroscopy, we have followed the oxidation and the reduction of Pd model catalysts in oxygen and CO pressures in the millibar range. The study includes a Pd(100) single crystal as well as SiOx-supported Pd nanoparticles of 15 or 35 nm diameter, respectively. We demonstrate that nanoparticles also form ultrathin surface oxides prior to the onset of the bulk PdO. The Pd nanoparticles are observed to bulk oxidize at sample temperatures 40 degrees lower than the single-crystal surface. In the Pd 3d(5/2) and the O 1s spectrum, we identify a component corresponding to undercoordinated atoms at the surface of the PdO oxide. The experimentally observed PdO core-level shift is supported by density functional theory calculations. In a CO atmosphere, the Pd 3d(5/2) component corresponding to undercoordinated PdO atoms is shifted by + 0.55 eV with respect to PdO bulk, demonstrating that CO molecules preferably adsorb at these sites. CO coordinated to Pd atoms in the metallic and the oxidized phases can also be distinguished in the C 1s spectrum. The initial reduction by CO is similar for the single-crystal and the nanoparticle samples, but after the complete removal of the oxide we detect a significant deviation between the two systems, namely that the nanoparticles incorporate carbon to form a Pd carbide. Our results indicate that CO can dissociate on the nanoparticle samples, whereas no such behavior is observed for the Pd(100) single crystal. These results demonstrate the similarities, as well as the important differences, between the single crystals used as model systems for catalysis and nm-sized particles on oxide supports.

Subject headings

NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
NATURVETENSKAP -- Fysik -- Den kondenserade materiens fysik (hsv//swe)
NATURAL SCIENCES -- Physical Sciences -- Condensed Matter Physics (hsv//eng)

Keyword

spark discharge
single-crystals
in-situ xps
catalyst nanoparticles
co oxidation
range 1-150 torr
root-5)r27-degrees-o surface oxide
ray photoelectron-spectroscopy
pd(111) oxidation
model catalyst

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By the author/editor: Westerström, Ras ...; Messing, Maria; Blomberg, Sara; Hellman, Anders, ...; Grönbeck, Henrik ...; Gustafson, Johan; show more...; Martin, Natalia; Balmes, O.; van Rijn, R.; Andersen, Jesper ...; Deppert, Knut; Bluhm, H.; Liu, Z.; Grass, M. E.; Havecker, M.; Lundgren, Edvin; show less...

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NATURAL SCIENCES: NATURAL SCIENCES; and Physical Science ...; and Atom and Molecul ...

NATURAL SCIENCES: NATURAL SCIENCES; and Physical Science ...; and Condensed Matter ...

Articles in the publication: Physical Review ...

By the university: Chalmers University of Technology; Lund University

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