Adsorption and Reaction of Acetone over CeOx(111) Thin Films

Journal Article · Wed Dec 31 23:00:00 EST 2008 · Journal of Physical Chemistry C

DOI:https://doi.org/10.1021/jp810403d· OSTI ID:979998

Senanayake, S; Gordon, W; Overbury, S; Mullins, D

This study reports the interaction of acetone (CH{sub 3}COCH{sub 3}), the simplest ketone, with well ordered CeO2(111) thin film surfaces. The fully oxidized CeO{sub 2}(111) surface shows a weak interaction with acetone with the sole desorption product (TPD) being acetone at 210 K. The chemisorbed molecule binds to the surface as the 1-acetone species rather than through a bridge-bonded dioxy-configuration. Exposure of a CeO{sub 2}(111) surface to acetone at 600K removes oxygen as CO and results in the conversion of Ce{sup 4+} to Ce{sup 3+}. Acetone chemisorbs strongly on reduced CeO{sub 2-x}(111) with molecular acetone desorbing near 500 K. Decomposition also occurs with H{sub 2} desorbing between 450 and 600 K and C reacting with O in the ceria to desorb above 650 K. A stable species exists from 200 to 500 K on the reduced surface that has three unique types of C. High resolution C 1s XPS spectra indicate these are Ce-CH{sub 2}, C-CH{sub 3} and C-O species. C k-edge NEXAFS indicates the presence of C{double_bond}C and C{double_bond}O bonds. It is postulated that the intermediate is a carbanion bonded through both O and C atoms to Ce cations.

• Research Organization: Brookhaven National Laboratory (BNL) National Synchrotron Light Source
• Sponsoring Organization: Doe - Office Of Science
• DOE Contract Number: AC02-98CH10886
• OSTI ID: 979998
• Report Number(s): BNL--92916-2010-JA
• Journal Information: Journal of Physical Chemistry C, Journal Name: Journal of Physical Chemistry C Journal Issue: 15 Vol. 113; ISSN 1932-7447
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
ACETONE
ADSORPTION
ANIONS
ATOMS
CATIONS
CONVERSION
DECOMPOSITION
DESORPTION
INTERACTIONS
MOLECULES
OXYGEN
RESOLUTION
SPECTRA
SURFACES
THIN FILMS
WEAK INTERACTIONS
WELLS
X-RAY PHOTOELECTRON SPECTROSCOPY
national synchrotron light source