Unraveling the Active Site in Copper-Ceria Systems for the Water-Gas Shift Reaction: In Situ Characterization of an Inverse Powder CeO2-x/CuO-Cu Catalyst
An inverse powder system composed of CeO{sub 2} nanoparticles dispersed over a CuO-Cu matrix is proposed as a novel catalyst for the water-gas shift reaction. This inverse CeO{sub 2}/CuO-Cu catalyst exhibits a higher activity than standard Cu/CeO{sub 2} catalysts. In situ synchrotron characterization techniques were employed to follow the structural changes of CeO{sub 2}/CuO-Cu under reaction conditions. Time-resolved X-ray diffraction experiments showed the transformation of CuO to metallic Cu via a Cu{sub 2}O intermediate. Short-order structural changes were followed by pair distribution function analysis and corroborated the results obtained by diffraction. Moreover, X-ray absorption spectroscopy also revealed oxidation state changes from Cu{sup 2+} to Cu{sup 0} and the partial reduction of CeO{sub x} nanoparticles. The activity data obtained by mass spectrometry revealed that hydrogen production starts once the copper has been fully reduced. The strong interaction of ceria and copper boosted the catalytic performance of the sample. The inverse catalyst was active at low temperatures, stable to several reaction runs and to redox cycles. These characteristics are highly valuable for mobile fuel cell applications. The active phases of the inverse CeO{sub 2}/CuO-Cu catalyst are partially reduced ceria nanoparticles strongly interacting with metallic copper. The nature and structure of the ceria nanoparticles are of critical importance because they are involved in processes related to water dissociation over the catalyst surface.
- Research Organization:
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
- Sponsoring Organization:
- DOE - OFFICE OF SCIENCE
- DOE Contract Number:
- DE-AC02-98CH10886
- OSTI ID:
- 1020121
- Report Number(s):
- BNL-95970-2011-JA; TRN: US201116%%102
- Journal Information:
- Journal of Physical Chemistry C, Vol. 114, Issue 8; ISSN 1932-7447
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
30 DIRECT ENERGY CONVERSION
ABSORPTION SPECTROSCOPY
CATALYSTS
COPPER
DIFFRACTION
DISSOCIATION
DISTRIBUTION FUNCTIONS
FUEL CELLS
HYDROGEN PRODUCTION
MASS SPECTROSCOPY
PERFORMANCE
STRONG INTERACTIONS
SYNCHROTRONS
TRANSFORMATIONS
VALENCE
WATER
WATER GAS
X-RAY DIFFRACTION
national synchrotron light source