skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Water-Gas Shift and CO Methanation Reactions over Ni-CeO2(111) Catalysts

Abstract

X-ray and ultraviolet photoelectron spectroscopies were used to study the interaction of Ni atoms with CeO{sub 2}(111) surfaces. Upon adsorption on CeO{sub 2}(111) at 300 K, nickel remains in a metallic state. Heating to elevated temperatures (500-800 K) leads to partial reduction of the ceria substrate with the formation of Ni{sup 2+} species that exists as NiO and/or Ce{sub 1-x}Ni{sub x}O{sub 2-y}. Interactions of nickel with the oxide substrate significantly reduce the density of occupied Ni 3d states near the Fermi level. The results of core-level photoemission and near-edge X-ray absorption fine structure point to weakly bound CO species on CeO{sub 2}(111) which are clearly distinguishable from the formation of chemisorbed carbonates. In the presence of Ni, a stronger interaction is observed with chemisorption of CO on the admetal. When the Ni is in contact with Ce{sup +3} cations, CO dissociates on the surface at 300 K forming NiC{sub x} compounds that may be involved in the formation of CH{sub 4} at higher temperatures. At medium and large Ni coverages (>0.3 ML), the Ni/CeO{sub 2}(111) surfaces are able to catalyze the production of methane from CO and H{sub 2}, with an activity slightly higher than that of Ni(100) or Ni(111).more » On the other hand, at small coverages of Ni (<0.3 ML), the Ni/CeO{sub 2}(111) surfaces exhibit a very low activity for CO methanation but are very good catalysts for the water-gas shift reaction.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE SC OFFICE OF SCIENCE (SC)
OSTI Identifier:
1042152
Report Number(s):
BNL-97830-2012-JA
Journal ID: ISSN 1022-5528; TRN: US201212%%563
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Topics in Catalysis
Additional Journal Information:
Journal Volume: 54; Journal Issue: 1-4; Journal ID: ISSN 1022-5528
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; ABSORPTION; ADSORPTION; ATOMS; CARBON MONOXIDE; CARBONATES; CATALYSTS; CATIONS; CHEMISORPTION; FERMI LEVEL; FINE STRUCTURE; HEATING; METHANATION; METHANE; NICKEL; OXIDES; PHOTOEMISSION; PRODUCTION; SUBSTRATES; WATER; WATER GAS

Citation Formats

Senanayake, S, Evans, J, Agnoli, S, Barrio, L, Chen, T, Hrbek, J, and Rodriguez, J. Water-Gas Shift and CO Methanation Reactions over Ni-CeO2(111) Catalysts. United States: N. p., 2011. Web. doi:10.1007/s11244-011-9645-6.
Senanayake, S, Evans, J, Agnoli, S, Barrio, L, Chen, T, Hrbek, J, & Rodriguez, J. Water-Gas Shift and CO Methanation Reactions over Ni-CeO2(111) Catalysts. United States. doi:10.1007/s11244-011-9645-6.
Senanayake, S, Evans, J, Agnoli, S, Barrio, L, Chen, T, Hrbek, J, and Rodriguez, J. Sat . "Water-Gas Shift and CO Methanation Reactions over Ni-CeO2(111) Catalysts". United States. doi:10.1007/s11244-011-9645-6.
@article{osti_1042152,
title = {Water-Gas Shift and CO Methanation Reactions over Ni-CeO2(111) Catalysts},
author = {Senanayake, S and Evans, J and Agnoli, S and Barrio, L and Chen, T and Hrbek, J and Rodriguez, J},
abstractNote = {X-ray and ultraviolet photoelectron spectroscopies were used to study the interaction of Ni atoms with CeO{sub 2}(111) surfaces. Upon adsorption on CeO{sub 2}(111) at 300 K, nickel remains in a metallic state. Heating to elevated temperatures (500-800 K) leads to partial reduction of the ceria substrate with the formation of Ni{sup 2+} species that exists as NiO and/or Ce{sub 1-x}Ni{sub x}O{sub 2-y}. Interactions of nickel with the oxide substrate significantly reduce the density of occupied Ni 3d states near the Fermi level. The results of core-level photoemission and near-edge X-ray absorption fine structure point to weakly bound CO species on CeO{sub 2}(111) which are clearly distinguishable from the formation of chemisorbed carbonates. In the presence of Ni, a stronger interaction is observed with chemisorption of CO on the admetal. When the Ni is in contact with Ce{sup +3} cations, CO dissociates on the surface at 300 K forming NiC{sub x} compounds that may be involved in the formation of CH{sub 4} at higher temperatures. At medium and large Ni coverages (>0.3 ML), the Ni/CeO{sub 2}(111) surfaces are able to catalyze the production of methane from CO and H{sub 2}, with an activity slightly higher than that of Ni(100) or Ni(111). On the other hand, at small coverages of Ni (<0.3 ML), the Ni/CeO{sub 2}(111) surfaces exhibit a very low activity for CO methanation but are very good catalysts for the water-gas shift reaction.},
doi = {10.1007/s11244-011-9645-6},
journal = {Topics in Catalysis},
issn = {1022-5528},
number = 1-4,
volume = 54,
place = {United States},
year = {2011},
month = {12}
}