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This content will become publicly available on October 27, 2017

Title: Room-temperature activation of methane and dry re-forming with CO2 on Ni-CeO2 (111) surfaces: Effect of Ce3+ sites and metal–support interactions on C–H bond cleavage

The results of core-level photoemission indicate that Ni-CeO2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CHx and COx (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6–0.7 eV for the cleavage of the first C–H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C–H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. The strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. Lastly, the coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.
Authors:
 [1] ;  [2] ;  [3] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [7]
  1. Instituto de Fisica Rosario (IFIR, CONICET-UNR), Santa Fe (Argentina)
  2. Univ. Central de Venezuela, Caracas (Venezuela)
  3. State Univ. of New York, Stony Brook, NY (United States)
  4. CIC Energigune, Alava (Spain)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. State Univ. of New York, Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  7. Instituto de Catalisis y Petroleoquimica (ICP-CSIC), Madrid (Spain)
Publication Date:
OSTI Identifier:
1333201
Report Number(s):
BNL--113197-2016-JA
Journal ID: ISSN 2155-5435; R&D Project: CO040; KC0302010
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Name: ACS Catalysis; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ceria; DFT; dry re-forming; methane activation; nickel; support effect; supported catalysts; XPS