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Title: Dry reforming of methane on a highly-active Ni-CeO 2 catalyst: Effects of metal-support interactions on C–H bond breaking

Ni-CeO 2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO 2 at temperatures as low as 300 K, generating CH x and CO x species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density-functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) to only 0.15 eV on Ni/CeO 2–x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH x or C species are detected in the C1s XPS region. As a result, the reforming of methane proceeds in a clean and efficient way.
 [1] ;  [2] ;  [3] ;  [2] ;  [4] ;  [1] ;  [2] ;  [5] ;  [2] ;  [4] ;  [6] ;  [3] ;  [7] ;  [2] ;  [8]
  1. State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. CONICET-Univ. Nacional de Rosario (Argentina)
  4. Univ. of Wyoming, Laramie, WY (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. CIC Energigune, Alava (Spain)
  7. Instituto de Catalisis y Petroleoquimica, CSIC, Madrid (Spain)
  8. State Univ. of New York at Stony Brook, Stony Brook NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
Journal ID: ISSN 1433-7851; R&D Project: CO040; KC0302010
Grant/Contract Number:
SC0012704; AC02-05CH11231; CTQ2012-32928; CTQ2015-71823-R
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 26; Journal ID: ISSN 1433-7851
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nickel; ceria; methane dissociation; X-ray photoelectron spectroscopy; density functional theory
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1378983; OSTI ID: 1400562