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Dry reforming of methane on a highly-active Ni-CeO2 catalyst: Effects of metal-support interactions on C–H bond breaking

Journal Article · · Angewandte Chemie (International Edition)
 [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)

Ni-CeO2 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/CeO2 at temperatures as low as 300 K, generating CHx and COx 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/CeO2–x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CHx or C species are detected in the C1s XPS region. As a result, the reforming of methane proceeds in a clean and efficient way.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1333199
Report Number(s):
BNL--113195-2016-JA; KC0302010
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 26 Vol. 55; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Nanosized Ni/SBA-15 Catalysts for CO2 Reforming of CH4 journal May 2019
Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts [Supplemental Data] preprint June 2018
Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts [Supplementary Data] other June 2018