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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)
+ Show Author Affiliations
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); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231; SC0012704
OSTI ID:
1333199
Alternate ID(s):
OSTI ID: 1400562
OSTI ID: 1378983
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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Cited By (25)

Strong Metal–Support Interactions between Copper and Iron Oxide during the High‐Temperature Water‐Gas Shift Reaction journal May 2019
Strong Metal–Support Interactions between Copper and Iron Oxide during the High‐Temperature Water‐Gas Shift Reaction journal May 2019
Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal-Oxide Interface Restructuring of Nickel/Zirconia journal September 2017
Mesoporous Ni(OH) 2 /CeNi x O y Composites Derived Ni/CeNi x O y Catalysts for Dry Reforming of Methane journal November 2017
A Review on Bimetallic Nickel-Based Catalysts for CO 2 Reforming of Methane journal August 2017
Interfacial CoO x Layers on TiO 2 as an Efficient Catalyst for Solvent-Free Aerobic Oxidation of Hydrocarbons journal October 2018
Controlling the Reduction Extent for Metal Catalysts journal May 2019
Kinetics of methane electrooxidation in pure and composite anodes of La0.3Y0.1Sr0.4TiO3−δ journal December 2019
Nitrogen-carbon layer coated nickel nanoparticles for efficient electrocatalytic reduction of carbon dioxide journal March 2019
Evaluating differences in the active-site electronics of supported Au nanoparticle catalysts using Hammett and DFT studies journal January 2018
Atomically dispersed nickel as coke-resistant active sites for methane dry reforming journal November 2019
Growth and structure of ultrathin praseodymium oxide layers on ruthenium(0001) journal January 2017
Ceria-based model catalysts: fundamental studies on the importance of the metal–ceria interface in CO oxidation, the water–gas shift, CO 2 hydrogenation, and methane and alcohol reforming journal January 2017
Low-temperature activation of methane on doped single atoms: descriptor and prediction journal January 2018
Synergistic catalysis between nano-Ni and nano semiconductor CeO 2 of Ni hybrid nanostructured catalysts for highly efficient selective hydrogenation journal January 2019
Synergy of the catalytic activation on Ni and the CeO 2 –TiO 2 /Ce 2 Ti 2 O 7 stoichiometric redox cycle for dramatically enhanced solar fuel production journal January 2019
Topologically immobilized catalysis centre for long-term stable carbon dioxide reforming of methane journal January 2019
Insights into interface engineering in steam reforming reactions for hydrogen production journal January 2019
Exotic electronic structures of Sm x Ce 3−x O y (x = 0-3; y = 2-4) clusters and the effect of high neutral density of low-lying states on photodetachment transition intensities journal August 2018
Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts journal June 2018
Large Specific Surface Area Macroporous Nanocast LaFe 1− x Ni x O 3 : A Stable Catalyst for Catalytic Methane Dry Reforming journal December 2019
Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal-Oxide Interface Restructuring of Nickel/Zirconia text January 2017
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Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts [Supplementary Data] other June 2018

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Dry Reforming of Methane on a Highly‐Active Ni‐CeO 2 Catalyst: Effects of Metal‐Support Interactions on C−H Bond Breaking
Journal Article · Tue May 03 20:00:00 EDT 2016 · Angewandte Chemie · OSTI ID:1400757

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
X-ray photoelectron spectroscopy
ceria
density functional theory
methane dissociation
nickel