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Title: 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-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/CeO2 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 C 1s XPS region. 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 Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704; AC02-05CH11231
OSTI ID:
1333199
Alternate ID(s):
OSTI ID: 1378983; OSTI ID: 1400562
Report Number(s):
BNL-113195-2016-JA; R&D Project: CO040; KC0302010
Journal Information:
Angewandte Chemie (International Edition), Vol. 55, Issue 26; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 245 works
Citation information provided by
Web of Science

References (33)

Methane activation on Ni(111): Effects of poisons and step defects journal October 2005
Theoretical investigation of the methane cracking reaction pathways on Ni (1 1 1) surface journal October 2015
Methane activation on Ni and Ru model catalysts journal December 2000
In Situ and Theoretical Studies for the Dissociation of Water on an Active Ni/CeO 2 Catalyst: Importance of Strong Metal-Support Interactions for the Cleavage of O-H Bonds journal February 2015
Development of Ni-Pd bimetallic catalysts for the utilization of carbon dioxide and methane by dry reforming journal September 2009
Synthesis of carbon nanotubes on Ni/carbon-fiber catalysts under mild conditions journal January 2004
Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al 2 O 3 Catalysts Induced by Strong Metal-Support Interactions journal February 2015
Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum journal June 2014
Enhanced Carbon-Resistant Dry Reforming Fe-Ni Catalyst: Role of Fe journal March 2015
Methane Activation by Heterogeneous Catalysis journal November 2014
Review on dry reforming of methane, a potentially more environmentally-friendly approach to the increasing natural gas exploitation journal November 2014
Water–Gas Shift and CO Methanation Reactions over Ni–CeO2(111) Catalysts journal January 2011
Morphology Dependence of Catalytic Properties of Ni/CeO 2 Nanostructures for Carbon Dioxide Reforming of Methane journal April 2012
Control of the Charge State of Metal Atoms on Thin MgO Films journal March 2007
Stable Performance of Ni Catalysts in the Dry Reforming of Methane at High Temperatures for the Efficient Conversion of CO 2 into Syngas journal October 2013
Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al 2 O 3 Catalysts Induced by Strong Metal-Support Interactions journal February 2015
Methane dissociation and adsorption on Ni(111), Pt(111), Ni(100), Pt(100), and Pt(110)-(1×2): Energetic study journal February 2010
Au Dimers on Thin MgO(001) Films: Flat and Charged or Upright and Neutral? journal June 2008
Auf dem Weg zu größtmöglicher Effizienz bei der katalytischen Nutzung von Edelmetallen: atomar dispergiertes Oberflächen-Platin journal June 2014
A New Type of Strong Metal–Support Interaction and the Production of H 2 through the Transformation of Water on Pt/CeO 2 (111) and Pt/CeO x /TiO 2 (110) Catalysts journal May 2012
Mode selectivity in methane dissociative chemisorption on Ni(111) journal January 2013
Consequences of Metal–Oxide Interconversion for C–H Bond Activation during CH 4 Reactions on Pd Catalysts journal October 2013
Interactions of Ni Nanoparticles with Reducible CeO 2 (111) Thin Films journal April 2012
Low-Temperature Dissociation of CO 2 on a Ni/CeO 2 (111)/Ru(0001) Model Catalyst journal March 2016
Promoting Strong Metal Support Interaction: Doping ZnO for Enhanced Activity of Cu/ZnO:M (M = Al, Ga, Mg) Catalysts journal April 2015
Mechanism and Site Requirements for Activation and Chemical Conversion of Methane on Supported Pt Clusters and Turnover Rate Comparisons among Noble Metals journal April 2004
Theoretical Studies of the Adsorption of CO and C on Ni(111) and Ni/CeO 2 (111): Evidence of a Strong Metal–Support Interaction journal April 2013
Importance of the Metal-Oxide Interface in Catalysis: In Situ Studies of the Water-Gas Shift Reaction by Ambient-Pressure X-ray Photoelectron Spectroscopy journal April 2013
Importance of the Metal-Oxide Interface in Catalysis: In Situ Studies of the Water-Gas Shift Reaction by Ambient-Pressure X-ray Photoelectron Spectroscopy journal April 2013
In situ spectroscopic detection ofSMSI effect in a Ni/CeO 2 system: hydrogen-induced burial and dig out of metallic nickel journal January 2010
A review of dry (CO 2 ) reforming of methane over noble metal catalysts journal January 2014
In Situ and Theoretical Studies for the Dissociation of Water on an Active Ni/CeO 2 Catalyst: Importance of Strong Metal-Support Interactions for the Cleavage of O-H Bonds journal February 2015
Aspects of Methane Chemistry journal June 1995

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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
Large Specific Surface Area Macroporous Nanocast LaFe 1− x Ni x O 3 : A Stable Catalyst for Catalytic Methane Dry Reforming journal December 2019
Synergistic catalysis between nano-Ni and nano semiconductor CeO 2 of Ni hybrid nanostructured catalysts for highly efficient selective hydrogenation journal January 2019
Strong Metal–Support Interactions between Copper and Iron Oxide during the High‐Temperature Water‐Gas Shift Reaction journal May 2019
Controlling the Reduction Extent for Metal Catalysts journal May 2019
Nitrogen-carbon layer coated nickel nanoparticles for efficient electrocatalytic reduction of carbon dioxide journal March 2019
A Review on Bimetallic Nickel-Based Catalysts for CO 2 Reforming of Methane journal August 2017
Growth and structure of ultrathin praseodymium oxide layers on ruthenium(0001) journal January 2017
Evaluating differences in the active-site electronics of supported Au nanoparticle catalysts using Hammett and DFT studies journal January 2018
Topologically immobilized catalysis centre for long-term stable carbon dioxide reforming of methane journal January 2019
Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal-Oxide Interface Restructuring of Nickel/Zirconia journal September 2017
Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts [Supplemental Data] preprint June 2018
Insights into interface engineering in steam reforming reactions for hydrogen production journal January 2019
Kinetics of methane electrooxidation in pure and composite anodes of La0.3Y0.1Sr0.4TiO3−δ journal December 2019
Strong Metal–Support Interactions between Copper and Iron Oxide during the High‐Temperature Water‐Gas Shift Reaction journal May 2019
Mesoporous Ni(OH) 2 /CeNi x O y Composites Derived Ni/CeNi x O y Catalysts for Dry Reforming of Methane journal November 2017
Nanosized Ni/SBA-15 Catalysts for CO2 Reforming of CH4 journal May 2019
Interfacial CoO x Layers on TiO 2 as an Efficient Catalyst for Solvent-Free Aerobic Oxidation of Hydrocarbons journal October 2018
Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal-Oxide Interface Restructuring of Nickel/Zirconia text January 2017
Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts [Supplementary Data] other June 2018
Tri-reforming of surrogate biogas over Ni/Mg/ceria–zirconia/alumina pellet catalysts journal June 2018