Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Changes in Ni-NiO equilibrium due to LaFeO3 and the effect on dry reforming of CH4

Journal Article · · Journal of Catalysis
 [1];  [2];  [2];  [2]
  1. University of Pennsylvania, Philadelphia, PA (United States); University of Pennsylvania
  2. University of Pennsylvania, Philadelphia, PA (United States)
The interactions between Ni and LaFeO3 were studied on catalysts prepared by Atomic Layer Deposition (ALD) of 0.5-nm films of LaFeO3 on MgAl2O4. Scanning Transmission Electron Microscopy showed that the films covered the support uniformly, even after 5 redox cycles at 1073 K, and X-Ray Diffraction showed that the films had the perovskite structure. Equilibrium between Ni and NiO was studied using coulometric-titration and flow-titration measurements on 5-wt% Ni catalysts, with and without LaFeO3. While equilibrium constants for Ni/MgAl2O4 were similar to that expected for bulk Ni, equilibrium PO2 were shifted to significantly lower values in the presence of LaFeO3. In studies of Methane Dry Reforming, the shift in equilibrium resulted in catalyst deactivation due to Ni oxidation at low CO:CO2 ratios, even though Ni/LaFeO3/MgAl2O4 otherwise showed a high reaction rate and excellent tolerance against coking.
Research Organization:
University of Pennsylvania, Philadelphia, PA (United States)
Sponsoring Organization:
National Science Foundation; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
SC0009440
OSTI ID:
1593967
Alternate ID(s):
OSTI ID: 1579763
Journal Information:
Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 381; ISSN 0021-9517
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (39)

Self-Regenerating Rh- and Pt-Based Perovskite Catalysts for Automotive-Emissions Control journal September 2006
A Nickel-Based Perovskite Catalyst with a Bimodal Size Distribution of Nickel Particles for Dry Reforming of Methane journal March 2018
Structural Reversibility and Nickel Particle stability in Lanthanum Iron Nickel Perovskite-Type Catalysts journal May 2017
Steam Reforming and Graphite Formation on Ni Catalysts journal July 2002
Strong metal-support interactions: Occurrence among the binary oxides of groups IIA?VB journal October 1978
Carbon dioxide reforming of methane to synthesis gas over Ni/La2O3 catalysts journal April 1996
Additive effect of noble metals on NiO-MgO solid solution in oxidative steam reforming of methane under atmospheric and pressurized conditions journal January 2006
A thermodynamic study of the redox properties of supported Co particles journal April 2011
LaMnO3-based perovskite with in-situ exsolved Ni nanoparticles: a highly active, performance stable and coking resistant catalyst for CO2 dry reforming of CH4 journal August 2018
Coke-resistant Ni@SiO2 catalyst for dry reforming of methane journal October 2015
Dry reforming of methane has no future for hydrogen production: Comparison with steam reforming at high pressure in standard and membrane reactors journal July 2012
CO2 dry-reforming of methane over La0.8Sr0.2Ni0.8M0.2O3 perovskite (M = Bi, Co, Cr, Cu, Fe): Roles of lattice oxygen on C–H activation and carbon suppression journal August 2012
Highly stable barium zirconate supported nickel oxide catalyst for dry reforming of methane: From powders toward shaped catalysts journal June 2018
Oxidation-induced degradation and performance fluctuation of solid oxide fuel cell Ni anodes under simulated high fuel utilization conditions journal April 2019
Effect of reaction temperature on activity of Pt- and Ru-substituted lanthanum zirconate pyrochlores (La2Zr2O7) for dry (CO2) reforming of methane (DRM) journal June 2013
Determination of the equilibrium oxygen non-stoichiometry and the electrical conductivity of La0.5Sr0.5FeO3-x journal November 2004
Oxidation enthalpies for reduction of ceria surfaces journal June 2007
New Atomic-Scale Insight into Self-Regeneration of Pt-CaTiO 3 Catalysts: Incipient Redox-Induced Structures Revealed by a Small-Angle Tilting STEM Technique journal August 2017
Evidence and Model for Strain-Driven Release of Metal Nanocatalysts from Perovskites during Exsolution journal December 2015
Dynamical Observation and Detailed Description of Catalysts under Strong Metal–Support Interaction journal June 2016
New Opportunity for in Situ Exsolution of Metallic Nanoparticles on Perovskite Parent journal July 2016
In Situ Observation of Rh-CaTiO 3 Catalysts during Reduction and Oxidation Treatments by Transmission Electron Microscopy journal January 2017
Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition journal July 2018
Approaches for Understanding and Controlling Interfacial Effects in Oxide-Supported Metal Catalysts journal July 2018
“Intelligent” Pt Catalysts Studied on High-Surface-Area CaTiO 3 Films journal June 2019
Cooperation of Ni and CaO at Interface for CO 2 Reforming of CH 4 : A Combined Theoretical and Experimental Study journal September 2019
Evidence for Entropy Effects in the Reduction of Ceria−Zirconia Solutions journal October 2006
Smart Pd Catalyst with Improved Thermal Stability Supported on High-Surface-Area LaFeO 3 Prepared by Atomic Layer Deposition journal January 2018
Facet-Dependent in Situ Growth of Nanoparticles in Epitaxial Thin Films: The Role of Interfacial Energy journal April 2019
Stability of Nanocrystals:  Thermodynamic Analysis of Oxidation and Re-reduction of Cobalt in Water/Hydrogen Mixtures journal March 2005
Search for a Self-Regenerating Perovskite Catalyst Using ab Initio Thermodynamics Calculations journal January 2013
Inverse NiAl 2 O 4 on LaAlO 3 –Al 2 O 3 : Unique Catalytic Structure for Stable CO 2 Reforming of Methane journal April 2013
Regeneration of Palladium Subsequent to Solid Solution and Segregation in a Perovskite Catalyst: An Intelligent Catalyst journal January 2001
Self-regeneration of a Pd-perovskite catalyst for automotive emissions control journal July 2002
Nano-socketed nickel particles with enhanced coking resistance grown in situ by redox exsolution journal September 2015
Trends in electrode development for next generation solid oxide fuel cells journal January 2016
Super-dry reforming of methane intensifies CO2 utilization via Le Chateliers principle journal October 2016
Polarization-Induced Hysteresis in CuCo-Doped Rare Earth Vanadates SOFC Anodes journal January 2012
Atomic Layer Deposition on Porous Materials: Problems with Conventional Approaches to Catalyst and Fuel Cell Electrode Preparation journal March 2018

Figures / Tables (14)


Similar Records

Dry reforming of methane over Ni supported on LaMnO3 thin films
Journal Article · Sat Aug 07 20:00:00 EDT 2021 · Catalysis Today · OSTI ID:1814128

Epitaxial and Strong Support Interactions between Pt and LaFeO3 Films Stabilize Pt Dispersion
Journal Article · Mon May 18 20:00:00 EDT 2020 · Journal of the American Chemical Society · OSTI ID:1619916