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

LaNixFe1–xO3 as flexible oxygen or carbon carriers for tunable syngas production and CO2 utilization

Journal Article · · Catalysis Today
 [1];  [2];  [3];  [4];  [2];  [4];  [2]
  1. North Carolina State Univ., Raleigh, NC (United States); North Carolina State University
  2. North Carolina State Univ., Raleigh, NC (United States)
  3. North Carolina State Univ., Raleigh, NC (United States); East China Univ. of Science and Technology, Shanghai (China)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
The current study reports LaFe1–xNixO3–δ redox catalysts as flexible oxygen or carbon carriers for CO2 utilization and tunable production of syngas at relatively low temperatures (~700 °C), in the context of a hybrid redox process. Specifically, perovskite-structured LaFe1–xNixO3–δ with seven different compositions (x = 0.4–1) were prepared and investigated. Cyclic experiments under alternating methane and CO2 flows indicated that all the samples exhibited favorable reactive performance: CH4 and CO2 conversions varied between 85% and 98% and 70–88%, respectively. While H2/CO ratio from Fe-rich redox catalysts was ~2.3:1 in the methane conversion step, Ni-rich catalysts produced a concentrated (~ 93.7 vol%) hydrogen stream via methane cracking. The flexibility of LaFe1–xNixO3–δ to produce syngas (or hydrogen) with tunable compositions was found to be governed by the iron/nickel (Fe/Ni) ratio. Redox catalysts with higher Fe contents act as a lattice oxygen carrier via chemical looping partial oxidation (CLPOx) of methane whereas those with higher Ni contents function as a carbon carrier via chemical looping methane cracking (CLMC) scheme. XRD analysis and temperature-programmed reactions revealed that both types of catalysts involve the formation of La2O3 and Ni0 /Ni-Fe phases under the methane environment. The ability to re-incorporate La2O3 and Ni/Fe into a perovskite structure gives rise to oxygen-carrying capacity whereas stable Ni0 or Ni/Fe phases would catalyze methane cracking without lattice oxygen exchange in the reaction cycles. Here, temperature programmed oxidation and Raman spectroscopy indicated the presence of graphitic and amorphous carbon species, which were effectively gasified by CO2 to produce concentrated CO. Stability tests over LaFe0.5Ni0.5O3 and LaNiO3 revealed that the redox performance was stable over a span of 50 cycles.
Research Organization:
North Carolina State Univ., Raleigh, NC (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE
Grant/Contract Number:
FE0031703
OSTI ID:
1899041
Journal Information:
Catalysis Today, Journal Name: Catalysis Today Vol. 416; ISSN 0920-5861
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (60)

Modifying La 0.6 Sr 0.4 MnO 3 Perovskites with Cr Incorporation for Fast Isothermal CO 2 ‐Splitting Kinetics in Solar‐Driven Thermochemical Cycles journal June 2019
Modified Ceria for “Low‐Temperature” CO 2 Utilization: A Chemical Looping Route to Exploit Industrial Waste Heat journal September 2019
Chemical Looping Dry Reforming as Novel, Intensified Process for CO2 Activation journal June 2012
Carbon Dioxide Reforming of Methane using an Isothermal Redox Membrane Reactor journal May 2015
Iron-Nickel Alloys for Carbon Dioxide Activation by Chemical Looping Dry Reforming of Methane journal May 2016
Chemical‐Looping Conversion of Methane: A Review journal December 2019
A review on coke management during dry reforming of methane: Revisiting coke management in dry reforming of methane journal January 2015
Methanol Synthesis from Industrial CO2 Sources: A Contribution to Chemical Energy Conversion journal January 2017
Deactivating and Non-Deactivating Coking Found on Ni-Based Catalysts during Combined Steam-Dry Reforming of Methane journal February 2021
Pulse study of CO2 reforming of methane over LaNiO3 journal August 2003
Regeneration of catalysts deactivated by coke deposition: A review journal July 2020
Effects of Fe partial substitution of La 2 NiO 4 /LaNiO 3 catalyst precursors prepared by wet impregnation method for the dry reforming of methane journal September 2016
In situ characterization of phase transformation and reactivity of high surface area lanthanum-based Ru catalysts for the combined reforming of methane journal May 2014
One-pot sol-gel synthesis of MgO nanoparticles supported nickel and iron catalysts for undiluted methane decomposition into COx free hydrogen and nanocarbon journal December 2017
Dry reforming of methane over bimetallic Ni-Co catalyst prepared from La(CoxNi1-x)0.5Fe0.5O3 perovskite precursor: Catalytic activity and coking resistance journal May 2019
Bifunctional core-shell architecture allows stable H2 production utilizing CH4 and CO2 in a catalytic chemical looping process journal December 2019
Production of inherently separated syngas streams via chemical looping methane cracking journal December 2017
Dry reforming of methane over Pt-Ni/CeO2 catalysts: Effect of the metal composition on the stability journal January 2021
Spinel oxides as coke-resistant supports for NiO-based oxygen carriers in chemical looping combustion of methane journal September 2019
Ni-Fe-Al mixed oxide for combined dry reforming and decomposition of methane with CO2 utilization journal May 2021
A review on dry reforming of methane over perovskite derived catalysts journal April 2021
Highly reversible CO2 capture using amino acid functionalized ionic liquids immobilized on mesoporous silica journal March 2016
Reverse Boudouard reforming produces CO directly suitable for the production of methanol from CO2 and CH4 journal March 2022
Chemical looping at the nanoscale — challenges and opportunities journal June 2018
The effect of promoters in La 0.9 M 0.1 Ni 0.5 Fe 0.5 O 3 (M = Sr, Ca) perovskite catalysts on dry reforming of methane journal June 2015
Study of defluidization of iron- and manganese-based oxygen carriers under highly reducing conditions in a lab-scale fluidized-bed batch reactor journal August 2021
Tailored hydrotalcite-based Mg-Ni-Al catalyst for hydrogen production via methane decomposition: Effect of nickel concentration and spinel-like structures journal May 2019
UV Raman spectroscopic studies of V/θ-Al2O3 catalysts in butane dehydrogenation journal January 2006
Catalytic decomposition of methane to produce hydrogen: A review journal July 2021
A novel carbon cycle process assisted by Ni/La2O3 catalyst for enhanced thermochemical CO2 splitting journal October 2021
Review of post-combustion carbon dioxide capture technologies using activated carbon journal September 2019
Evolution characteristics of different types of coke deposition during catalytic removal of biomass tar journal December 2020
Self-generated Ni nanoparticles/LaFeO3 heterogeneous oxygen carrier for robust CO2 utilization under a cyclic redox scheme journal November 2021
Recent advances in elevated-temperature pressure swing adsorption for carbon capture and hydrogen production journal November 2019
Isothermal redox for H 2 O and CO 2 splitting – A review and perspective journal November 2017
LaNi x Fe 1– x O 3−δ as a Robust Redox Catalyst for CO 2 Splitting and Methane Partial Oxidation journal August 2021
CH4 Cracking over the Cu–Ni/Al-MCM-41 Catalyst for the Simultaneous Production of H2 and Highly Ordered Graphitic Carbon Nanofibers journal November 2019
Mesoporous Fe 2 O 3 –CeO 2 –Al 2 O 3 Oxygen Carrier for Chemical Looping Dry Reforming with Subsequent Water Splitting journal August 2020
Carbon Capture and Utilization Technology without Carbon Dioxide Purification and Pressurization: A Review on Its Necessity and Available Technologies journal May 2019
Effect of Partial Fe Substitution in La 0.9 Sr 0.1 NiO 3 Perovskite-Derived Catalysts on the Reaction Mechanism of Methane Dry Reforming journal September 2020
Liquid Metal Shell as an Effective Iron Oxide Modifier for Redox-Based Hydrogen Production at Intermediate Temperatures journal August 2021
Perovskites as Geo-inspired Oxygen Storage Materials for Chemical Looping and Three-Way Catalysis: A Perspective journal July 2018
Reduction of CO 2 to Chemicals and Fuels: A Solution to Global Warming and Energy Crisis journal June 2018
Structure Characterization and CO2 Gasification Kinetics of Tri-High Coal-Chars Derived from High-Temperature Pyrolysis journal November 2019
Efficient and New Production Methods of Chemicals and Liquid Fuels by Carbon Monoxide Hydrogenation journal December 2019
Tunable Oxygen Vacancy Formation Energetics in the Complex Perovskite Oxide Sr x La 1– x Mn y Al 1– y O 3 journal November 2014
Defluidization Conditions for a Fluidized Bed of Iron Oxide-, Nickel Oxide-, and Manganese Oxide-Containing Oxygen Carriers for Chemical-Looping Combustion journal December 2005
Reversible Ionic Liquid Stabilized Carbamic Acids: A Pathway Toward Enhanced CO2 Capture
  • Switzer, Jackson R.; Ethier, Amy L.; Flack, Kyle M.
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 36, p. 13159-13163 https://doi.org/10.1021/ie4018836
journal August 2013
Metal oxide redox chemistry for chemical looping processes journal October 2018
Thermochemical CO 2 splitting via redox cycling of ceria reticulated foam structures with dual-scale porosities journal January 2014
Principles of doping ceria for the solar thermochemical redox splitting of H 2 O and CO 2 journal January 2017
Mixed conductive composites for ‘Low-Temperature’ thermo-chemical CO 2 splitting and syngas generation journal January 2020
High-throughput oxygen chemical potential engineering of perovskite oxides for chemical looping applications journal January 2022
CoFe2O4 on a porous Al2O3 nanostructure for solar thermochemical CO2 splitting journal January 2012
General equation for the determination of the crystallite size La of nanographite by Raman spectroscopy journal April 2006
Perovskite nanocomposites as effective CO 2 -splitting agents in a cyclic redox scheme journal August 2017
High-Flux Solar-Driven Thermochemical Dissociation of CO2 and H2O Using Nonstoichiometric Ceria journal December 2010
Catalytic molten metals for the direct conversion of methane to hydrogen and separable carbon journal November 2017
A Selection of Recent Advances in C1 Chemistry journal June 2016
Kinetics and Selectivity Study of Fischer–Tropsch Synthesis to C5+ Hydrocarbons: A Review journal March 2021

Similar Records

LaNixFe1–xO3–δ as a Robust Redox Catalyst for CO2 Splitting and Methane Partial Oxidation
Journal Article · Thu Aug 19 20:00:00 EDT 2021 · Energy and Fuels · OSTI ID:1899040

Mixed conductive composites for ‘Low-Temperature’ thermo-chemical CO2 splitting and syngas generation
Journal Article · Thu Jun 11 20:00:00 EDT 2020 · Journal of Materials Chemistry. A · OSTI ID:1721339