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Title: Low Temperature Dry Reforming of Methane Using Ru-Ni-Mg/Ceria-Zirconia Catalysts: Effect of Ru Loading and Reduction Temperature

Journal Article · · Applied Catalysis A: General

Dry reforming catalysts, especially those with activity at moderate temperatures, have been intensely investigated to enhance the conversion of biogas. Here, Ru is evaluated as a promoter for Ni-Mg based catalysts. Catalysts based on 1.4 wt%Ni-1.0 wt%Mg-Ce0.6Zr0.4O2 with Ru (0.02-0.32 wt%) were prepared using incipient wetness. The reducibility of the catalysts and conversions increased with increasing Ru content. Increases in conversions with increasing Ru loading was attributed to the additional active sites and synergistic effect between Ru and Ni, which weakened Ni-Mg interactions. Samples showed dry reforming activity at low temperatures (450-510 degrees C). Reaction rates and activation energies of higher loading Ru samples (1.4 wt%Ni-1.0 wt%Mg/Ce0.6Zr0.4 O2 with 0.16 and 0.32 wt%Ru) decreased when the reduction temperature was raised from 300 to 400 degrees C. A 20 h TOS study showed stable catalytic activity with minimal coke deposition. The results suggest that Ru is an alternative to Pt in promoting low temperature dry reforming of methane.

Research Organization:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office
DOE Contract Number:
AC36-08GO28308
OSTI ID:
1889669
Report Number(s):
NREL/JA-5100-82918; MainId:83691; UUID:7238e38f-cb37-46a9-8986-193ee08f86b9; MainAdminID:65482
Journal Information:
Applied Catalysis A: General, Vol. 645
Country of Publication:
United States
Language:
English

References (57)

Precious Metal Doped Ni–Mg/Ceria–Zirconia Catalysts for Methane Conversion to Syngas by Low Temperature Bi-reforming journal February 2018
Bi-reforming of Methane from Any Source with Steam and Carbon Dioxide Exclusively to Metgas (CO–2H 2 ) for Methanol and Hydrocarbon Synthesis journal December 2012
Single Step Bi-reforming and Oxidative Bi-reforming of Methane (Natural Gas) with Steam and Carbon Dioxide to Metgas (CO-2H 2 ) for Methanol Synthesis: Self-Sufficient Effective and Exclusive Oxygenation of Methane to Methanol with Oxygen journal June 2015
Carbon Dioxide Reforming of Methane To Produce Synthesis Gas over Metal-Supported Catalysts:  State of the Art journal January 1996
A review on dry reforming of methane in aspect of catalytic properties journal March 2019
BINARY MgO-BASED SOLID SOLUTION CATALYSTS FOR METHANE CONVERSION TO SYNGAS journal August 2002
Catalytic reforming of methane with carbon dioxide over nickel catalysts I. Catalyst characterization and activity journal August 1996
Catalytic reforming of methane with carbon dioxide over nickel catalysts II. Reaction kinetics journal August 1996
Recent advances in dry reforming of methane over Ni-based catalysts journal September 2017
The effects of Pt addition to supported Ni catalysts on dry (CO2) reforming of methane to syngas journal June 2014
Low temperature dry reforming of methane over Pt–Ni–Mg/ceria–zirconia catalysts journal December 2015
Impact of Ni and Mg Loadings on Dry Reforming Performance of Pt/Ceria-Zirconia Catalysts journal May 2019
A review of solar methane reforming systems journal October 2015
Synthesis gas production from dry reforming of methane over Ce0.75Zr0.25O2-supported Ru catalysts journal February 2010
Highly Active Ceria-Supported Ru Catalyst for the Dry Reforming of Methane: In Situ Identification of Ru δ+ –Ce 3+ Interactions for Enhanced Conversion journal March 2019
Enhanced activity and durability of Ru catalyst dispersed on zirconia for dry reforming of methane journal September 2017
A review of recent developments in hydrogen production via biogas dry reforming journal September 2018
An investigation on the influence of catalyst composition, calcination and reduction temperatures on Ni/MgO catalyst for dry reforming of methane journal January 2016
Influence of the reduction temperature on catalytic activity of Co/TiO2 (anatase-type) for high pressure dry reforming of methane journal November 2003
Ce0.70La0.20Ni0.10O2-δ catalyst for methane dry reforming: Influence of reduction temperature on the catalytic activity and stability journal December 2017
Promoting effect of Pt, Pd and Rh noble metals to the Ni0.03Mg0.97O solid solution catalysts for the reforming of CH4 with CO2 journal December 1997
Effect of reduction temperature on the CO2-reforming of methane over TiO2-supported Ni catalyst journal January 1997
Synthesis gas production to desired hydrogen to carbon monoxide ratios by tri-reforming of methane using Ni–MgO–(Ce,Zr)O2 catalysts journal November 2012
Characterization of cubic ceria–zirconia powders by X-ray diffraction and vibrational and electronic spectroscopy journal October 2003
The prevalence of surface oxygen vacancies over the mobility of bulk oxygen in nanostructured ceria for the total toluene oxidation journal September 2015
Nickel aluminate spinel-derived catalysts for the aqueous phase reforming of glycerol: Effect of reduction temperature journal May 2019
Morphology effect of Ru/CeO2 catalysts for the catalytic combustion of chlorobenzene journal October 2014
Synthesis and catalytic activity of a Pd doped Ni–MgO catalyst for dry reforming of methane journal January 2017
Effects of Zr Doping into Ceria for the Dry Reforming of Methane over Ni/CeZrO 2 Catalysts: In Situ Studies with XRD, XAFS, and AP-XPS journal January 2020
Estimation of Average Crystallites Size of Active Phase in Ceria-Supported Cobalt-Based Catalysts by Hydrogen Chemisorption vs TEM and XRD Methods journal August 2016
Variation of crystal structure in nickel nanoparticles filled in carbon nanotubes journal November 2012
Graphene Oxide-Doped MgO Nanostructures for Highly Efficient Dye Degradation and Bactericidal Action journal April 2021
A Spectroscopic Characterization of the Reduction of Ceria from Electronic Transitions of Intrinsic Point Defects journal June 1994
Effect of ceria morphology on the catalytic activity of Ru/ceria for the dehydrogenation of ammonia borane journal March 2017
Catalytic behavior of supported Ru nanoparticles on the {1 0 0}, {1 1 0}, and {1 1 1} facet of CeO2 journal September 2015
Preparation of Alumina-Supported Ceria. II. Measurement of Ceria Surface Area after Impregnation with Platinum or Rhodium journal July 1997
Phosphate-Functionalized CeO2 Nanosheets for Efficient Catalytic Oxidation of Dichloromethane journal October 2018
Mechanistic aspects of the dry reforming of methane over ruthenium catalysts journal August 2000
Hydrothermal Synthesis of SnO2 Nanoneedle-Anchored NiO Microsphere and its Gas Sensing Performances journal July 2019
FTIR Studies of CO Adsorption on Al 2 O 3 - and SiO 2 -Supported Ru Catalysts journal January 2006
Methanation of CO2 on supported Ru catalysts
  • Solymosi, Frigyes; Erdöhelyi, András; Kocsis, Mária
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 77, Issue 5 https://doi.org/10.1039/f19817701003
journal January 1981
Temperature-programmed reduction study of NiO–MgO interactions in magnesia-supported Ni catalysts and NiO–MgO physical mixture journal January 1990
The transient species formed over Ru$z.sbnd;RuOx/TiO2 catalyst in the CO and CO + H2 interaction: FTIR spectroscopic study journal October 1992
Kinetic modeling and transient DRIFTS–MS studies of CO2 methanation over Ru/Al2O3 catalysts journal November 2016
IR study of polycrystalline ceria properties in oxidised and reduced states journal April 1999
Characterizations of platinum catalysts supported on Ce, Zr, Pr-oxides and formation of carbonate species in catalytic wet air oxidation of acetic acid journal June 2007
Carbon monoxide and carbon dioxide adsorption on cerium oxide studied by Fourier-transform infrared spectroscopy. Part 1.—Formation of carbonate species on dehydroxylated CeO2, at room temperature
  • Li, Can; Sakata, Yoshihisa; Arai, Toru
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 85, Issue 4 https://doi.org/10.1039/f19898500929
journal January 1989
An infrared spectroscopic investigation of the surface properties of magnesium aluminate spinel journal March 1978
Mechanism of CO 2 Hydrogenation on Pd/Al 2 O 3 Catalysts: Kinetics and Transient DRIFTS-MS Studies journal September 2015
Effect of metal-oxygen bond strength on properties of oxides. 1. Infrared spectroscopy of adsorbed carbon monoxide and carbon dioxide journal January 1986
Silica–Ceria sandwiched Ni core–shell catalyst for low temperature dry reforming of biogas: Coke resistance and mechanistic insights journal August 2018
Low-Temperature Water-Gas Shift:  In-Situ DRIFTS−Reaction Study of a Pt/CeO 2 Catalyst for Fuel Cell Reformer Applications journal September 2003
CO2 reforming of methane over Ni-Ru supported catalysts: On the nature of active sites by operando DRIFTS study journal March 2018
A fourier transform infrared spectroscopic study of C02 methanation on supported ruthenium journal May 1991
The Effect of the Support on the Infrared Spectra of Carbon Monoxide Adsorbed on Nickel journal June 1961
Production of hydrogen by methane dry reforming over ruthenium-nickel based catalysts deposited on Al2O3, MgAl2O4, and YSZ journal October 2019
Eclectic trimetallic Ni–Co–Ru catalyst for the dry reforming of methane journal July 2020