Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures
Abstract
Abstract Methane is converted over nickel on ceria zirconia (Ni/CZ) into ethane, aromatics, and hydrogen at steady state up to the thermodynamic limit at temperatures of 350 to 500 °C. At 450 and 500 °C, traces of ethylene are also produced. Ni/NiO particles activate methane and couple the resulting surface species to hydrocarbon products. Large Ni particles are responsible for the formation of carbonaceous deposits. Furthermore, aromatics are formed on these sites. Smaller Ni/NiO particles are responsible for the formation of ethane and ethylene and appear to provide sustained activity. It is suggested that these Ni sites are too small to assemble aromatic deposits, and hence they remain active throughout the reaction.
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1475145
- Alternate Identifier(s):
- OSTI ID: 1437199
- Report Number(s):
- BNL-209099-2018-JAAM
Journal ID: ISSN 1867-3880
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 12; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; carbon nanotubes; coking dispersion; Lewis acids; nickel oxide
Citation Formats
Okolie, Chukwuemeka, Lyu, Yimeng, Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures. United States: N. p., 2018.
Web. doi:10.1002/cctc.201701892.
Okolie, Chukwuemeka, Lyu, Yimeng, Kovarik, Libor, Stavitski, Eli, & Sievers, Carsten. Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures. United States. https://doi.org/10.1002/cctc.201701892
Okolie, Chukwuemeka, Lyu, Yimeng, Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Mon .
"Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures". United States. https://doi.org/10.1002/cctc.201701892. https://www.osti.gov/servlets/purl/1475145.
@article{osti_1475145,
title = {Coupling of Methane to Ethane, Ethylene, and Aromatics over Nickel on Ceria-Zirconia at Low Temperatures},
author = {Okolie, Chukwuemeka and Lyu, Yimeng and Kovarik, Libor and Stavitski, Eli and Sievers, Carsten},
abstractNote = {Abstract Methane is converted over nickel on ceria zirconia (Ni/CZ) into ethane, aromatics, and hydrogen at steady state up to the thermodynamic limit at temperatures of 350 to 500 °C. At 450 and 500 °C, traces of ethylene are also produced. Ni/NiO particles activate methane and couple the resulting surface species to hydrocarbon products. Large Ni particles are responsible for the formation of carbonaceous deposits. Furthermore, aromatics are formed on these sites. Smaller Ni/NiO particles are responsible for the formation of ethane and ethylene and appear to provide sustained activity. It is suggested that these Ni sites are too small to assemble aromatic deposits, and hence they remain active throughout the reaction.},
doi = {10.1002/cctc.201701892},
journal = {ChemCatChem},
number = 12,
volume = 10,
place = {United States},
year = {Mon Jan 22 00:00:00 EST 2018},
month = {Mon Jan 22 00:00:00 EST 2018}
}
Web of Science
Figures / Tables:
Works referenced in this record:
Effects of carbon deposition and de-coking treatments on the activation of CH4 and CO2 in CO2 reforming of CH4 over Ni/yttria-doped ceria catalysts
journal, September 2004
- Wang, Jenshi B.; Wu, Yen-Shiun; Huang, Ta-Jen
- Applied Catalysis A: General, Vol. 272, Issue 1-2
Oxidative Methane Upgrading
journal, July 2012
- Hammond, Ceri; Conrad, Sabrina; Hermans, Ive
- ChemSusChem, Vol. 5, Issue 9
Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature
journal, April 2016
- Narsimhan, Karthik; Iyoki, Kenta; Dinh, Kimberly
- ACS Central Science, Vol. 2, Issue 6
Effect of the preparation method on the properties of zirconia-ceria materials
journal, January 1999
- Rossignol, Sylvie; Gérard, François; Duprez, Daniel
- Journal of Materials Chemistry, Vol. 9, Issue 7
Methane decomposition to carbon nanotubes and hydrogen on an alumina supported nickel aerogel catalyst
journal, May 2002
- Piao, Lingyu; Li, Yongdan; Chen, Jiuling
- Catalysis Today, Vol. 74, Issue 1-2
Hydrodeoxygenation of Guaiacol over Ceria-Zirconia Catalysts
journal, June 2015
- Schimming, Sarah M.; LaMont, Onaje D.; König, Michael
- ChemSusChem, Vol. 8, Issue 12
Partial oxidation of methane by oxygen over silica
journal, January 1987
- Kasztelan, Slavik; Moffat, John B.
- Journal of the Chemical Society, Chemical Communications, Issue 21
A low temperature reaction sequence for methane conversion
journal, January 1991
- Koerts, Tijs; van Santen, Rutger A.
- Journal of the Chemical Society, Chemical Communications, Issue 18
Raman Spectrum of Graphite
journal, August 1970
- Tuinstra, F.; Koenig, J. L.
- The Journal of Chemical Physics, Vol. 53, Issue 3
Nickel-Based Ceria, Zirconia, and Ceria–Zirconia Catalytic Systems for Low-Temperature Carbon Dioxide Reforming of Methane
journal, November 2007
- Kumar, Prashant; Sun, Yanping; Idem, Raphael O.
- Energy & Fuels, Vol. 21, Issue 6
Non-oxidative coupling of methane catalysed by supported tungsten hydride onto alumina and silica–alumina in classical and H2 permeable membrane fixed-bed reactors
journal, January 2010
- Szeto, K. C.; Norsic, S.; Hardou, L.
- Chemical Communications, Vol. 46, Issue 22
Low temperature steam reforming of methane over Ni–Ce(1−x)Zr(x)O2 catalysts under severe conditions
journal, June 2012
- Roh, Hyun-Seog; Eum, Ic-Hwan; Jeong, Dae-Woon
- Renewable Energy, Vol. 42
A Mercury-Catalyzed, High-Yield System for the Oxidation of Methane to Methanol
journal, January 1993
- Periana, R. A.; Taube, D. J.; Evitt, E. R.
- Science, Vol. 259, Issue 5093
Effect of the Nickel Precursor on the Impregnation and Drying of γ-Al 2 O 3 Catalyst Bodies: A UV−vis and IR Microspectroscopic Study
journal, April 2008
- Espinosa-Alonso, Leticia; de Jong, Krijn P.; Weckhuysen, Bert M.
- The Journal of Physical Chemistry C, Vol. 112, Issue 18
Comprehensive IR study on acid/base properties of metal oxides
journal, August 2012
- Tamura, Masazumi; Shimizu, Ken-ichi; Satsuma, Atsushi
- Applied Catalysis A: General, Vol. 433-434
Characterization of a Mo/ZSM-5 Catalyst for the Conversion of Methane to Benzene
journal, July 1997
- Wang, Dingjun; Lunsford, Jack H.; Rosynek, Michael P.
- Journal of Catalysis, Vol. 169, Issue 1
Oxidative Coupling of Methane over BaO Mixed with CaO and MgO
journal, January 1987
- Yamagata, Nobutsugu; Tanaka, Katsutoshi; Sasaki, Shoichi
- Chemistry Letters, Vol. 16, Issue 1
The Determination of Pore Volume and Area Distributions in Porous Substances. I. Computations from Nitrogen Isotherms
journal, January 1951
- Barrett, Elliott P.; Joyner, Leslie G.; Halenda, Paul P.
- Journal of the American Chemical Society, Vol. 73, Issue 1
Methane decomposition into hydrogen and carbon nanofibers over supported Pd–Ni catalysts
journal, December 2003
- Takenaka, Sakae; Shigeta, Yukio; Tanabe, Eishi
- Journal of Catalysis, Vol. 220, Issue 2
Synthesis of ethylene and ethane by partial oxidation of methane over lithium-doped magnesium oxide
journal, April 1985
- Ito, Tomoyasu; Lunsford, Jack H.
- Nature, Vol. 314, Issue 6013
Preparation of zirconia–ceria materials by soft chemistry
journal, April 1999
- Rossignol, S.; Madier, Y.; Duprez, D.
- Catalysis Today, Vol. 50, Issue 2
Platinum Catalysts for the High-Yield Oxidation of Methane to a Methanol Derivative
journal, April 1998
- Periana, R. A.
- Science, Vol. 280, Issue 5363
Characterization of Graphite Fiber Surfaces with Raman Spectroscopy
journal, October 1970
- Tuinstra, F.; Koenig, J. L.
- Journal of Composite Materials, Vol. 4, Issue 4
Kinetics of hydrogen activation on ceria–zirconia
journal, September 2015
- Schimming, Sarah M.; Foo, Guo Shiou; LaMont, Onaje D.
- Journal of Catalysis, Vol. 329
Direct conversion of methane under nonoxidative conditions
journal, May 2003
- Xu, Yide; Bao, Xinhe; Lin, Liwu
- Journal of Catalysis, Vol. 216, Issue 1-2
Calculations of electron inelastic mean free paths (IMFPS). IV. Evaluation of calculated IMFPs and of the predictive IMFP formula TPP-2 for electron energies between 50 and 2000 eV
journal, January 1993
- Tanuma, S.; Powell, C. J.; Penn, D. R.
- Surface and Interface Analysis, Vol. 20, Issue 1
Oxygen defects and formation of Ce 3+ affecting the photocatalytic performance of CeO 2 nanoparticles
journal, January 2014
- Choudhury, Biswajit; Chetri, Pawan; Choudhury, Amarjyoti
- RSC Adv., Vol. 4, Issue 9
Conversion of Methane into Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor
journal, September 2017
- Okolie, Chukwuemeka; Belhseine, Yasmeen F.; Lyu, Yimeng
- Angewandte Chemie International Edition, Vol. 56, Issue 44
Metal-catalyzed graphitic nanostructures as sorbents for vapor-phase ammonia
journal, January 2011
- Long, Jeffrey W.; Laskoski, Matthew; Peterson, Gregory W.
- Journal of Materials Chemistry, Vol. 21, Issue 10
Catalytic partial oxidation of methane to synthesis gas over Ni–CeO2
journal, February 2001
- Zhu, Tianli; Flytzani-Stephanopoulos, Maria
- Applied Catalysis A: General, Vol. 208, Issue 1-2
Characterization of cubic ceria–zirconia powders by X-ray diffraction and vibrational and electronic spectroscopy
journal, October 2003
- Sánchez Escribano, Vicente; Fernández López, Enrique; Panizza, Marta
- Solid State Sciences, Vol. 5, Issue 10
Selective anaerobic oxidation of methane enables direct synthesis of methanol
journal, May 2017
- Sushkevich, Vitaly L.; Palagin, Dennis; Ranocchiari, Marco
- Science, Vol. 356, Issue 6337
Advances in the Development of Novel Cobalt Fischer−Tropsch Catalysts for Synthesis of Long-Chain Hydrocarbons and Clean Fuels
journal, May 2007
- Khodakov, Andrei Y.; Chu, Wei; Fongarland, Pascal
- Chemical Reviews, Vol. 107, Issue 5
Investigations of Active Sites for Methane Activation in the Oxidative Coupling Reaction over Pure and Li-Promoted MgO Catalysts
journal, April 1993
- Wu, M. C.; Truong, C. M.; Coulter, K.
- Journal of Catalysis, Vol. 140, Issue 2
Non-Oxidative Coupling Reaction of Methane to Ethane and Hydrogen Catalyzed by the Silica-Supported Tantalum Hydride: (≡SiO) 2 Ta−H
journal, April 2008
- Soulivong, Daravong; Norsic, Sébastien; Taoufik, Mostafa
- Journal of the American Chemical Society, Vol. 130, Issue 15
Conversion of Methanol to Hydrocarbons: Spectroscopic Characterization of Carbonaceous Species Formed over H-ZSM-5
journal, June 2008
- Palumbo, Luisa; Bonino, Francesca; Beato, Pablo
- The Journal of Physical Chemistry C, Vol. 112, Issue 26
Raman microspectroscopy of soot and related carbonaceous materials: Spectral analysis and structural information
journal, July 2005
- Sadezky, A.; Muckenhuber, H.; Grothe, H.
- Carbon, Vol. 43, Issue 8
Decomposition of methane over supported-Ni catalysts: effects of the supports on the catalytic lifetime
journal, September 2001
- Takenaka, Sakae; Ogihara, Hitoshi; Yamanaka, Ichiro
- Applied Catalysis A: General, Vol. 217, Issue 1-2
Determination of the Au active site and surface active species via operando transmission FTIR and isotopic transient experiments on 2.3wt.% Au/TiO2 for the WGS reaction
journal, May 2012
- Wang, Jun; Kispersky, Vincent F.; Nicholas Delgass, W.
- Journal of Catalysis, Vol. 289
Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts
journal, August 2003
- Fu, Q.
- Science, Vol. 301, Issue 5635
Direct catalytic conversion of methane
journal, October 1991
- Poirier, Michel G.; Sanger, Alan R.; Smith, Kevin J.
- The Canadian Journal of Chemical Engineering, Vol. 69, Issue 5
Investigations into the Structure of Nitrogen-Containing CMK-3 and OCM-0.75 Carbon Replicas and the Nature of Surface Functional Groups by Spectroscopic and Sorption Techniques
journal, December 2009
- Lezanska, Maria; Pietrzyk, Piotr; Sojka, Zbigniew
- The Journal of Physical Chemistry C, Vol. 114, Issue 2
Adsorption of Gases in Multimolecular Layers
journal, February 1938
- Brunauer, Stephen; Emmett, P. H.; Teller, Edward
- Journal of the American Chemical Society, Vol. 60, Issue 2, p. 309-319
The Structure and Dimensions of the Benzene Ring
journal, December 1927
- Morse, J. K.
- Proceedings of the National Academy of Sciences, Vol. 13, Issue 12
The Influence of Hydrogen-Permeable Membranes and Pressure on Methane Dehydroaromatization in Packed-Bed Catalytic Reactors
journal, March 2017
- Kee, Benjamin; Karakaya, Canan; Zhu, Huayang
- Industrial & Engineering Chemistry Research, Vol. 56, Issue 13
Identification of molybdenum oxide nanostructures on zeolites for natural gas conversion
journal, April 2015
- Gao, J.; Zheng, Y.; Jehng, J. -M.
- Science, Vol. 348, Issue 6235
Direct, Nonoxidative Conversion of Methane to Ethylene, Aromatics, and Hydrogen
journal, May 2014
- Guo, X.; Fang, G.; Li, G.
- Science, Vol. 344, Issue 6184
IR study on methanol-to-olefin reaction over zeolites with different pore structures and acidities
journal, March 2009
- Park, Ji Won; Seo, Gon
- Applied Catalysis A: General, Vol. 356, Issue 2
The conversion of methane to ethylene and ethane with near total selectivity by low temperature (< 610 � C) oxydehydrogenation over a calcium-nickel-potassium oxide catalyst
journal, January 1990
- Pereira, P.; Lee, S. H.; Somorjai, G. A.
- Catalysis Letters, Vol. 6, Issue 3-6
Fundamentals and Catalytic Applications of CeO 2 -Based Materials
journal, April 2016
- Montini, Tiziano; Melchionna, Michele; Monai, Matteo
- Chemical Reviews, Vol. 116, Issue 10
Catalytic Dehydrocondensation of Methane with CO and CO2toward Benzene and Naphthalene on Mo/HZSM-5 and Fe/Co-Modified Mo/HZSM-5
journal, February 1999
- Ohnishi, Ryuichiro; Liu, Shetian; Dong, Qun
- Journal of Catalysis, Vol. 182, Issue 1
Effects of thermal pretreatment on the redox behaviour of Ce0.5Zr0.5O2: isotopic and spectroscopic studies
journal, December 2001
- Fornasiero, P.; Montini, T.; Graziani, M.
- Physical Chemistry Chemical Physics, Vol. 4, Issue 1
Catalytic Conversion of Methane and Ethylene to Propylene
journal, January 1998
- Lunsford, Jack H.; Qiu, Ping; Rosynek, Michael P.
- The Journal of Physical Chemistry B, Vol. 102, Issue 1
Catalytic reaction of CH4 with CO2 over alumina-supported Pt metals
journal, January 1991
- Solymosi, F.; Kuts�n, Gy.; Erd�helyi, A.
- Catalysis Letters, Vol. 11, Issue 2
Ceria nanoparticles as an efficient catalyst for oxidation of benzylic CH bonds
journal, May 2012
- Akhlaghinia, Batool; Ebrahimabadi, Hossein; Goharshadi, Elaheh K.
- Journal of Molecular Catalysis A: Chemical, Vol. 357
The characterization of activated carbons with oxygen and nitrogen surface groups
journal, January 1997
- Biniak, S.; Szymański, G.; Siedlewski, J.
- Carbon, Vol. 35, Issue 12
Advances in the Development of Novel Cobalt Fischer—Tropsch Catalysts for Synthesis of Long-Chain Hydrocarbons and Clean Fuels
journal, August 2007
- Khodakov, Andrei Y.; Chu, Wei; Fongarland, Pascal
- ChemInform, Vol. 38, Issue 33
Characterization of Cubic Ceria—Zirconia Powders by X-Ray Diffraction and Vibrational and Electronic Spectroscopy.
journal, February 2004
- Sanchez Escribano, Vicente; Fernandez Lopez, Enrique; Panizza, Marta
- ChemInform, Vol. 35, Issue 6
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