Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator
Abstract
Abstract Die Umwandlung von Methan in Alkohole unter milden Reaktionsbedingungen ist eine vielversprechende Technologie für die Nutzung abgelegener Methanvorkommen. Die flüssigen Alkohole können in Pipelines transportiert und zu wertvolleren Chemikalien weiterverarbeitet werden. Hier wird gezeigt, dass ein Katalysator aus Nickeloxidpartikeln auf einen Ceroxid‐Zirconiumoxid‐Träger (NiO/CZ) Methan in einem einzigen, kontinuierlich betriebenen Reaktor zu Methanol und Ethanol umwandeln kann. Die Reaktion geschieht bei milden Temperaturen (723 K) mit O 2 als Oxidationsmittel. Die Produktion von Alkoholen erfordert die Gegenwart von Wasserdampf, um die vollständige Oxidation zu CO 2 zu unterdrücken. Die Synergie zwischen Lewis‐aciden NiO‐Partikeln und dem redoxaktiven Ceroxid‐Zirconiumoxid‐Träger ermöglicht die ungewöhnliche Reaktivität dieses Katalysators.
- Authors:
-
- School of Chemical &, Biomolecular Engineering Georgia Institute of Technology 311 Ferst Drive NW Atlanta GA 30332 USA
- National Renewable Energy Laboratory Golden CO USA
- Environmental Molecular Sciences Laboratory Pacific Northwest National Lab Richland WA USA
- National Synchrotron Light Source II Brookhaven National Laboratory Upton NY USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1394848
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Angewandte Chemie
- Additional Journal Information:
- Journal Name: Angewandte Chemie Journal Volume: 129 Journal Issue: 44; Journal ID: ISSN 0044-8249
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Okolie, Chukwuemeka, Belhseine, Yasmeen F., Lyu, Yimeng, Yung, Matthew M., Engelhard, Mark H., Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator. Germany: N. p., 2017.
Web. doi:10.1002/ange.201704704.
Okolie, Chukwuemeka, Belhseine, Yasmeen F., Lyu, Yimeng, Yung, Matthew M., Engelhard, Mark H., Kovarik, Libor, Stavitski, Eli, & Sievers, Carsten. Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator. Germany. https://doi.org/10.1002/ange.201704704
Okolie, Chukwuemeka, Belhseine, Yasmeen F., Lyu, Yimeng, Yung, Matthew M., Engelhard, Mark H., Kovarik, Libor, Stavitski, Eli, and Sievers, Carsten. Tue .
"Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator". Germany. https://doi.org/10.1002/ange.201704704.
@article{osti_1394848,
title = {Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator},
author = {Okolie, Chukwuemeka and Belhseine, Yasmeen F. and Lyu, Yimeng and Yung, Matthew M. and Engelhard, Mark H. and Kovarik, Libor and Stavitski, Eli and Sievers, Carsten},
abstractNote = {Abstract Die Umwandlung von Methan in Alkohole unter milden Reaktionsbedingungen ist eine vielversprechende Technologie für die Nutzung abgelegener Methanvorkommen. Die flüssigen Alkohole können in Pipelines transportiert und zu wertvolleren Chemikalien weiterverarbeitet werden. Hier wird gezeigt, dass ein Katalysator aus Nickeloxidpartikeln auf einen Ceroxid‐Zirconiumoxid‐Träger (NiO/CZ) Methan in einem einzigen, kontinuierlich betriebenen Reaktor zu Methanol und Ethanol umwandeln kann. Die Reaktion geschieht bei milden Temperaturen (723 K) mit O 2 als Oxidationsmittel. Die Produktion von Alkoholen erfordert die Gegenwart von Wasserdampf, um die vollständige Oxidation zu CO 2 zu unterdrücken. Die Synergie zwischen Lewis‐aciden NiO‐Partikeln und dem redoxaktiven Ceroxid‐Zirconiumoxid‐Träger ermöglicht die ungewöhnliche Reaktivität dieses Katalysators.},
doi = {10.1002/ange.201704704},
journal = {Angewandte Chemie},
number = 44,
volume = 129,
place = {Germany},
year = {Tue Sep 26 00:00:00 EDT 2017},
month = {Tue Sep 26 00:00:00 EDT 2017}
}
https://doi.org/10.1002/ange.201704704
Works referenced in this record:
Hydrogen and synthesis gas by steam- and C02 reforming
journal, January 2002
- Rostrup-Nielsen, Jens R.; Sehested, Jens; Nørskov, Jens K.
- Advances in Catalysis, Vol. 47, p. 65-139
Selective Oxidation of Methane by the Bis(μ-oxo)dicopper Core Stabilized on ZSM-5 and Mordenite Zeolites
journal, February 2005
- Groothaert, Marijke H.; Smeets, Pieter J.; Sels, Bert F.
- Journal of the American Chemical Society, Vol. 127, Issue 5
Oxidative Methane Upgrading
journal, July 2012
- Hammond, Ceri; Conrad, Sabrina; Hermans, Ive
- ChemSusChem, Vol. 5, Issue 9
Rationalization of the Catalytic Behavior of Lanthanide Oxides and Praseodymium Molybdates in Total and Selective Oxidation of Isobutene
journal, December 2001
- De Smet, Frédéric; Ruiz, Patricio; Delmon, Bernard
- The Journal of Physical Chemistry B, Vol. 105, Issue 49
Platinum Catalysts for the High-Yield Oxidation of Methane to a Methanol Derivative
journal, April 1998
- Periana, R. A.
- Science, Vol. 280, Issue 5363
Direct catalytic conversion of methane to acetic acid in an aqueous medium
journal, April 1994
- Lin, Minren; Sen, Ayusman
- Nature, Vol. 368, Issue 6472
Mechanistic Studies on the Hydroxylation of Methane by Methane Monooxygenase
journal, June 2003
- Baik, Mu-Hyun; Newcomb, Martin; Friesner, Richard A.
- Chemical Reviews, Vol. 103, Issue 6
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
Oxidation of methane to methanol on the surface of FeZSM-5 zeolite
journal, April 2013
- Starokon, Eugeny V.; Parfenov, Mikhail V.; Arzumanov, Sergey S.
- Journal of Catalysis, Vol. 300
Kinetics of hydrogen activation on ceria–zirconia
journal, September 2015
- Schimming, Sarah M.; Foo, Guo Shiou; LaMont, Onaje D.
- Journal of Catalysis, Vol. 329
Status and prospects in higher alcohols synthesis from syngas
journal, January 2017
- Luk, Ho Ting; Mondelli, Cecilia; Ferré, Daniel Curulla
- Chemical Society Reviews, Vol. 46, Issue 5
A [Cu 2 O] 2+ core in Cu-ZSM-5, the active site in the oxidation of methane to methanol
journal, October 2009
- Woertink, Julia S.; Smeets, Pieter J.; Groothaert, Marijke H.
- Proceedings of the National Academy of Sciences, Vol. 106, Issue 45
Hydrogen production by catalytic cracking of methane over nickel gauze under periodic reactor operation
journal, January 2001
- Monnerat, B.; Kiwi-Minsker, L.; Renken, A.
- Chemical Engineering Science, Vol. 56, Issue 2
A Spectroscopic Characterization of the Reduction of Ceria from Electronic Transitions of Intrinsic Point Defects
journal, June 1994
- Binet, Claude; Badri, Ahmed; Lavalley, Jean-Claude
- The Journal of Physical Chemistry, Vol. 98, Issue 25
Catalytic and spectroscopic studies of Ag1.2V3CeyO8+x catalysts for oxidation of toluene
journal, October 1991
- Yan, Z.
- Journal of Catalysis, Vol. 131, Issue 2
Hydrodeoxygenation of Guaiacol over Ceria-Zirconia Catalysts
journal, June 2015
- Schimming, Sarah M.; LaMont, Onaje D.; König, Michael
- ChemSusChem, Vol. 8, Issue 12
Iron complexes in zeolites as a new model of methane monooxygenase
journal, July 1997
- Panov, G. I.; Sobolev, V. I.; Dubkov, K. A.
- Reaction Kinetics and Catalysis Letters, Vol. 61, Issue 2
Mixed alcohols synthesis from syngas over Cs- and Ni-modified Cu/CeO2 catalysts
journal, February 2013
- Liu, Yanyong; Murata, Kazuhisa; Inaba, Megumu
- Fuel, Vol. 104
Direct Catalytic Conversion of Methane to Methanol in an Aqueous Medium by using Copper-Promoted Fe-ZSM-5
journal, April 2012
- Hammond, Ceri; Forde, Michael M.; Ab Rahim, Mohd Hasbi
- Angewandte Chemie International Edition, Vol. 51, Issue 21
Water-gas shift: in situ spectroscopic studies of noble metal promoted ceria catalysts for CO removal in fuel cell reformers and mechanistic implications
journal, May 2004
- Jacobs, Gary; Patterson, Patricia M.; Williams, Leann
- Applied Catalysis A: General, Vol. 262, Issue 2
C−H Bond Activation and Organometallic Intermediates on Isolated Metal Centers on Oxide Surfaces
journal, February 2010
- Coperet, Christophe
- Chemical Reviews, Vol. 110, Issue 2
Direct conversion of methane to methanol
journal, September 1997
- Raja, Robert; Ratnasamy, Paul
- Applied Catalysis A: General, Vol. 158, Issue 1-2
Heterolytic Splitting of H 2 and CH 4 on γ-Alumina as a Structural Probe for Defect Sites
journal, November 2006
- Joubert, Jérôme; Salameh, Alain; Krakoviack, Vincent
- The Journal of Physical Chemistry B, Vol. 110, Issue 47
Bio-inspired oxidation of methane in water catalyzed by N-bridged diiron phthalocyanine complex
journal, January 2008
- Sorokin, Alexander B.; Kudrik, Evgeny V.; Bouchu, Denis
- Chemical Communications, Issue 22
Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
journal, June 2015
- Grundner, Sebastian; Markovits, Monica A. C.; Li, Guanna
- Nature Communications, Vol. 6, Issue 1
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 to Methanol in an Aqueous Medium by using Copper-Promoted Fe-ZSM-5
journal, April 2012
- Hammond, Ceri; Forde, Michael M.; Ab Rahim, Mohd Hasbi
- Angewandte Chemie, Vol. 124, Issue 21
Advances in low temperature Fischer-Tropsch synthesis
journal, January 1995
- Jager, B.; Espinoza, R.
- Catalysis Today, Vol. 23, Issue 1
Diiron N-bridged species bearing phthalocyanine ligand catalyzes oxidation of methane, propane and benzene under mild conditions
journal, October 2008
- Kudrik, Evgeny V.; Afanasiev, Pavel; Bouchu, Denis
- Journal of Porphyrins and Phthalocyanines, Vol. 12, Issue 10
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
Pre-reforming of natural gas on a Ni catalyst
journal, March 2005
- Sperle, Thomas; Chen, De; Lødeng, Rune
- Applied Catalysis A: General, Vol. 282, Issue 1-2
Oxidation of methane by a biological dicopper centre
journal, April 2010
- Balasubramanian, Ramakrishnan; Smith, Stephen M.; Rawat, Swati
- Nature, Vol. 465, Issue 7294
Selective oxidation of methane to synthesis gas using transition metal catalysts
journal, March 1990
- Ashcroft, A. T.; Cheetham, A. K.; Foord, J. S.
- Nature, Vol. 344, Issue 6264
Conversion of methane to methanol on copper-containing small-pore zeolites and zeotypes
journal, January 2015
- Wulfers, M. J.; Teketel, S.; Ipek, B.
- Chemical Communications, Vol. 51, Issue 21
Generation of active oxygen species on solid surfaces. Opportunity for novel oxidation technologies over zeolites
journal, June 1998
- Panov, Gennady I.; Uriarte, Anthony K.; Rodkin, Mikhail A.
- Catalysis Today, Vol. 41, Issue 4
Synthesis of Ethanol via Syngas on Cu/SiO 2 Catalysts with Balanced Cu 0 –Cu + Sites
journal, May 2012
- Gong, Jinlong; Yue, Hairong; Zhao, Yujun
- Journal of the American Chemical Society, Vol. 134, Issue 34
Infrared Study of Oxygen Adsorption and Activation on Cerium–Zirconium Mixed Oxides
journal, November 2000
- Descorme, C.; Madier, Y.; Duprez, D.
- Journal of Catalysis, Vol. 196, Issue 1