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Partial oxidation of methane over rhodium catalysts for power generation applications
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
2005 (English)In: Catalysis Today, ISSN 0920-5861, E-ISSN 1873-4308, Vol. 100, 447-451 p.Article in journal (Refereed) Published
Abstract [en]

The partial oxidation of methane (POM) to syngas, i.e. H-2 and CO, over supported Rh catalysts was investigated at atmospheric pressure. The influence of support material, Rh loading and the presence of water vapor on the methane conversion efficiency and the product gas composition was studied. The catalysts containing ceria in the support material showed the highest activity and formation of H2 and CO. By increasing the Rh loading, a decrease of the ignition temperature was obtained. The addition of water vapor to the reactant gas mixture was found to increase the ignition temperature and the formation of hydrogen, which is favorable for combustion applications where the catalytic POM stage is followed by H-2-stabilized homogeneous combustion.

Place, publisher, year, edition, pages
2005. Vol. 100, 447-451 p.
Keyword [en]
catalytic combustion, partial oxidation of methane, rhodium catalysts, ceria
National Category
Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-6639DOI: 10.1016/j.cattod.2004.09.077ISI: 000229275100041Scopus ID: 2-s2.0-17344365926OAI: oai:DiVA.org:kth-6639DiVA: diva2:11403
Note
QC 20101126. 11th Nordic Symposium on Catalysis. Oulu, FINLAND. MAY 23-25, 2004 Available from: 2006-12-15 Created: 2006-12-15 Last updated: 2011-10-12Bibliographically approved
In thesis
1. Development of catalysts for natural gas-fired gas turbine combustors
Open this publication in new window or tab >>Development of catalysts for natural gas-fired gas turbine combustors
2006 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

Due to continuously stricter regulations regarding emissions from power generation processes, further development of existing gas turbine combustors is essential. A promising alternative to conventional flame combustion in gas turbines is catalytic combustion, which can result in ultralow emission levels of NOx, CO and unburned hydrocarbons. The work presented in this thesis concerns the development of methane oxidation catalysts for gas turbine combustors. The application of catalytic combustion to different combustor concepts is addressed in particular.

The first part of the thesis (Paper I) reports on catalyst development for fuel-lean methane combustion. Supported Pd-based catalysts were investigated at atmospheric pressure. The effect on catalytic activity of diluting the reaction mixture with water and/or carbon dioxide was studied in order to simulate a combustion process with exhaust gas recirculation. The catalytic activity was found to decrease significantly in the presence of water and CO2. However, modifying the catalyst by changing support material can have a considerable impact on the performance.

In the second part of this thesis (Papers II-IV), the development of rhodium catalysts for fuel-rich methane combustion is addressed. The effect of catalyst composition, oxygen-to-fuel ratio and catalyst pre-treatment on the methane conversion and the product gas composition was studied. An experimental investigation at elevated pressures of partial oxidation of methane/oxygen mixtures in exhaust gas-rich environments was also conducted. The most suitable catalyst identified for fuel-rich catalytic combustion of methane, i.e. Rh/Ce-ZrO2, showed benefits such as low light-off temperature, high activity and enhanced hydrogen selectivity.

In the final part of the thesis (Paper V), a numerical investigation of fuel-rich catalytic combustion is presented. Measurements and predictions were compared for partial oxidation of methane in exhaust gas diluted mixtures at elevated pressures. The numerical model was validated for several Rh-based catalysts. The key parameter controlling the catalytic performance was found to be the noble metal dispersion.

Place, publisher, year, edition, pages
Stockholm: KTH, 2006. 67 p.
Series
Trita-KET, ISSN 1104-3466 ; R232
Keyword
AZEP, catalytic combustion, CPO, methane oxidation, palladium, rhodium, support effect
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-4239 (URN)91-7178-543-4 (ISBN)978-91-7178-543-5 (ISBN)
Public defence
2006-12-19, D2, D, Lindstedtsvägen 5, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20110125Available from: 2006-12-15 Created: 2006-12-15 Last updated: 2011-01-25Bibliographically approved
2. Development of methane oxidation catalysts for different gas turbine combustor concepts
Open this publication in new window or tab >>Development of methane oxidation catalysts for different gas turbine combustor concepts
2005 (English)Licentiate thesis, comprehensive summary (Other scientific)
Abstract [en]

Due to continuously stricter regulations regarding emissions from power generation processes, development of existing gas turbine combustors is essential. A promising alternative to conventional flame combustion in gas turbines is catalytic combustion, which can result in ultra low emission levels of NOx, CO and unburned hydrocarbons. The work presented in this thesis concerns the development of methane oxidation catalysts for gas turbine combustors. The application of catalytic combustion to different combustor concepts is addressed in particular.

The first part of the thesis (Paper I) reports on catalyst development for fuel-lean methane combustion. The effect on catalytic activity of diluting the reaction mixture with water and carbon dioxide was studied in order to simulate a combustion process with exhaust gas recirculation. Palladium-based catalysts were found to exhibit the highest activity for methane oxidation under fuel-lean conditions. However, the catalytic activity was significantly decreased by adding water and CO2, resulting in unacceptably high ignition temperatures of the fuel.

In the second part of this thesis (Paper II), the development of rhodium catalysts for fuel-rich methane combustion is addressed. The effect of water addition on the methane conversion and the product gas composition was studied. A significant influence of the support material and Rh loading on the catalytic behavior was found. The addition of water influenced both the low-temperature activity and the product gas composition.

Place, publisher, year, edition, pages
Stockholm: KTH, 2005. 35 p.
Series
Trita-KET, ISSN 1104-3466 ; 211
Keyword
Chemical engineering, catalytic combustion, methane oxidation, ceria, palladium, platinum, rhodium, TPO, Kemiteknik
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-311 (URN)
Presentation
2005-04-15, Teknikringen 42, Stockholm, 10:00
Supervisors
Note
QC 20101126Available from: 2005-07-18 Created: 2005-07-18 Last updated: 2010-11-26Bibliographically approved

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