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Development of methane oxidation catalysts for different gas turbine combustor concepts
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
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 [en]
Chemical engineering, catalytic combustion, methane oxidation, ceria, palladium, platinum, rhodium, TPO
Keyword [sv]
Kemiteknik
National Category
Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-311OAI: oai:DiVA.org:kth-311DiVA: diva2:8871
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
List of papers
1. Catalytic combustion of methane in steam and carbon dioxide-diluted reaction mixtures
Open this publication in new window or tab >>Catalytic combustion of methane in steam and carbon dioxide-diluted reaction mixtures
2006 (English)In: Applied Catalysis, ISSN 0166-9834, E-ISSN 1873-3867, Vol. 312, 95-101 p.Article in journal (Refereed) Published
Abstract [en]

Supported palladium catalysts have been tested for methane combustion under lean conditions in the temperature range of 200-800 degrees C. The effect of diluting the reaction mixture with high amounts of water and carbon dioxide was studied in order to simulate a combustion process with exhaust gas recirculation. The influence of support material, i.e. ZrO2 or doped CeO2, on the catalytic performance was also investigated.

The catalyst support material was found to influence the light-off temperature significantly, which increased in the following order: Pd/ZrO2 < Pd/Zr-CeO2 < Pd/La-CeO2. The order of activity changed at higher temperatures resulting in Pd/La-CeO2 being the most active catalyst above 670 degrees C. This catalyst also shows a more stable performance with no distinct deactivation occurring at higher temperatures during cooling.

Both water and CO2 were found to have a negative influence on the catalytic activity. The inhibitory effect was, however, more pronounced for water. This inhibitory effect was present in the entire temperature range investigated. Adding CO2 in the presence of water resulted in conversions similar to the ones observed when feeding water alone for Pd/ZrO2 and Pd/La-CeO2, On the contrary, the activity of Pd/Zr-CeO2 was further decreased when co-feeding water and CO2.

Keyword
catalytic combustion, palladium, TPO, AZEP, water inhibition, CO2 inhibition
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-6638 (URN)000240639000012 ()2-s2.0-33747828180 (Scopus ID)
Note
QC 20101126Available from: 2006-12-15 Created: 2006-12-15 Last updated: 2017-12-14Bibliographically approved
2. Partial oxidation of methane over rhodium catalysts for power generation applications
Open this publication in new window or tab >>Partial oxidation of methane over rhodium catalysts for power generation applications
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.

Keyword
catalytic combustion, partial oxidation of methane, rhodium catalysts, ceria
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-6639 (URN)10.1016/j.cattod.2004.09.077 (DOI)000229275100041 ()2-s2.0-17344365926 (Scopus ID)
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: 2017-12-14Bibliographically approved

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Citation style
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