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Fuel-rich catalytic combustion of methane in zero emissions power generation processes
KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
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2006 (English)In: Catalysis Today, ISSN 0920-5861, E-ISSN 1873-4308, Vol. 117, no 4, 447-453 p.Article in journal (Refereed) Published
Abstract [en]

A novel catalytic combustion concept for zero emissions power generation has been investigated. Catalysts consisting of Rh supported on ZrO2, Ce-ZrO2 or alpha-Al2O3 were prepared and tested under fuel-rich conditions, i.e. for catalytic partial oxidation (CPO) of methane. The experiments were performed in a subscale gas-turbine reactor operating at 5 bar with exhaust gas-diluted feed mixtures.The catalyst support material was found to influence the light-off temperature significantly, which increased in the following order Rh/Ce-ZrO2 < Rh/ZrO2 < Rh/alpha-Al2O3. The Rh loading, however, only had a minor influence. The high activity of Rh/Ce-ZrO2 is probably related to the high dispersion of Rh on Ce-ZrO2 and the high oxygen mobility of this support compared to pure ZrO2. The formation of hydrogen was also found to increase over the catalyst containing ceria in the support material.

Place, publisher, year, edition, pages
2006. Vol. 117, no 4, 447-453 p.
Keyword [en]
catalytic combustion, catalytic partial oxidation (CPO) of methane, AZEP, rhodium catalysts, ceria
National Category
Chemical Engineering
URN: urn:nbn:se:kth:diva-6641DOI: 10.1016/j.cattod.2006.06.010ISI: 000241085000009ScopusID: 2-s2.0-33748617867OAI: diva2:11405
QC 20110125Available from: 2006-12-15 Created: 2006-12-15 Last updated: 2011-09-28Bibliographically 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.
Trita-KET, ISSN 1104-3466 ; R232
AZEP, catalytic combustion, CPO, methane oxidation, palladium, rhodium, support effect
National Category
Chemical Engineering
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
QC 20110125Available from: 2006-12-15 Created: 2006-12-15 Last updated: 2011-01-25Bibliographically approved

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