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Supported palladium-platinum catalyst for methane combustion at high pressure
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 Industrial Engineering and Management (ITM), Energy Technology, Heat and Power Technology.
KTH, School of Industrial Engineering and Management (ITM), Energy Technology, Heat and Power Technology.
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2005 (English)In: Catalysis Today, ISSN 0920-5861, E-ISSN 1873-4308, Vol. 100, 479-483 p.Article in journal (Refereed) Published
Abstract [en]

Catalytic combustion of methane over a supported bimetallic Pd-Pt catalyst and a monometallic Pd catalyst has been investigated experimentally. Two different reactor configurations were used in the study, i.e. a tubular lab-scale reactor working at atmospheric pressure and a high-pressure reactor working at up to 15 bar. The results showed that the bimetallic catalyst has a clearly more stable activity during steady-state operation compare to the palladium only catalyst. The activity of the bimetallic catalyst was slightly higher than for the palladium catalyst. These results were established in both test facilities. Further, the impact of pressure on the combustion activity has been studied experimentally. The tests showed that the methane conversion decreases with increasing pressure. However, the impact of pressure is more prominent at lower pressures and levels out for pressures above 10 bar

Place, publisher, year, edition, pages
2005. Vol. 100, 479-483 p.
Keyword [en]
high pressure, palladium, platinum, bimetallic catalysts, methane, combustion stability
National Category
Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-6564DOI: 10.1016/j.cattod.2004.08.018ISI: 000229275100047Scopus ID: 2-s2.0-17344370162OAI: oai:DiVA.org:kth-6564DiVA: diva2:11310
Note
QC 20100916. 11th Nordic Symposium on Catalysis. Oulu, FINLAND. MAY 23-25, 2004 Available from: 2006-12-11 Created: 2006-12-11 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Bimetallic Palladium Catalysts for Methane Combustion in Gas Turbines
Open this publication in new window or tab >>Bimetallic Palladium Catalysts for Methane Combustion in Gas Turbines
2006 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

Catalytic combustion is a promising combustion technology for gas turbines, which results in ultra low emission levels of nitrogen oxides (NOx), carbon monoxide (CO) and unburned hydrocarbons (UHC). Due to the low temperature achieved in catalytic combustion almost no thermal NOx is formed. This thesis is concentrated on the first stage in a catalytic combustion chamber, i.e. the ignition catalyst. The catalyst used for this application is often a supported palladium based catalyst due to its excellent activity for methane combustion. However, this type of catalyst has a serious drawback; the methane conversion decreases severely with time during operation. The unstable activity will result in increasing difficulties to ignite the fuel. The parameters that govern the poor stability and other features of the palladium catalysts are discussed in the thesis.

The objective of the work is to improve the catalytic performance of supported palladium catalysts, with focus on stabilising the methane conversion. A large number of different bimetallic palladium catalysts have been evaluated, where the influence of co-metals, molar ratio and support material is addressed. Results from the activity tests of methane combustion showed that it is possible to stabilise the activity by adding certain co-metals into the palladium catalyst. An extensive characterisation study has been carried out on the various bimetallic catalysts in order to gain a better understanding of how their morphology and physicochemical properties determine the various patterns of combustion behaviour.

The environment inside a gas turbine combustor is very harsh for a catalyst. Since the stability of the catalyst is of great importance for ignition catalysts, it is essential to evaluate the risk of deactivation. In this work special emphasis has been given to thermal deactivation, water inhibition and sulphur poisoning. It was found that a bimetallic Pd Pt catalyst is significantly more tolerant to the various deactivation processes investigated than the monometallic palladium catalyst.

Finally, the influence of pressure on the catalytic performance has been investigated. The catalysts were assessed at more realistic conditions for gas turbines, in a high-pressure test facility with 100 kW fuel power.

Place, publisher, year, edition, pages
Stockholm: KTH, 2006. 80 p.
Series
Trita-KET, ISSN 1104-3466 ; R231
Keyword
activity, bimetal, catalytic combustion, DRIFTS, EDS, gas turbine, methane, morphology, palladium, platinum, pressure, PXRD, stability, TEM, TPO, XPS
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-4222 (URN)91-7178-529-9 (ISBN)978-91-7178-529-9 (ISBN)
Public defence
2006-12-15, D3, Lindstedtsvägen 5, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20100916Available from: 2006-12-11 Created: 2006-12-11 Last updated: 2010-09-16Bibliographically approved
2. Experimental Investigations of High Pressure Catalytic Combustion for Gas Turbine Applications
Open this publication in new window or tab >>Experimental Investigations of High Pressure Catalytic Combustion for Gas Turbine Applications
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This work is devoted to generate knowledge and high quality experimental data of catalytic combustion at operational gas turbine conditions.

The initial task of the thesis work was to design and construct a high pressure combustion test facility, where the catalytic combustion experiments can be performed at real gas turbine conditions. With this in mind, a highly advanced combustion test facility has been designed, constructed and tested. This test facility is capable of simulating combustion conditions relevant to a wide range of operating gas turbine conditions and different kinds of fuel gases. The shape of the combustor (test section) is similar to a “can” type gas turbine combustor, but with significant differences in its type of operation. The test combustor is expected to operate at near adiabatic combustion conditions and there will be no additions of cooling, dilution or secondary supply of air into the combustion process. The geometry of the combustor consists of three main zones such as air/fuel mixing zone, catalytic reaction zone and downstream gas phase reaction zone with no difference of the mass flow at inlet and exit. The maximum capacity of the test facility is 100 kW (fuel power) and the maximum air flow rate is 100g/s.

The significant features of the test facility are counted as its operational pressure range (1 – 35 atm), air inlet temperatures (100 – 650 °C), fuel flexibility (LHV 4 - 40 MJ/m3) and air humidity (0 – 30% kg/kg of air). Given these features, combustion could be performed at any desired pressure up to 35 bars while controlling other parameters independently. Fuel flexibility of the applications was also taken into consideration in the design phase and proper measures have been taken in order to utilize two types of targeted fuels, methane and gasified biomass.

Experimental results presented in this thesis are the operational performances of highly active precious metal catalysts (also called as ignition catalysts) and combinations of precious metal, perovskites and hexaaluminate catalysts (also called as fully catalytic configuration). Experiments were performed on different catalytic combustor configurations of various types of catalysts with methane and simulated gasified biomass over the full range of pressure. The types of catalysts considered on the combustor configurations are palladium on alumina (Pd/AL2O3), palladium lanthanum hexaaluminate (PdLaAl11O19), platinum on alumina (Pt/AL2O3),and palladium:platinum bi-metal on alumina (Pd:Pt/AL2O3). The influence of pressure, inlet temperature, flow velocity and air fuel ratio on the ignition, combustion stability and emission generation on the catalytic system were investigated and presented.

Combustion catalysts were developed and provided mainly by the project partner, the Division of Chemical Technology, KTH. Division of Chemical Reaction Technology, KTH and Istituto di Ricerche sulla Combustione (CNR) Italy were also collaborated with some of the experimental investigations by providing specific types of catalysts developed by them for the specific conditions of gas turbine requirements.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2013. xxiv, 122 p.
Series
TRITA-KRV, ISSN 1100-7990 ; 13:10
Keyword
Gas Turbine Combustion, Catalytic Combustion, High Pressure, Ultra-low emissions
National Category
Engineering and Technology
Research subject
SRA - Energy
Identifiers
urn:nbn:se:kth:diva-134445 (URN)978-91-7501-937-6 (ISBN)
Public defence
2013-12-11, M3, Brinellvägen 64, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Swedish Energy Agency
Note

QC 20131125

Available from: 2013-11-25 Created: 2013-11-25 Last updated: 2017-03-07Bibliographically approved
3. Catalytic Combustion in Gas Turbines: Experimental Study on Gasified Biomass Utilization
Open this publication in new window or tab >>Catalytic Combustion in Gas Turbines: Experimental Study on Gasified Biomass Utilization
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Environmental and geopolitical concerns encourage societies towards the utilization of renewable energy sources (RES). Photovoltaic and wind power can produce electricity directly, although their intermittent characteristic negatively affects the security and safety of the energy supply chain; moreover, in order to be viable it is necessary to establish energy storage systems and to find mechanisms to adapt the power distribution grid to larger production variability. In contrast, biomass (a carbon neutral fuel if adequately managed) can be stored, is relatively widely available, and after simple treatments can be gasified and ready to be used for power production. Correspondingly, gas turbines are a well-established technology that first became relevant in industrial applications and power production since 1940’s. The use of biomass in gas turbines is an important step forward towards more sustainable power production; however, this combination presents some technical challenges that have yet to be overcome.

Gasified biomass is generally a gas with low or medium heating value that is usually composed of a mixture of gases such as CO, H2, CH4, CO2, and N2 as well as other c60*6nents in small fractions. Its firing in standard gas turbine combustors might be unstable at certain load conditions. Moreover, gasified biomass contains undesirable compounds; in particular the nitrogen-containing compounds that may produce elevated NOx emissions once the biomass is burned.

Catalytic combustion is an alternative for using gasified biomass in a gas turbine, and it is investigated in this study. Using catalytic combustion is possible to burn such a mixture of gases under very lean conditions, extending the normal flammability limits, reducing the maximum temperature of the reaction zone, and thus reducing the thermal NOx formation. It also reduces the vibration levels, and it is possible to avoid fuel-NOx formation using alternative catalytic techniques, such as Selective Catalytic Oxidation (SCO).

In the present study the feasibility of using catalytic combustion in a gas turbine combustor is evaluated. The tests performed indicate the necessity of using hybrid combustion chamber concepts to achieve turbine inlet temperatures levels of modern gas turbines. The different catalytic burning characteristic of H2, CO and CH4 was evaluated and different techniques were applied to equalize their burning behaviour such as the diffusion barrier, and partially coated catalyst. Fuel-NOx is another subject treated in this work, where a Selective Catalytic Oxidation (SCO) technique is applied reaching up to 42% of fuel NOx reduction. Finally, the use of Catalytic Partial Oxidation (CPO) of methane was experimentally investigated.

In this study, two one-of-a-kind test facilities were used directly, namely the high-pressure test facility and the pilot scale test facility. This gives a unique characteristic to the study performed. Finally, the catalytic combustion approach allows the utilization of gasified biomass with some restrictions depending on whether it is a Catalytic Lean, Catalytic Rich or Catalytic Partial Oxidation (CPO) approach.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2014. xiv, 152 p.
Series
TRITA-KRV, ISSN 1100-7990 ; 14:01
National Category
Energy Engineering
Research subject
Energy Technology
Identifiers
urn:nbn:se:kth:diva-144102 (URN)978-91-7595-048-8 (ISBN)
Public defence
2014-04-11, Sal B1, Brinellvägen 23, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Sida - Swedish International Development Cooperation Agency, 5110-2003-06929/2152-1
Note

QC 201140409

Available from: 2014-04-09 Created: 2014-04-09 Last updated: 2014-04-11Bibliographically approved

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