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Catalytic Combustion in Gas Turbines: Experimental Study on Gasified Biomass Utilization
KTH, School of Industrial Engineering and Management (ITM), Energy Technology, Heat and Power Technology.
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: urn:nbn:se:kth:diva-144102ISBN: 978-91-7595-048-8 (print)OAI: oai:DiVA.org:kth-144102DiVA: diva2:711124
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
List of papers
1. Catalytic Partial Oxidation of Natural Gas in Gas Turbine Applications
Open this publication in new window or tab >>Catalytic Partial Oxidation of Natural Gas in Gas Turbine Applications
2013 (English)In: Proceedings of ASME Turbo Expo 2013, 2013Conference paper, Published paper (Other academic)
Abstract [en]

The demands of emissions, combustion efficiency over a wider operational range, and fuel flexibility for industrial gas turbine applications are expected to increase in the coming years. Currently, it is common the use of a stabilizing piloting diffusion flame during part load operation, this flame is accountable for an important part of the thermal NOx emissions on partial load, and in some cases also at full load operation. On the other hand Catalytic Partial Oxidation (CPO) of natural gas is a technique used in petrochemical industry for the Fischer-Tropsch process and for H2 production, and is based in the production of Syn-Gas rich in H2 and CO.

The present work explores the possibility to use the CPO of natural gas in industrial gas turbine applications, it is based in experiments performed between 5 and 13 bar using an arrangement of Rh based catalyst and CH4. The experiments were done at the Catalytic Combustion High Pressure Test Facility, at the Royal Institute of Technology (KTH) in Sweden. The gas produced leaves the CPO reactor between 700 and 850 °C and it is rich in H2 and CO. It was found that the most important parameter after reaching the light off temperature in the CPO reactor is the equivalence ratio Φ, which evidences the kinetically controlled regime in the Rh catalyst that depends on O2 availability. The H2/CO ratio is close to the theoretical value of 2 and the selectivity towards H2 and CO are 90% and 95% respectively while the CH4 conversion reached approximately 55%.

Pressure on the other hand had a small negative influence in the tested pressure range and it is more relevant at richer fuel conditions (high equivalence ratios). The CPO process had shown that it is relatively easy to control the operation temperature of the catalyst. This temperature is kept below the maximum allowed by reducing the O2 availability.

The high temperature Syn-Gas gas produced through CPO process could be burnt in the downstream of the catalysts steadily at flame temperatures below the thermal-NOx threshold. The CPO reactor could provide the flame stabilization function at a wide range of operational conditions, and replace the diffusion piloting flame. This approach could cope with NOx and CO emissions in a wider operational range and offers the possibility of using different fuels as the reaction controlling factor is O2 availability. Furthermore, an initial design of a possible combustion strategy downstream of the CPO reactor is also presented.

National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-134606 (URN)10.1115/GT2013-95338 (DOI)2-s2.0-84890189567 (Scopus ID)978-0-7918-5511-9 (ISBN)
Conference
ASME Turbo Expo 2013, June 3-7, 2013, San Antonio, Texas
Note

QC 20131125

Available from: 2013-11-25 Created: 2013-11-25 Last updated: 2014-04-09Bibliographically approved
2. Staged Lean Catalytic Combustion of Gasified Biomass for Gas Turbine Applications: an Experimental Approach to Investigate Performance of Catalysts
Open this publication in new window or tab >>Staged Lean Catalytic Combustion of Gasified Biomass for Gas Turbine Applications: an Experimental Approach to Investigate Performance of Catalysts
2013 (English)In: Proceedings of ASME Turbo Expo 2013, 2013Conference paper, Published paper (Other academic)
Abstract [en]

Emission demands for gas turbine utilization will become more stringent in the coming years. Currently different techniques are used to reach low levels of NOx emissions. One possible solution is the Staged Lean Catalytic Combustion. In this concept a catalysts arrangement is used to generate high temperature combustion gases. The high temperature gases could be used to feed a second combustion stage in which more fuel is injected.

In this work a series of experiments were performed at the Catalytic Combustion High Pressure Test Facility at the Royal Institute of Technology (KTH) in Sweden. The fuel used was a simulated gasified biomass and the catalytic combustor consisted of an arrangement of different catalysts, e.g. bimetallic, hexaaluminates, and perovskites catalysts. These were used as, ignition catalyst, medium temperature catalyst and high temperature catalyst respectively.

The tests were performed between 5 and 13.5 bar, and the overall conversion varied between 60% and 70% and the temperature of flue gases could reach 750°C and contains high level of oxygen. The determining factor to control the exit gas temperature was the richness of the mixture (λ value). On the other hand, the increased pressure had a moderate negative effect in the overall fuel conversion. This effect is stronger at leaner mixtures compared to richer ones. Moreover, λ value and also pressure affected the temperature distribution along the reactor.

The utilization of a lean catalytic combustion approach makes possible the use of a post catalytic combustion. In this region additional fuel is injected to fully burn the exiting gases and increase the exit temperature to the desired levels. This staged lean catalytic combustion approach could resemble moderate levels exhaust gas recirculation techniques and/or high air temperature combustion and it is also briefly examined in the present work.

National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-134605 (URN)10.1115/GT2013-95339 (DOI)2-s2.0-84890216723 (Scopus ID)978-0-7918-5513-3 (ISBN)
Conference
ASME Turbo Expo 2013, June 3-7, 2013, San Antonio, Texas
Note

QC 20131125

Available from: 2013-11-25 Created: 2013-11-25 Last updated: 2014-04-09Bibliographically approved
3. Catalytic Combustion of Gasified Biomass for Gas Turbine Applications: Experimental Study for Reducing Fuel NOx Formation
Open this publication in new window or tab >>Catalytic Combustion of Gasified Biomass for Gas Turbine Applications: Experimental Study for Reducing Fuel NOx Formation
2005 (English)In: 14th European Biomass Conference & Exhibition, 2005, Vol. 100Conference paper, Published paper (Refereed)
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-144103 (URN)
Conference
14th European Biomass Conference & Exhibition
Note

QC 20140409

Available from: 2014-04-09 Created: 2014-04-09 Last updated: 2014-04-09Bibliographically approved
4. High-pressure catalytic combustion of gasified biomass in a hybrid combustor
Open this publication in new window or tab >>High-pressure catalytic combustion of gasified biomass in a hybrid combustor
Show others...
2005 (English)In: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 293, no 1-2, 129-136 p.Article in journal (Refereed) Published
Abstract [en]

Catalytic combustion of synthetic gasified biomass was conducted in a high-pressure facility at pressures ranging from 5 to 16 bars. The catalytic combustor design considered was a hybrid monolith (400 cpsi, diameter 3.5 cm, length 3.6 cm and every other channel coated). The active phase consisted of 1 wt.% Pt/gamma-Al2O3 With wash coat loading of total monolith 15 wt.%. In the interpretation of the experiments, a twodimensional boundary layer model was applied successfully to model a single channel of the monolith. At constant inlet velocity to the monolith the combustion efficiency decreased with increasing pressure. A multi-step surface mechanism predicted that the flux of carbon dioxide and water from the surface increased with pressure. However, as the pressure (i.e. the Reynolds number) was increased, unreacted gas near the center of the channel penetrated significantly longer into the channel compared to lower pressures. For the conditions studied (lambda = 46, T-in = 218-257 degrees C and residence time similar to 5 ms), conversion of hydrogen and carbon monoxide were diffusion limited after ignition, while methane never ignited and was kinetically controlled. According to the kinetic model surface coverage of major species changed from CO, H and CO2 before ignition to O, OH, CO2 and free surface sites after ignition. The model predicted further that for constant mass flow combustion efficiency increased with pressure, and was more pronounced at lower pressures (2.5-10 bar) than at higher pressures (> 10 bar).

Keyword
catalytic combustion, gasified biomass, platinum, high pressure, catalytically stabilized combustion, CHEMKIN
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-7571 (URN)10.1016/j.apcata.2005.07.003 (DOI)000232436200014 ()2-s2.0-24644491216 (Scopus ID)
Note
QC 20100916Available from: 2007-11-06 Created: 2007-11-06 Last updated: 2014-04-09Bibliographically approved
5. Catalytic Combustion of Gasified Biomass for Gas Turbine Applications: Experimental Investigation at High Pressure
Open this publication in new window or tab >>Catalytic Combustion of Gasified Biomass for Gas Turbine Applications: Experimental Investigation at High Pressure
Show others...
2005 (English)In: Proceedings of the 6th International Workshop on Catalytic Combution, 2005, Vol. 100, 9-14 p.Conference paper, Published paper (Refereed)
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-144097 (URN)
Conference
6th International Workshop on Catalytic Combution
Note

QC 20140409

Available from: 2014-04-09 Created: 2014-04-09 Last updated: 2014-04-09Bibliographically approved
6. Lean Catalytic Combustion for Ultra-low Emissions at High Temperature in Gas-Turbine Burners
Open this publication in new window or tab >>Lean Catalytic Combustion for Ultra-low Emissions at High Temperature in Gas-Turbine Burners
Show others...
2011 (English)In: Energy & Fuels, ISSN 0887-0624, E-ISSN 1520-5029, Vol. 25, 136-143 p.Article in journal (Refereed) Published
Abstract [en]

Catalytic systems for methane combustion, with Rh and Pt in a BaZrO3-based perovskite, were synthesized at the University of L'Aquila and tested at close to industrial conditions at the KTH Energy Centre in Stockholm. Because of the resistance to high temperature of BaZrO3 (up to similar to 2600 degrees C), such systems are suitable for resolving stability problems frequently encountered with high-temperature operations. Furthermore, these perovskites contain the noble metal in a high oxidation state, giving rise to very active compounds. They also result in ultra-low emissions, compatible with legislation in such places as southern California and Japan.

National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-30960 (URN)10.1021/ef100656y (DOI)000287345900016 ()2-s2.0-78751666225 (Scopus ID)
Note
QC 20110307Available from: 2011-03-07 Created: 2011-03-07 Last updated: 2017-12-11Bibliographically approved
7. Palladium-manganese catalysts supported on monolith systems for methane combustion
Open this publication in new window or tab >>Palladium-manganese catalysts supported on monolith systems for methane combustion
Show others...
2008 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 79, no 2, 122-131 p.Article in journal (Refereed) Published
Abstract [en]

Alumina-supported bimetallic and monometallic Mn and Pd monolithic catalysts were prepared and tested in methane combustion. Two different reactor configurations were adopted for catalyst testing, i.e. a fixed-bed laboratory-scale reactor and a pilot-plant reactor which allowed work at different temperatures and pressures. The results of catalyst performance showed that all bimetallic catalysts are considerably more stable for methane combustion than the monometallic palladium catalyst. With the aim to explain the relationship between activity-stability and structure and surface properties, the catalysts were characterized by TPO, XRD, XPS and ICP-AES. The high stability displayed by the bimetallic systems is attributed to the influence of manganese in retarding the decomposition of PdO into metallic palladium. Thus, it appears that manganese oxides inhibit PdO decomposition, as a consequence of the increase in oxygen mobility in the manganese oxide spinel phase.

Keyword
catalytic combustion, methane, palladium, manganese, monolith, alumina
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-34109 (URN)10.1016/j.apcatb.2007.10.014 (DOI)000253607400005 ()2-s2.0-38149043495 (Scopus ID)
Note
QC 20110525Available from: 2011-05-25 Created: 2011-05-25 Last updated: 2017-12-11Bibliographically approved
8. Gasified biomass fuelled gas turbine: Combustion stability and selective catalytic oxidation of fuel-bound nitrogen
Open this publication in new window or tab >>Gasified biomass fuelled gas turbine: Combustion stability and selective catalytic oxidation of fuel-bound nitrogen
Show others...
2006 (English)In: Proceedings of the ASME Turbo Expo 2006, Vol 1, 2006, 773-780 p.Conference paper, Published paper (Refereed)
Abstract [en]

Low heating value of gasified biomass and its fuel bound nitrogen containing compounds challenge the efforts on utilizing gasified biomass on gas turbine combustor. Low heating value of the gas brings along combustion stability issues and pollutant emission concerns. The fuel bound nitrogen present in gasified biomass could completely be converted to NOx during the combustion process. Catalytic combustion technology, showing promising developments on ultra low emission gas turbine combustion of natural gas could also be the key to successful utilization of biomass in gas turbine combustor. Catalysts could stabilize the combustion process of low heating value gas while the proper design of the catalytic configuration could selectively convert the fuel bound nitrogen into molecular nitrogen. This paper presents preliminary results of the experimental investigations on combustion stability and nitrogen selectivity in selective catalytic oxidation of ammonia in catalytic combustion followed by a brief description of the design of catalytic combustion test facility. The fuel-NOx reduction strategy considered in this study was to preprocess fuel in the catalytic system to remove fuel bound nitrogen before real combustion reactions occurs. The catalytic combustion system studied here contained two stage reactor in one unit containing fuel preprocessor (SCO catalyst) and combustion catalysts. Experiments were performed under lean combustion conditions (lambda value from 6 up to 22) using a simulated mixture of gasified biomass. The Selective Catalytic Oxidation approach was considered to reduce the conversion of NH3 into N-2. Results showed very good combustion stability, higher combustion efficiency and good ignition performances under the experimental conditions. However, the selective oxidation of fuel bound nitrogen into N-2 was only in the range of 20% to 30% under the above conditions.

National Category
Energy Engineering
Identifiers
urn:nbn:se:kth:diva-42238 (URN)10.1115/GT2006-90988 (DOI)000243377500078 ()2-s2.0-33750836430 (Scopus ID)0-7918-4236-3 (ISBN)
Conference
51st ASME Turbo Expo Location: Barcelona, Spain, Date: MAY 06-11, 2006
Note

QC 20111007

Available from: 2011-10-07 Created: 2011-10-06 Last updated: 2014-04-09Bibliographically approved
9. Supported palladium-platinum catalyst for methane combustion at high pressure
Open this publication in new window or tab >>Supported palladium-platinum catalyst for methane combustion at high pressure
Show others...
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

Keyword
high pressure, palladium, platinum, bimetallic catalysts, methane, combustion stability
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-6564 (URN)10.1016/j.cattod.2004.08.018 (DOI)000229275100047 ()2-s2.0-17344370162 (Scopus ID)
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: 2014-04-09Bibliographically approved

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