As the world energy demand increases and the utilization of non-traditional fossil fuels becomes more attractive, natural gas, from shale gas and in gaseous and liquefied forms, becomes one of the most promising alternative fuels nowadays. The natural gas offers lower fuel production and transportation costs, a lower carbon content, a higher combustion efficiency and a greater applicability to most of existing power plants and combustion engines. Challenges exist, especially in improving its ignition characteristics and to further reduce its greenhouse gas and particulate matter emissions. To overcome these restraints, hydrogen addition, catalyst modification and fuel lean combustion have been investigated recently. In this thesis, the ignition and emission properties of methane and its mixtures with hydrogen additive are first studied in the mini-channel reactor. Numerical investigations have been performed using the CHEMKIN PRO software for pure methane and the mixtures of methane and hydrogen in non-catalytic and catalytic combustion. These effects of the hydrogen fractions, Pt-catalyst, wall temperature and inlet conditions on the ignition delay and NO formation are investigated. Available gas phase kinetics and heterogeneous surface reaction mechanisms in the literature are implemented and analyzed. As the second part of this thesis, natural gas combustion on a counter-flow burner is investigated experimentally and numerically, with a focus on NO formation. The NO profiles, measured by the FT-IR spectroscopy, are compared with model results from CHEMIKIN and with the GRI-Mech 3.0 mechanism. The formation mechanism of NO and effects of the different fuel/oxidizer ratios on the NO formation are investigated.

Catalytic combustion provides us an efficient approach for the utilization and mitigation of methane, the major component of natural gas as well as an important greenhouse gas in global warming. From the research of catalytic combustion of methane, better understandings as well as solutions to the current methane-related problems can be obtained. This study investigates lean methane combustion on palladium-based catalysts. Catalysts activities were tested through ignition and extinction experiments. Several pretreatments and their influence were studied. Instrumental neutron activation analysis (INAA) and x-ray diffraction (XRD) were used as characterization tools for the catalysts. It was found that after being reduced, catalysts had stable and excellent abilities for methane conversion. However, these abilities were strongly compromised by additional water in the feeds. XRD results, combined with other testing results, implied that reduction produced the most active samples, while INAA revealed the real Pd concentrations of these catalysts. / Chemical Engineering

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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. / <p>QC 20131125</p>

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The catalytic combustion of methane in excess of O2 over Pd catalysts was studied on model catalysts, including polycrystalline palladium foil and palladium single crystals. The kinetics of this reaction could be measured at conditions not accessible to supported catalysts and, thus, the issues of structure sensitivity, mechanism, hysteresis on oxidation, and deactivation could be studied in detail. Methane oxidation on PdO was insensitive to the original metal surface structure which PdO grew from, with turnover rates in the range of 1.3-4.7 s-1 on (111), (100) and (110) single crystals at 160 Torr O2, 16 Torr CH-4, 1 Torr H2O and 598 K. Methane oxidation on Pd metal was also insensitive to the original surface structure, with the turnover rate in the range of 2.0-2.8 s-1 on the three single crystals at 2.3 Torr O2, 0.46 Torr CH4, 0.05 Torr H2O and 973 K. Since there is no support effect and the surface purity could be certified, these turnover rates for this reaction can be used as a benchmark. The turnover rate for methane oxidation was found to decrease 95% when PdO decomposed to Pd metal at 888 K, showing that PdO was more active than Pd metal for methane combustion at this temperature. Water inhibition to the reaction was not observed at a temperature above 813 K on both PdO and Pd metal, while it was observed at 598 K on PdO. The activation energy on PdO was 32 kJ mol-1 in the range of 783-873 K, while it was 125 kJ mol-1 in the range of 568-623 K. The activation energy on Pd metal was 125 kJ mol-1 in the range of 930-980 K. The change of reaction orders and activation energies suggests that the reaction mechanism is a function of temperature and palladium chemical states. We propose that adsorbed water, the most abundant surface intermediate at 598 K, was not present in significant quantities at temperatures above 783 K. This change in surface inhibition by water is the reason for lower activation energy at temperatures above 783 K. Interaction between the catalyst and support, or presence of impurities, is one of the factors for catalyst deactivation. The interaction between oxidized silicon and palladium was investigated on a polycrystalline palladium foil and on supported Pd/SiO2 catalysts. During methane oxidation, oxidized silicon covered the palladium oxide surface as observed by TEM on Pd/SiO2 catalysts and by XPS on palladium foil. On Pd foil, the source of silica was a silicon impurity, common on bulk metal samples. The migration of oxidized silicon onto PdO deactivated the catalysts by blocking the active sites for methane oxidation. Silicon oxide overlayers were also observed covering the Pd surface after reduction of Pd/SiO2 by H2 at 923 K.

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