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- Darmastuti, Zhafira
(author)
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SiCFET gassensors : theory, developent, and applications to flue gas cleaning processes in power plants
- 2012
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Licentiate thesis (other academic/artistic)abstract
- Environmental and health concerns lead to stricter regulations on power plant emission. Sensors play an important role, not only as part of the process control to ensure that the effluent stays under the regulated values, but also to increase the pollution removal efficiency and to decrease the reagent consumption.Previous studies, on the use of SiC based Field Effect Transistors (FET) as NH3 sensors in Tekniska Verken power plants and as CO sensors for the control of the domestic boilers, have shown promising results. Moreover, these sensors can withstand high temperature operation and are considerably cheaper than most conventional sensors used in power plants. The price of the sensors enable the installation of multiple sensors in one flue gas duct section, which lead to better monitoring of the flue gas uniformity. Based on that argument, this study is performed to determine whether it is possible to expand the possible application of SiC-FET sensors for the detection of other pollutants emitted by power plants. This thesis reports the characterization and performance testing of SiC-FET sensors towards other selected air pollutants: H2S, methanol as a product of CO2 hydrogenation, and SO2.The study is performed by I-V characterization of the sensors toward the test gas in different background gases and studies of the detection mechanism. Detection mechanism studies include DRIFT spectroscopy, mass spectroscopy, and theoretical study of the surface reaction with Density Functional Theory (DFT).Ir-gate SiC-FET sensors at 350oC show a very high sensitivity to H2S. The large response reduces the possibility of cross-sensitivity from other gases. Pt-gate sensors offer very fast response with decent response magnitude at 200oC for methanol. The presence of oxygen improves the response to methanol, which is favorable for the leak detection application. Besides oxygen, the influence of hydrogen, propene, and water vapor is also observed in the experiment with methanol. The detection mechanism and different sensing behavior of Pt and Ir gates are illustrated with model reaction mechanisms on the surface of the metals. Sensor characterization has been performed for SO2 with several catalytic metal gates: Pt, Ir, Cu, and Au. The results suggest that a single sensor with any of Pt, Ir, Cu, and Au gates is able to detect the presence of SO2 in the air or nitrogen background. However, they are unable to measure different SO2 concentration. Moreover, the response level to SO2 is so small, that it will probably disappear if there is any other gas present in the mixture.
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| 2. |
- Darmastuti, Zhafira
(author)
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SiC-FET Gas Sensors Developed for Control of the Flue Gas Desulfurization System in Power Plants Experimental and Modeling : Experimental and Modeling
- 2014
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Doctoral thesis (other academic/artistic)abstract
- Electricity and power generation is an essential part of our life. However, powergeneration activities also create by-products (such as sulphur oxides, nitrogen oxides,carbon monoxide, etc), which can be dangerous when released to the atmosphere.Sensors, as part of the control system, play very vital role for the fluegas cleaning processes in power plants. This thesis concerns the development ofSilicon Carbide Field Effect Transistor (SiC-FET) gas sensors as sensors for sulfurcontaining gases (SO2 and H2S) used as part of the environmental control systemin power plants. The works includes sensor deposition and assembly, sensinglayer characterization, operation mode development, performance testing of thesensors in a gas mixing rig in the laboratory and field test in a desulfurization pilotunit, and both experimental and theoretical studies on the detection mechanismof the sensors.The sensor response to SO2 was very small and saturated quickly. SO2 is a verystable gas and therefore reaction with other species requires a large energy input.SO2 mostly reacts with the catalyst through physisorption, which results in lowresponse level. Another problem was that once it finally reacted with oxygen andadsorbed on the surface of the catalyst in form of a sulfate compound, it is desorbedwith difficulty. Therefore, the sensor signal saturated after a certain timeof exposure to SO2. Different gate materials were tested in static operation (Pt,Ir, Au), but the saturation phenomena occurred in all three cases. Dynamic sensoroperation using temperature cycling and multivariate data analysis could mitigatethis problem. Pt-gate sensors were operated at several different temperatures in acyclic fashion. One of the applied temperatures was chosen to be very high for ashort time to serve as cleaning step. This method was also termed the virtual multisensor method because the data generated could represent the data from multiplesensors in static operation at different temperatures. Then, several features of thesignal, such as mean value and slope, were extracted and processed with multivariatedata analysis. Linear Discrimination Analysis (LDA) was chosen since itiiiallows controlled data analysis. It was shown that it was possible to quantify SO2with a 2-step LDA. The background was identified in the first step and SO2 wasquantified in the second step. Pt sensors in dynamic operation and 2-step LDAevaluation has also demonstrated promising results for SO2 measurement in thelaboratory as well as in a desulfurization pilot unit. For a commercial sensor, algorithmhave to be developed to enable on-line measurement in real time.It was observed that Ir-gate sensors at 350oC were very sensitive to H2S. The responseobtained by Ir sensors to H2S was almost five times larger than that of Ptsensors, which might be due to the higher oxygen coverage of Ir. Moreover, Irsensors were also more stable with less drift during the operation as a result ofhigher thermal stability. However, the recovery time for Ir sensors was very long,due to the high desorption energy. Overall, the Ir sensors performed well whentested for a leak detection application (presence of oxygen and dry environment).The geothermal application, where heat is extracted from the earth, requires thesensor to be operated in humid condition in the absence (or very low concentration)of oxygen, and this poses a problem. Temperature cycle operation and smartdata evaluation might also be an option for future development.Along with the sensor performance testing, a study on the detection mechanismwas also performed for SO2 sensor, both experimentally and theoretically. The experimentincluded the study of the species formed on the surface of the catalystwith DRIFT (diffuse reflectance infrared frourier transform) spectroscopy and theanalysis of the residual gas with mass spectroscopy. Explanatory investigation ofthe surface reactions was performed using quantum-chemical calculations. Theoreticalcalculations of the infrared (IR) vibration spectra was employed to supportthe identification of peaks in the DRIFT measurement. Based on the study on theresidual gas analysis and quantum-chemical calculations, a reaction mechanismfor the SO2 molecule adsorption on the sensor surface was suggested.
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