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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

The Study of Catalytic Oxidation of Isopropyl Alcohol in an Air Stream over Honeycomb Catalyst

Huang, Shi-wei 29 June 2004 (has links)
ABSTRACT Isopropyl Alcohol (denoted as IPA) is a valuable chemical product, which is used in the chemical industry such as synthetic resin, essential oils and surface paint. Moreover, factory of the production of photography and electronics are also the user of IPA.IPA is the typical pollutant emitted from those industrial processing . It is known to be causing severe irritation and burns and is suspected to have long-term effects such as bronchitis. This study was to investigate the effect on conversion, deactivation of long-term test, selectivity of product and kinetics in oxidation of IPA over Cu and Cu/Ce catalysts supported on ceramic honeycomb. The explanation of results can be divided into several major parts as follows: 1. In the of selection catalyst, we find that 20%Cu/Ce catalysts prepared by wet- impregnation has the best conversion and selectivity. 2. The conversion of IPA in catalytic reaction is increased with the increasing both of reaction temperature and influent concentration of oxygen but decreased with the going up of initial concentration of IPA, space velocity and relative humidity. 3. In the catalyst stability of long-term test, Cu/Ce catalysts had a good stability after 7 days reaction in heterogeneous reactor. The tests such as XRD, SEM and EA were also determined to verify the stability from surface of catalyst. 4. Two kinetic models, Power rate law and Mars-Van Krevelen model were used to fit the kinetic data of the decomposition of IPA. Power rate law is suitable to describe the catalytic decomposition of IPA under the operation range in this work.
2

Microstructure and electrochemical performance of fully ceramic composite anodes for SOFCs

Schlegl, Harald January 2015 (has links)
Solid Oxide Fuel Cells could play a key role in energy systems of the future because they can directly convert the chemical energy of fuels into electrical energy in a reliable and energy efficient way. The choice of materials for the components of fuel cells is crucial for the achievement of the high performance and the low price necessary to establish fuel cell technology in the energy market. Current state of the art anodes consisting of nickel and yttria stabilised zirconia (Ni/YSZ) offer good electrochemical performance but suffer from limitations like carbon deposition, redox instability and sulphur poisoning. This thesis explores the properties of composite fully ceramic anodes consisting of a skeleton of yttria stabilised zirconia (YSZ) or cerium gadolinium oxide (CGO) and a perovskite phase based on B-site doped lanthanum strontium titanate. The perovskite phase was fabricated in situ inside the pores of the skeleton material by the infiltration of an aqueous precursor and subsequent firing (impregnation method). Material characterisation of the composite anodes was carried out by X-ray diffraction and the microstructure investigated by electron microscope techniques. The electrochemical performance was tested by IV-curves and impedance spectroscopy. Particularly the investigation of the connection between the microstructure of the impregnated anodes and their electrochemical performance is a main objective of this work. The electrochemical performance of cells with a CGO skeleton and an impregnated lanthanum strontium titanate phase was found to be inferior compared to cells with a YSZ skeleton, even if the ionic conductivity of CGO is known to be higher than the ionic conductivity of YSZ. The difference was assigned to mass transport problems tightly connected to the different microstructure of the composite anodes. A significant improvement of the performance could be achieved by the utilisation of A-site deficient perovskites as impregnated phase in a YSZ skeleton. Cells with composite anodes of YSZ and La₀.₄Sr₀.₄Ti₀.₉₄Mn₀.₀₆O[sub](3-δ) show power densities of 156.2 mW/cm² at a measuring temperature of 750 °C compared to 58.5 mW/cm² measured in a similar cell with A-site stoichiometric LSTM, both cells having an electrolyte thickness of around 60 μm. The superiority of the performance of anodes with A-site deficient perovskites is mainly due to a lower ohmic resistance of only 0.5 Ω*cm², indicating better conductivity of the composite with A-site deficient perovskites. The investigation of the microstructure of composite anodes with A-site deficient perovskites showed the decoration of the surface with nanoparticles after reduction. These nanoparticles originate from exsolution of ions from the B-site of the perovskite and can't be found in A-site stoichiometric perovskites. The influence of fabrication parameters like firing temperature of the skeleton, firing temperature after impregnation or vacuum impregnation on the microstructure and electrochemical performance of the composite anodes was studied. Particularly the increase of the firing temperature of the skeleton from 1400 °C to 1500 °C resulted in an impressive improvement of total cell resistance and maximal power density.
3

The Study of Catalytic Oxidation of Nitrogen Monoxide

Wang, Ching-Chie 31 July 2000 (has links)
The study of catalytic oxidation on the removal of NO was investigated over the Cu-catalysts . The Cu-catalysts , including Cu/TiO2 , Cu/Al2O3 and Cu/SiO2 , were prepared by impregnation method . Alougth NO2 , the product of this reaction , has higher toxicity than NO , but it might be removed completely by absorption with H2O or alkalinal solution for its high solubility . The experiments can be divided into three parts , i.e. , the screen of test catalysts , the effect of operating factors on the conversion of NO and the kinetic model . In the first part , the activity of test catalysts , which were prepared by mixing three various sources of Cu-ions¡]i.e., Cu(NO3)2 , Cu(CH3COO)2 , and CuSO4¡^with three different types of support¡]i.e., TiO2 , Al2O3 , and SiO2¡^, and were compared in form of conversion on NO to find the best catalyst . The results show that the mixture Cu(NO3)2 / TiO2 has the good performance on the conversion of NO , and also has more wider operating in range of temperature . In order to find the optimal loading of Cu on Cu(NO3)2 / TiO2 , additional test of various dosage over the catalysts was conduct in series . It is found that 8wt.% of Cu loading on Cu(NO3)2 / TiO2 is the most economic dosage . Therefore , we select this type of Cu oxide as the best catalyst in the following work . In the second part , the effect of NO inlet concentration , space velocity and humidity on the conversion of NO were performed . The results show that the conversion of NO decreases with the increasing of [NO]in when [NO]in is larger than 1000ppm¡Fthe conversion of NO is not changed with [NO]in when [NO]in is lower than 1000ppm . The better space velocity is 15000hr-1 , i.e.,the empty bed residence time is 0.24 second . The reaction on NO conversion would be restrained by higher humidity contenting in inlet gas stream , but the effect of inhibition on NO conversion is not significant . Finally , the kinetics of the oxidation of NO over 8wt.% Cu(NO3)2 / TiO2 was obtained by integral method .It is found that the oxidations of NO can be described by first order reversible reaction and the observed activation energy are 15.8 kcal/mole¡]forward reaction¡^and 25.9 kcal/mole¡]backward reaction¡^, respectively . By comparing the conversion of predicted NO with the experimentals , we can find the suitable operation conditions in application of the kinetic model : the inlet concentration of NO in a range of 300-1000ppm , the empty-bed residence time ranging from 0.12-0.48 second , and the absolute humidity ranging from 4854 to 42475ppm .
4

Performance and Reaction Mechanisms of Solid Oxide Fuel Cell Cathodes Fabricated by the Impregnation Method

Zhang, Qi 08 1900 (has links)
<p> The exploration of cathode materials and fabrication methods plays an important role in the development of solid oxide fuel cell (SOFC) technology. The objective of this study is first to optimize the cathode microstructure by the impregnation method, and then investigate the potential application of copper manganese spinel as a new cathode material with optimized microstructure and explore the reaction mechanism of the cathodes.</p> <p> The impregnation method was employed to fabricate a composite cathode with electrocatalyst particles dispersed in a framework of electrolyte material. The impregnation method is relatively easy to apply and yield the optimized microstructure, allowing extended three phase boundary length and absence of secondary phase formation during fabrication.</p> <p> The polarization performance of copper manganese spinel (CMO) impregnated YSZ cathodes was examined by adjusting catalyst particle size, electrode thickness and catalyst content. A critical thickness of 16.9±2.0 μm for the CMO-YSZ composite cathode was calculated from Tanner's model. Decreased catalyst particle size and a thickness close to the critical value were found to eliminate polarization loss. The composite cathode with 50 wt% CMO impregnation showed a polarization resistance as low as 0.3 Ωcm^2 at 750°C. At 800°C, an SOFC with CMO-YSZ composite cathode had a power density of 172 mW/cm^2, which was 2.5 times higher than the cell with the traditional LSM-YSZ composite cathode under the same conditions.</p> <p> The cathode reaction mechanism of CMO-YSZ and strontium doped lanthanum ferrite (LSCF) impregnated Gd doped ceria ( CGO) composite cathodes was studied, using impedance spectroscopy, cyclic voltammetry and current interruption techniques. Surface diffusion and mass transfer were determined to be the rate controlling steps for CMO-YSZ composite cathode at low and high temperatures, respectively. A low frequency process at low temperatures and at least two processes at high temperatures were identified as rate determining steps of LSCF -CGO composite cathodes. A cathodic current activation effect was observed on CMO-YSZ cathode under current passage. The catalytic activity of CMO was enhanced by the cathodic current and the effect existed in both long-term and short-term experiments.</p> <p> The results of this study suggest that copper manganese spinel has attractive properties as a new catalyst material for the cathodic reaction with the composite structure obtained by the impregnation method.</p> / Thesis / Master of Applied Science (MASc)

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