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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

Reaction kinetics of the iron-catalysed decomposition of SO3 / Abraham Frederik van der Merwe

Van der Merwe, Abraham Frederik January 2014 (has links)
In this study the performance of pure, very fine iron (III) oxide powder was investigated as catalyst for the decomposition of sulphur trioxide into sulphur dioxide and oxygen. This highly endothermic reaction requires a catalyst to lower the reaction temperature. This reaction forms part of the HyS (Hybrid Sulphur) cycle, a proposed thermochemical process for the industrial scale production of hydrogen and oxygen from water. The study aimed at obtaining reaction kinetics for this reaction employing pure, unsupported iron (III) oxide as catalyst as a cheaper alternative compared to supported iron catalysts. It was found that the SO3 conversion was carried out in the absence of diffusion limitations and that the reverse reaction did not play a significant role. By assuming plug flow conditions in the reactor and 1st order kinetics, the kinetic parameters of the reaction were obtained. These parameters that form part of the Arrhenius law in describing the reaction rate constant, were determined to be 118(±23) kj / mol for the activation energy ( Ea ), and a value of 3(±0.5) x 108hr-1 was obtained for the Arrhenius frequency factor ( A ). Both values correspond to literature, although in general larger activation energies were published for iron (III) oxide derived supported catalysts. A comparison of the performance of the pure, unsupported iron (III) oxide catalyst with other iron (III) oxide derived supported catalysts (or pellets) has shown that the pure iron (III) oxide catalyst exhibit similar activities. Avoiding expensive catalyst preparation will be an initial step in the direction of developing a cost effective catalyst for the decomposition of sulphur trioxide. It is, however, recommended to investigate different particle sizes as well as purity levels of the unsupported iron (III) oxide to find an optimum cost to performance ratio, as the degree of fineness and the degree of purity will largely influence the final catalyst cost. A qualitative investigation with various reaction product species as well as water in the reactor feed was conducted to assess the influence of these species on the reaction rate. The addition of these species seems to have a larger influence on the reaction rate at low reaction temperatures around 700°C than at higher reaction temperatures (i.e. 750°C and 825°C). This can be attributed to adsorption rates of such species that reduce at higher temperatures. Observations at higher reaction temperatures also suggest that the reaction is of a first-order nature. / MIng (Chemical Engineering), North-West University, Potchefstroom Campus, 2014
2

Reaction kinetics of the iron-catalysed decomposition of SO3 / Abraham Frederik van der Merwe

Van der Merwe, Abraham Frederik January 2014 (has links)
In this study the performance of pure, very fine iron (III) oxide powder was investigated as catalyst for the decomposition of sulphur trioxide into sulphur dioxide and oxygen. This highly endothermic reaction requires a catalyst to lower the reaction temperature. This reaction forms part of the HyS (Hybrid Sulphur) cycle, a proposed thermochemical process for the industrial scale production of hydrogen and oxygen from water. The study aimed at obtaining reaction kinetics for this reaction employing pure, unsupported iron (III) oxide as catalyst as a cheaper alternative compared to supported iron catalysts. It was found that the SO3 conversion was carried out in the absence of diffusion limitations and that the reverse reaction did not play a significant role. By assuming plug flow conditions in the reactor and 1st order kinetics, the kinetic parameters of the reaction were obtained. These parameters that form part of the Arrhenius law in describing the reaction rate constant, were determined to be 118(±23) kj / mol for the activation energy ( Ea ), and a value of 3(±0.5) x 108hr-1 was obtained for the Arrhenius frequency factor ( A ). Both values correspond to literature, although in general larger activation energies were published for iron (III) oxide derived supported catalysts. A comparison of the performance of the pure, unsupported iron (III) oxide catalyst with other iron (III) oxide derived supported catalysts (or pellets) has shown that the pure iron (III) oxide catalyst exhibit similar activities. Avoiding expensive catalyst preparation will be an initial step in the direction of developing a cost effective catalyst for the decomposition of sulphur trioxide. It is, however, recommended to investigate different particle sizes as well as purity levels of the unsupported iron (III) oxide to find an optimum cost to performance ratio, as the degree of fineness and the degree of purity will largely influence the final catalyst cost. A qualitative investigation with various reaction product species as well as water in the reactor feed was conducted to assess the influence of these species on the reaction rate. The addition of these species seems to have a larger influence on the reaction rate at low reaction temperatures around 700°C than at higher reaction temperatures (i.e. 750°C and 825°C). This can be attributed to adsorption rates of such species that reduce at higher temperatures. Observations at higher reaction temperatures also suggest that the reaction is of a first-order nature. / MIng (Chemical Engineering), North-West University, Potchefstroom Campus, 2014

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