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Study of gas molecule - surface interaction
Kettner, Miroslav ; Nehasil, Václav (advisor) ; Johánek, Viktor (referee)
Title: Study of gas molecule - surface interaction Author: Miroslav Kettner Department: Department of surface and plasma science Supervisor: doc. RNDr. Václav Nehasil, Dr., Department of surface and plasma science Abstract: In this work, we examined the suitability of rhodium deposited on a plasma sprayed substrate of titanium dioxide for catalysis reactions. With X-ray photoelectron spectroscopy method, the thermal stability of TiO2 prepared with plasma spray technology on aluminum plate was tested at first. Then, rhodium was evaporated on substrate and thermal stability of the whole system Rh/TiO2 was determined. Further methods of thermal desorption spectroscopy and molecular beam were used to study adsorption and desorption of CO and reaction of CO with oxygen. It was verified that the system Rh/TiO2 ceases to adsorbing CO after heating above 620 K, also the CO reaction with oxygen exhibits considerably lower intensity after heating above 620 K. After calibrating on rhodium plate, it was determined that the intensity of CO2 creation on Rh/TiO2 is four times lower than intensity on the rhodium plate. Unprompted adsorption and desorption passivation of the system, however, seems to be the most significant problem. Therefore, the system was assessed as unsuitable for further research. Keywords: Rh, TiO2,...
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Study of CeOx / Rh inverse catalyst
Kettner, Miroslav ; Nehasil, Václav (advisor) ; Johánek, Viktor (referee)
Title: Study of CeOX / Rh inverse catalyst Author: Bc. Miroslav Kettner Department: Department of Surface and Plasma Science Supervisor: doc. RNDr. Václav Nehasil, Dr., Department of Surface and Plasma Science Abstract: Inverse catalysts of cerium oxide deposited on polycrystalline and monocrystalline (111) rhodium substrates were studied by means of surface science experimental methods. Growth characteristics of cerium oxide were investigated in dependence on deposition conditions and different thickness determination methods were compared. Acording to oxidizing or reducing exposition conditions changes in degree of oxidation of CeOX were observed. Further spectra analysis showed additional Ce-Rh alloy formation. Adsorption positions CO on-top and CO hollow on Rh (111) surface were differentiated by spectra fitting procedures. Oxygen absorption and reverse desorption in CeOX was confirmed. Performed experiments indicate that this process occurs through oxide-metal interface. CO oxidation reaction mechanisms at room temperature were proposed. Cerium oxide presence is necessary for reaction occurrence. Significant influence of deposited CeOX on proposed CO oxidation reaction mechanisms was proved by this way. Keywords: Rhodium, cerium oxide, alloy, inverse catalyst, CO oxidation.
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Reactivity of transition metals - influence of the degree of oxidation of active substrate
Kettner, Miroslav ; Nehasil, Václav (advisor) ; Jiříček, Petr (referee) ; Lykhach, Yaroslava (referee)
The impacts of fluorine doping of ceria are studied by means of surface science experimental methods. Fluorine-doped and fluorine-free ceria layers are epitaxially grown on rhodium single crystals and their properties are compared in regular and inverse catalyst configurations. A procedure for epitaxial growth of CeO2(110) and CeOxFy(110) layers on Rh(110) single crystal is developed and described in detail. Shape alterations of Ce 3d spectrum brought about by fluorine doping are explained and a suitable deconvolution method is proposed. Special attention is focused towards stability of fluorine in ceria. Presented data show that fluorine incorporation in ceria lattice causes stable reduction of ceria, which withstands up to 200řC in near-ambient pressure conditions. Morphological changes are observed due to elongation of surface lattice constant of reduced ceria. Oxygen storage capacities and hydrogen oxidation reaction rates of four different studied systems are compared and discussed. The twofold nature of oxygen exposure of fluorinated ceria is discovered and explained. Oxygen repels fluorine from the surface, while the remaining part of fluorine is expelled to adsorbate positions, where its electronic state is altered. Moreover, such fluorine is prone to interact with atomic hydrogen. This reaction is...
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Reactivity of transition metals - influence of the degree of oxidation of active substrate
Kettner, Miroslav ; Nehasil, Václav (advisor)
The impacts of fluorine doping of ceria are studied by means of surface science experimental methods. Fluorine-doped and fluorine-free ceria layers are epitaxially grown on rhodium single crystals and their properties are compared in regular and inverse catalyst configurations. A procedure for epitaxial growth of CeO2(110) and CeOxFy(110) layers on Rh(110) single crystal is developed and described in detail. Shape alterations of Ce 3d spectrum brought about by fluorine doping are explained and a suitable deconvolution method is proposed. Special attention is focused towards stability of fluorine in ceria. Presented data show that fluorine incorporation in ceria lattice causes stable reduction of ceria, which withstands up to 200řC in near-ambient pressure conditions. Morphological changes are observed due to elongation of surface lattice constant of reduced ceria. Oxygen storage capacities and hydrogen oxidation reaction rates of four different studied systems are compared and discussed. The twofold nature of oxygen exposure of fluorinated ceria is discovered and explained. Oxygen repels fluorine from the surface, while the remaining part of fluorine is expelled to adsorbate positions, where its electronic state is altered. Moreover, such fluorine is prone to interact with atomic hydrogen. This reaction is...
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Reactivity of transition metals - influence of the degree of oxidation of active substrate
Kettner, Miroslav ; Nehasil, Václav (advisor)
The impacts of fluorine doping of ceria are studied by means of surface science experimental methods. Fluorine-doped and fluorine-free ceria layers are epitaxially grown on rhodium single crystals and their properties are compared in regular and inverse catalyst configurations. A procedure for epitaxial growth of CeO2(110) and CeOxFy(110) layers on Rh(110) single crystal is developed and described in detail. Shape alterations of Ce 3d spectrum brought about by fluorine doping are explained and a suitable deconvolution method is proposed. Special attention is focused towards stability of fluorine in ceria. Presented data show that fluorine incorporation in ceria lattice causes stable reduction of ceria, which withstands up to 200řC in near-ambient pressure conditions. Morphological changes are observed due to elongation of surface lattice constant of reduced ceria. Oxygen storage capacities and hydrogen oxidation reaction rates of four different studied systems are compared and discussed. The twofold nature of oxygen exposure of fluorinated ceria is discovered and explained. Oxygen repels fluorine from the surface, while the remaining part of fluorine is expelled to adsorbate positions, where its electronic state is altered. Moreover, such fluorine is prone to interact with atomic hydrogen. This reaction is...
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Reactivity of transition metals - influence of the degree of oxidation of active substrate
Kettner, Miroslav ; Nehasil, Václav (advisor) ; Jiříček, Petr (referee) ; Lykhach, Yaroslava (referee)
The impacts of fluorine doping of ceria are studied by means of surface science experimental methods. Fluorine-doped and fluorine-free ceria layers are epitaxially grown on rhodium single crystals and their properties are compared in regular and inverse catalyst configurations. A procedure for epitaxial growth of CeO2(110) and CeOxFy(110) layers on Rh(110) single crystal is developed and described in detail. Shape alterations of Ce 3d spectrum brought about by fluorine doping are explained and a suitable deconvolution method is proposed. Special attention is focused towards stability of fluorine in ceria. Presented data show that fluorine incorporation in ceria lattice causes stable reduction of ceria, which withstands up to 200řC in near-ambient pressure conditions. Morphological changes are observed due to elongation of surface lattice constant of reduced ceria. Oxygen storage capacities and hydrogen oxidation reaction rates of four different studied systems are compared and discussed. The twofold nature of oxygen exposure of fluorinated ceria is discovered and explained. Oxygen repels fluorine from the surface, while the remaining part of fluorine is expelled to adsorbate positions, where its electronic state is altered. Moreover, such fluorine is prone to interact with atomic hydrogen. This reaction is...
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Study of CeOx / Rh inverse catalyst
Kettner, Miroslav ; Nehasil, Václav (advisor) ; Johánek, Viktor (referee)
Title: Study of CeOX / Rh inverse catalyst Author: Bc. Miroslav Kettner Department: Department of Surface and Plasma Science Supervisor: doc. RNDr. Václav Nehasil, Dr., Department of Surface and Plasma Science Abstract: Inverse catalysts of cerium oxide deposited on polycrystalline and monocrystalline (111) rhodium substrates were studied by means of surface science experimental methods. Growth characteristics of cerium oxide were investigated in dependence on deposition conditions and different thickness determination methods were compared. Acording to oxidizing or reducing exposition conditions changes in degree of oxidation of CeOX were observed. Further spectra analysis showed additional Ce-Rh alloy formation. Adsorption positions CO on-top and CO hollow on Rh (111) surface were differentiated by spectra fitting procedures. Oxygen absorption and reverse desorption in CeOX was confirmed. Performed experiments indicate that this process occurs through oxide-metal interface. CO oxidation reaction mechanisms at room temperature were proposed. Cerium oxide presence is necessary for reaction occurrence. Significant influence of deposited CeOX on proposed CO oxidation reaction mechanisms was proved by this way. Keywords: Rhodium, cerium oxide, alloy, inverse catalyst, CO oxidation.
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Study of gas molecule - surface interaction
Kettner, Miroslav ; Nehasil, Václav (advisor) ; Johánek, Viktor (referee)
Title: Study of gas molecule - surface interaction Author: Miroslav Kettner Department: Department of surface and plasma science Supervisor: doc. RNDr. Václav Nehasil, Dr., Department of surface and plasma science Abstract: In this work, we examined the suitability of rhodium deposited on a plasma sprayed substrate of titanium dioxide for catalysis reactions. With X-ray photoelectron spectroscopy method, the thermal stability of TiO2 prepared with plasma spray technology on aluminum plate was tested at first. Then, rhodium was evaporated on substrate and thermal stability of the whole system Rh/TiO2 was determined. Further methods of thermal desorption spectroscopy and molecular beam were used to study adsorption and desorption of CO and reaction of CO with oxygen. It was verified that the system Rh/TiO2 ceases to adsorbing CO after heating above 620 K, also the CO reaction with oxygen exhibits considerably lower intensity after heating above 620 K. After calibrating on rhodium plate, it was determined that the intensity of CO2 creation on Rh/TiO2 is four times lower than intensity on the rhodium plate. Unprompted adsorption and desorption passivation of the system, however, seems to be the most significant problem. Therefore, the system was assessed as unsuitable for further research. Keywords: Rh, TiO2,...
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