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Model study of biomolecules bonding to cerium oxide nanoparticles
Pittnerová, Daniela ; Matolínová, Iva (advisor) ; Vorokhta, Mykhailo (referee)
In the last few years cerium oxide due to its convenient properties for biomedical applications has been studied as a promising material for fabrication of third-generation of mediator-less enzymatic biosensors. The bonding of biomolecules with cerium oxide is a crucial parameter, which is difficult to study due to the complexity of the problem. Therefore the model studies on epitaxial and polycrystalline cerium oxide were carried out. In this thesis we continued in this line of the research with the complex study of bonding of amino acids histidine, glycine and sarcosine to cerium oxide nanoparticles. The nanoparticles' properties as the size and chemical composition were measured by electron microscopies and related techniques (TEM, SEM, EDX), and a series of photoemission spectroscopies (XPS, SRPES, RPES and NEXAFS). The dependence of zeta potential on the pH was measure by DLS technique.
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Role of surface defects in ceria-based catalysis
Tovt, Andrii ; Mysliveček, Josef (advisor) ; Čechal, Jan (referee) ; Švec, Martin (referee)
Title: Role of surface defects in ceria-based catalysis Author: Andrii Tovt Department: Department of Surface and Plasma Science Supervisor of the doctoral thesis: doc. Mgr. Josef Mysliveček Ph.D., Department of Surface and Plasma Science Abstract: This work concentrates on the analysis of fundamental physicochemical properties of Pt-CeOx, single-atom Pt1 /CeOx, and inverse CeOx/Cu(111) catalysts. Preparation method for stabilized atomically-dispersed Pt2+ ions on ceria was developed and adsorption sites for Pt ions were thoroughly studied using advanced surface science techniques supported by theoretical methods. The mechanism of Pt2+ stabilization on ceria steps was revealed and the step capacity towards Pt2+ ions was estimated. Also, the preparation method for well-ordered cerium oxide ultrathin films with different stoichiometry and ordering of surface oxygen vacancies was developed, and the Ceria/Cu(111) interaction was investigated. Key words: heterogeneous catalysis, model systems, single-atom catalysis, platinum ions, cerium oxide.
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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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Electron microscopy study of nanostructured thin film catalysts for micro-fuel cell application
Lavková, Jaroslava ; Matolínová, Iva (advisor) ; Ruterana, Pierre (referee) ; Šubrt, Jan (referee)
Present doctoral thesis is focused on electron microscopy and spectroscopy investigation of novel metal-oxide anode catalyst for fuel cell application. Catalyst based on Pt- doped cerium oxide in form of thin layers prepared by simultaneous magnetron sputtering deposition on intermediate carbonaceous films grown on silicon substrate has been studied. The influence of catalyst support composition (a-C and CNx films), deposition time of CeOx layer and other deposition parameters, as deposition rate, composition of working atmosphere and Pt concentration on the morphology of Pt-CeOx layers has been investigated mainly by Transmission Electron Microscopy (TEM). The obtained results have shown that by suitable preparation conditions combination we are able to tune final morphology and composition of catalyst. Composition of carbonaceous films and Pt-CeOx layers was examined by complementary spectroscopy techniques - Energy Dispersive X-ray Spectroscopy (EDX), Electron Energy Loss Spectroscopy (EELS) and X-ray Photoelectron Spectroscopy (XPS). Such prepared porous structures of Pt-CeOx are of promising as anode catalytic material for real fuel cell application. Keywords: cerium oxide, platinum, fuel cell, magnetron sputtering, Transmission Electron Microscopy
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Physically chemical properties of epitaxial films CeO2/Cu(110)
Aulická, Marie ; Veltruská, Kateřina (advisor) ; Nehasil, Václav (referee)
In this work ways of preparation of thin epitaxial cerium oxide film on Cu(110) surface were studied. X-ray photoelectron spectroscopy (XPS), X-ray photoelectron difraction (XPD), low energy electron difraction (LEED), ion scattering spectroscopy (ISS) and scanning tunneling microscopy (STM) were used for the characterization of prepared systems. The island structure of CeO2 was prepared by the method of reactive evaporation in oxygen atmosphere. The influence of temperature on the electronic structure and morphology was studied. At the temperature above 550 ˚C partial reduction to Ce2O3 and reordering of the islands to the CeO2(331) structure was observed. The ceria promoted oxidation of copper surface was approved, since the clean c(6x2) reconstruction of the surface was observed at the oxygen exposure 1,5 order of magnitude lower then on Cu(110) alone. The other model system was prepared by cerium evaporation to the oxygen precovered Cu(110) surface. The mix of (2x1) and c(6x2) surface reconstruction was formed by oxygen exposition at 300 ˚C. Cerium was deposited on this surface, also at 300 ˚C. During the following heating to 500 ˚C the formation of epitaxial film Ce2O3(0001) was observed, accompanied by the formation of large hundreds nm long smooth band structures in the [11̄0] direction.
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Study of dependence of the metal-oxide electron structure on the reactivity of these systems
Ševčíková, Klára
Title: Study of dependence of the metal-oxide electron structure on the reactivity of these systems Author: Klára Ševčíková Supervisor: doc. RNDr. Václav Nehasil, Dr., Department of Surface and Plasma Science Abstract The presented thesis focuses on studying the interaction between rhodium and cerium oxide and its impact on the reactivity. We investigated two different systems, Rh/CeOx and Rh- CeOx, by means of the photoelectron spectroscopy and the temperature programmed reactions. Rh/CeOx stands for rhodium nanoparticles supported by cerium oxide thin film. We show that there is an electronic metal-substrate interaction between rhodium and cerium oxide. The type of the interaction depends on a degree of cerium oxide reduction and it has a tremendous impact on the reactivity of the system. On the other hand, Rh-CeOx represents cerium oxide thin films doped by rhodium. We characterized the properties of the films with various concentration of rhodium. We show that the morphology, chemical composition and reactivity of the samples strongly depend on the concentration of the rhodium dopant.
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Study of the structural properties of model ceria based catalysts
Beran, Jan
This work is concerning the study of model ceria based calalysts structure by methods of electron diffraction RHEED and photoelectron spectroscopy XPS. The influence of deposition conditions and substrate on the growth of epitaxial cerium oxide films on copper single crystals is described in detail. The work then describes the interaction of cerium and tin in model systems and the creation of SnCeOx mixed oxide and its structure. In the last chapter, the interaction of palladium with cerium and tin oxide layers is examined, and the creation of paladium bimetallic alloys is described. Powered by TCPDF (www.tcpdf.org)
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The preparation and study of catalytic system Cu(O)-CeO2 using surface analytical methods
Šmíd, Břetislav
Title: The preparation and study of catalytic system Cu(O)-CeO2 using surface analytical methods Author: Břetislav Šmíd Department: Department of Surface and Plasma Science Supervisor of the doctoral thesis: Doc. Mgr. Iva Matolínová, Dr. Abstract: This work is concerned with a study of copper/copper oxide - cerium dioxide systems and their interaction with CO and H2O molecules. Investigated samples were prepared in the form of powder catalysts and also as very well defined model inverse systems. The low temperature CO oxidation powder catalysts were studied by means of XPS, XRD, SEM, TEM and in micro-reactor system allowing the CO oxidation examination. The study of H2O adsorption and co-adsorption of H2O with CO were carried out on model inverse systems CeOx(111)/Cu(111) in ultra-high vacuum conditions using X-ray, synchrotron radiation (SRPES), resonant (RPES) photoelectron spectroscopies and LEED. It was observed on the stoichiometric surface water adsorbs molecularly at 120 K while on the reduced surface and surface of CeO2 islands on Cu(111) the H2O adsorption is partially dissociative with formation of OH groups. The increase of Ce3+ species (i.e. surface reduction) observed after H2O adsorption was explained as an electronic effect of the Ce 4f charge accumulation and Ce 5d charge depletion....
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Role of surface defects in ceria-based catalysis
Tovt, Andrii ; Mysliveček, Josef (advisor)
Title: Role of surface defects in ceria-based catalysis Author: Andrii Tovt Department: Department of Surface and Plasma Science Supervisor of the doctoral thesis: doc. Mgr. Josef Mysliveček Ph.D., Department of Surface and Plasma Science Abstract: This work concentrates on the analysis of fundamental physicochemical properties of Pt-CeOx, single-atom Pt1 /CeOx, and inverse CeOx/Cu(111) catalysts. Preparation method for stabilized atomically-dispersed Pt2+ ions on ceria was developed and adsorption sites for Pt ions were thoroughly studied using advanced surface science techniques supported by theoretical methods. The mechanism of Pt2+ stabilization on ceria steps was revealed and the step capacity towards Pt2+ ions was estimated. Also, the preparation method for well-ordered cerium oxide ultrathin films with different stoichiometry and ordering of surface oxygen vacancies was developed, and the Ceria/Cu(111) interaction was investigated. Key words: heterogeneous catalysis, model systems, single-atom catalysis, platinum ions, cerium oxide.
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Model systems with the use of CeO2 for bioapplication
Bercha, Sofiia ; Tsud, Nataliya (advisor) ; Lykhach, Yaroslava (referee) ; Švec, Martin (referee)
Title: Model systems with the use of CeO2 for bioapplication Author: Sofiia Bercha Department: Department of Surface and Plasma Science Supervisor: Ing. Nataliya Tsud Ph.D., Department of Surface and Plasma Science Abstract: This thesis is focused on the investigation of model systems for bioapplications. Interfaces between biomolecules and inorganic materials were studied by means of advanced surface science techniques with emphasis on the molecular electronic structure and bonding geometry as a function of material morphology and/or molecular deposition method. For the histidine/cerium oxide system it is demonstrated that the morphology of the oxide determines the mechanism of the molecular adsorption. The presence of an aqueous medium does not alter the histidine interaction with the nanostructured cerium oxide. For the adenine/cerium oxide system we have shown that the adenine molecule chemisorbs on CeO2 intact via nitrogen atoms, independent of the oxide morphology and deposition technique. The adenine molecule was found to decompose on a reduced surface of the cerium oxide. Combining experimental and theoretical methods two distinct phases of adenine on CeO2 were found. For adenine/Cu(111) system it was shown that the strong interaction with the surface keeps the molecule intact on the surface till...
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