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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.
31

Herstellung und Untersuchung zirkoniumbasierter Oxide als Dielektrika zur Anwendung in dynamischen Halbleiterspeichern

Grube, Matthias 02 September 2013 (has links)
In dieser Arbeit sind Dielektrika mit hoher relativer Permittivität untersucht worden, welche eine Anwendung in dynamischen Halbleiter-Speicherzellen (DRAM) zum Ziel haben. Sie unterstützen das Weiterführen der fortschreitenden Miniaturisierung der Speicherzellen bzw. der Erhöhung der Speicherdichten und dienen als Alternative zu den bisherigen Standardmaterialien SiO2 und Si3N4. Als Herstellungsmethoden für mehrkomponentige Oxide wurden zum einen die Molekularstrahl-Deposition und zum anderen die Ko-Sputterdeposition gewählt, da sie eine sehr große Flexibilität bei der Wahl der abscheidbaren Elemente und Oxide bieten sowie eine hohe Ratenstabilität und Reinheit versprechen. Hierfür wurden Prozesse zur simultanen Abscheidung dünner Schichten aus mehreren Quellen entwickelt und optimiert. Als neuartige Dielektrika wurden ZrO2 und SrZrO3 hergestellt und untersucht. Hierbei wurden besonders die dielektrischen und kristallographischen Eigenschaften in Abhängigkeit von der Stöchiometrie umfangreich analysiert. Die maximale erreichte Dielektrizitäszahl des ZrO2 betrug ca. 30 und die des SrZrO3 ca. 31. Es wurde dargelegt, dass die Dielektrizitätszahl des ZrO2 unter bestimmten Umständen von der Schichtdicke im Bereich von 5 bis 50 nm abhängig ist. Dies konnte durch die Beimischung von Sr erfolgreich stabilisiert werden. Die für DRAM-Anwendungen zum Teil zu hohen Leckstromdichten konnten durch die Entwicklung eines neuen Ausheilverfahrens deutlich verbessert werden. Aufgrund der hohen Dielektrizitätszahl in Verbindung mit gesenkten Leckströmen konnte für ZrO2 eine minimale kapazitätsäquivalente Dicke von CET = 1,2 nm und für SrZrO3 eine CET = 1,4 nm erreicht werden, welche der DRAM-Grenze für Leckstromdichten von J = 100 nA/cm² genügen. Diese Werte sind deutlich geringer als die dünnsten, theoretisch möglichen Schichten des klassischen SiO2 und Si3N4, wodurch sowohl ZrO2 als auch SrZrO3 ihr Potential, als Alternative für Speicheranwendungen zu dienen, unterstreichen. / In this work, dielectrics with a high relative permittivity were investigated, which are intended for the application in dynamic random access memory cells (DRAM). Their successful implementation ensures the continuation of the ongoing scaling of memory devices, thus increasing the storage density. They serve as alternative for the standard materials SiO2 and Si3N4. In order to to grow multi-component oxides, molecular beam deposition as well as co-sputter deposition were chosen, given their high flexibility to evaporate various elements and oxides. Additionally, both hold their promise of a good control of the growth rate and high purity. Therefore processes were developed and optimized for growing thin films by using multiple sources simultaneously. The alternative dielectrics ZrO2 and SrZrO3 were fabricated and analysed. Especially, the dependency of the dielectric and crystallographic properties on the stoichiometry were evaluated comprehensively. The highest achieved relative permittivity for ZrO2 and SrZrO3 were approx. 30 and 31, respectively. Under specific and controllable circumstances, the relative permittivity of ZrO2 was found to depend on the film thickness in the range of 5 to 50 nm. However, the admixture of Sr stabilises the relative permittivity. In some cases, the leakage current densities of ZrO2 and SrZrO3 films were too high for DRAM applications. It was possible to decrease those currents drastically by developing a new healing process. The high permittivity in addition with the improved leakage current densities led in the case of ZrO2 to a minimum capacitance equivalent thickness of CET = 1.2 nm and in the case of SrZrO3 to a CET = 1.4 nm, which fulfill the DRAM leakage current density limit of J = 100 nA/cm². Those values are much lower than the thinnest theoretically possible films of the conventional SiO2 or Si3N4. Therefore, ZrO2 and SrZrO3 accentuate their potential for memory applications.
32

ETUDE STRUCTURALE ET MORPHOLOGIQUE DE MULTICOUCHES DISCONTINUES METAL-OXYDE

Micha, Jean-Sébastien 06 March 2002 (has links) (PDF)
Cette étude présente les résultats de caractérisations structurales et morphologiques de multicouches discontinues métal-oxyde, composés d'un empilement de plans de nanoparticules métalliques noyées dans une matrice d'oxyde. L'amplitude de la magnétorésistance tunnel dans ces matériaux dépend de l'organisation du métal à plusieurs échelles. De multiples techniques ont été utilisées afin de sonder l'ordre local structural et magnétique (XAFS, Spectroscopie Mössbauer), l'ordre à moyenne distance (Réflectivité X, GISAXS, MET) et l'ordre à grande distance (Diffraction X). Les données issues de ces différentes techniques sont comparées et confrontées à celles des mesures magnétiques. Trois systèmes ont été étudiés, Fe/ZrO2, Co/ZrO2 et Co/SiO2, en faisant varier l'épaisseur de la couche nominale de métal déposé eM, la température du recuit TR effectué après l'élaboration par pulvérisation cathodique et la vitesse de dépôt des couches. Les ions paramagnétiques mis en évidence en périphérie des nanoparticules ne font pas partie intégrante d'une couche d'un oxyde connu du métal déposé. Ils sont « morts » du point de vue des propriétés magnétiques et électriques. La fraction d'atomes « morts » est plus importante avec la zircone qu'avec la silice et peut être diminuée en augmentant TR, eM et/ou en diminuant la vitesse de dépôt. La valeur de eM correspondant au seuil de percolation dans le plan des couches est déplacée vers les grandes valeurs de eM en augmentant TR. Le mouillage métal-oxyde est important avec la zircone (comparée à la silice) et avec le fer (comparée au cobalt). La morphologie des couches granulaires qui en résulte, notamment la taille des particules, détermine le comportement superparamagnétique ou ferromagnétique des particules. Pour chaque système métal-oxyde, un diagramme schématique (TR, eM) résume les propriétés magnétiques, structurales et morphologiques observées.
33

Développement de surface artificielles pour cathode sous forme de couche mince pour accumulateurs Li-ion / Development of artificial surface layers for thin film cathode materials

Carrillo solano, Mercedes alicia 30 October 2015 (has links)
Ce travail porte sur la recherche de différentes compositions de couches minces pouraccumulateurs Li-ion.Une première partie a été dédiée au dépôts de cathode sous forme de couche mince d’unmatériau connu, LiCoO2, et d’un matériau alternatif, Li(NiMnCo)O2 en utilisant le dépôtphysique en phase vapeur (PVD) et le dépôt chimique en phase vapeur (CVD),respectivement. Les résultats (LiCoO2) ont montrés comment, après cyclage, il y a diminutionde la capacité à cycler à régime rapide et augmentation de la résistance à l’interface. Ladiffraction des rayons X a montré la présence de différentes orientations, peu cristallisées,appartenant à la phase LiCoO2 HT selon confirmation par la littérature. Les couches mincesde Li(NixMnyCo1-x-y)O2 ont été préparées par dépôt chimique en phase vapeur assisté paraérosol. La diffraction des rayons X et l’analyse Rietveld utilisant le modèle March-Dollase aété mise en oeuvre pour la détermination de la texture et des caractéristiques microstructurales.La morphologie des films a été caractérisée par microscopie électronique à balayage. L’étudea montré que la concentration de la solution de précurseur et la pression totale ont un effetmajeur sur la morphologie des films et leur texture.Une seconde partie s’est focalisée sur l’interface cathode-électrolyte pour trois cas d’étude : 1)couche mince de matériau de cathode LiCoO2, 2) couche mince de LiCoO2 recouvert de ZrO2et 3) couche mince de LiCoO2 recouvert de LIPON. L’interface cathode-électrolyte de cestrois cas d’étude a été étudiée avant et après cyclage galvanostatique afin de déterminer lescaractéristiques de la couche de surface et les changements provenant à l’interface lors dufonctionnement de l’accumulateur. L’interface des couches minces de LiCoO2 a été étudiéeplus en détail après trempage dans un électrolyte liquide afin de comprendre l’effet desprocédures de stockages courts dans les accumulateurs.De plus, les couches minces de LiPON ont été étudiées sur la base de changementsstructuraux se produisant avec la nitruration et sa corrélation à un possible mécanisme ayantlieu durant la conduction ionique. / The present work was based on the investigation of different thin film components of Li ionbatteries. A first part was dedicated to the deposition of cathodes in thin film form of aknown material, LiCoO2, and an alternative one, Li(NiMnCo)O2 employing physical vapordeposition (PVD) and chemical vapor deposition (CVD), respectively. Results on thedeposition of LiCoO2 showed how after cycling there is a reduction of rate capability andincrease in interface resistance. The X-ray diffraction pattern showed the presence of severalorientations related to the known HT phases found in literature for LiCoO2 with lowcrystallinity. On the other hand Li(NixMnyCoz)O2 thin films prepared via aerosol assistedCVD were analyzed with X-ray diffraction and Rietveld refinement using the March-Dollasemodel for the determination of the texturing and microstructural characteristics. Additionallythe morphology of the films was characterized using scanning electron microscopy. Theinvestigation showed that concentration of precursor solution and process pressures have asignificant effect on the film morphology and texturing. A second part was focused on the cathode-electrolyte interface for three case studies: 1) asdeposited LiCoO2 cathode thin film, 2) ZrO2 coated LiCoO2 thin film and 3) LiPON coatedLiCoO2 thin film. The interface cathode-electrolyte of these three cases were studied beforeand after galvanostatic cycling to determine surface layer characteristics and changes arisingon the interface after battery operation. The interface of a bare LiCoO2 layer was furtherstudied after soaking in liquid electrolyte to elucidate the effect of short storage procedures inbatteries.Surface analysis done on LiCoO2 thin films showed changes occurring at the interface layersafter the electrode was in short contact with the electrolyte solution and after galvanostaticcycling. Washing and soaking the electrode material in electrolyte and solvent showed thatsurface reactions start from the first contact. A main component of the electrolyte solution,LiPF6, has critical effect since it can decompose and form HF which reacts with carbonatesand forms LiF on the surface. Given the large amount of LiF, a high reactivity of LiCoO2 withthe decomposed species was observed, as the main components of the film were related to thedecomposed LiPF6 salt.The surface chemistry of the layer formed on LiCoO2 after cycling was mainly based ondecomposed species from the electrolyte salt arising from carbonated and fluorinated species.Artificial surface layers were deposited on LiCoO2 by means of rf sputtering. The thin layersof ZrO2 and LiPON used as coatings had minor effects on the original film morphology andcrystalline structure. An XPS analysis of the interface showed how the nature of each layerafter galvanostatic cycling was different for each case. The resulting artificial surface layerformed from ZrO2 coating showed mainly inorganic species, while the LiPON coatedcathode showed an organic nature. The final surface layers after electrochemical cycling ofthe ZrO2 coated film resembled that of the uncoated LiCoO2. Additionally, LiPON thin films were studied on the basis of structural changes occurringwith nitrogenation and its correlation to a possible mechanism during ion conduction.Composition of phosphate glasses with rf sputtering was proven to be greatly influenced bythe gas ratio employed. The largest variations were observed for lower amounts of N2 in thegas mixture. The IR spectra results showed important differences in the short range order forfilms with a similar amount of lithium. The lithium phosphorus oxynitride films depositedhere presented glassy structures with mainly ortho and pyro-phosphate units with smallamounts of short metaphosphate chains. Nitrogen insertion favors stability of lithium bygiving an environment with lower potential energy, as was evidenced by the far-IR results.
34

Materiais com gradiente funcional (MGF) à base de alumina (Al2O3) e zircônia estabilizada com ítria (3Y-ZrO2) obtidos por coprensagem e sinterização em dois estágios / Functionally graded materials based on alumina/zirconia composites processed by co-pressing and two-stage sintering

Antonio Luiz Pereira Neto 20 June 2016 (has links)
O interesse em materiais com gradiente funcional (MGF) tem crescido nos últimos anos devido à possibilidade de se obter peças com variação de propriedades ao longo de uma ou mais dimensões, gerando desempenho ótimo dependendo da solicitação imposta ao material. Por outro lado, a sinterização em dois estágios, consiste em aquecer a peça conformada até que esta apresente densidade relativa entre 75% e 92% da densidade teórica, e, em seguida, submetê-la a um resfriamento rápido até uma temperatura inferior, onde deve permanecer por um período até o fim da densificação. Desta maneira, é possível obter peças densas, com tamanho médio de grãos inferior ao obtido via sinterização convencional, melhorando suas propriedades mecânicas. Neste trabalho, foram caracterizados, por dilatometria, compósitos alumina-zircônia parcialmente estabilizada com ítria (3Y-ZrO2), com teor de ZrO2 variando de 0 a 30% massa/massa. Após compatibilização do comportamento destes compósitos durante a sinterização e determinação da temperatura de pico do processo de sinterização em dois estágios (TSS), foram montadas peças com gradiente de composição. Estas peças foram sinterizadas em dois estágios, com temperatura de pico de 1450°C e temperatura de patamar de 1350°C por 8 horas. A microestrutura foi avaliada com o uso de microscópio eletrônico de varredura e realizou-se a caracterização mecânica por ensaios de dureza, tenacidade à indentação, a fim de se fazer um estudo comparativo dos resultados obtidos para as peças sinterizadas em dois estágios com os das peças com gradiente funcional densificadas via sinterização convencional a 1500°C. A co-prensagem, seguida da técnica de sinterização em dois estágios utilizada para obtenção de peças com gradiente funcional, foi eficiente em produzir peças com densidade aparente relativa de 98,1% DT, valores de tenacidade a indentação variando entre 4,3 MPa.m1/2 a 9,8 MPa.m1/2 e valores de dureza entre 17,5 GPa a 18,4 GPa. / The interest for functionally graded materials (FGM) has grown up during last 2 decades owing to the possibility of developing pieces and devices with a gradual properties variation along one or more dimensions, which allows an optimum performance as a function of imposed solicitation. On the other hand, two stage sintering is a relative new sintering technique, where the shaped pieces are heated up to a relative density of 75-92% t.d., followed by a fast cooling step, up to an inferior temperature, where the piece in maintained up to the end of dense structures, whit finer microstructures, responsible for better mechanical properties. In this work, we characterized alumina-ytria-stabilized zirconia composites, with different amounts of 3Y-ZrO2, by dilatometry. After fitting thermal behavior of the distinct composites during sintering and determining temperature of maximum densification rate, co-pressed FGMs were constructed. Then pieces were sintered by pressureless traditional technique and two stage sintering, with a peak temperature of 1450°C and soaking temperature of 1350°C x 8 hours. Microstructure was studied by SEM and mechanical properties: microhardness and indentation toughness, in order to compare pressureless sintered FGMs at 1500°C and two stage sintered FGMs.
35

Flammgespritzte Schichten im System Al2O3-TiO2-ZrO2

Kratschmer, Tim 17 January 2011 (has links) (PDF)
Beim Flammspritzen von Mischungen im System Al2O3-TiO2-ZrO2 treten vielfältige Effekte auf. Es kommt z.B. zur Ausbildung eines amorphen Anteils, der in Form von amorphen Sublamellen, dem primären amorphen Anteil, und in dendritisch geprägten Bereichen, dem sekundären amorphen Anteil im Gefüge vorliegt. Dieser beeinflusst die mechanischen Eigenschaften deutlich. Bei einer Temperaturbehandlung entstehende Ausscheidungen von ZrO2 oder verschiedenen Zirkoniumtitanaten beeinflussen die mechanischen Eigenschaften ebenfalls signifikant.
36

Oxydation en voie humide des effluents des distilleries d'alcool à partir de canne à sucre en présence de catalyseurs Ru et Pt supportés sur TiO2 ou ZrO2 / Wet air of alcohol distillery effluent from sugarcane in the presence of noble catalysts (RU, PT) supported on TiO2 or ZrO2

Le, Phuong Thu 24 October 2013 (has links)
La vinasse est un effluent aqueux issu des distilleries d'éthanol produit à partir de mélasse de canne à sucre, caractérisé par une couleur intense, une forte Demande Chimique en Oxygène (DCO) et un faible Demande Biologique en Oxygène (DBO). Le traitement de ce type d'effluent par Oxydation en Voie Humide (OVH) a fait l'objet d'une étude sur catalyseurs métaux nobles supportés sur TiO2 ou ZrO2 à 190-210°C sous 50-70 bar d'air. L'addition de catalyseurs au Ru permet la minéralisation complète de la partie carbone des polluants modèles (saccharose, polyéthylène glycol, mélanoïdine) ou des effluents réels (vinasse de Cognac et vinasse de canne); les catalyseurs au Pt sont également très efficaces, mais ne convertissent que très peu l'acide acétique formé intermédiairement. Dans ces conditions, l'azote sous forme organique est converti en ammonium. Alors qu'en l'absence de catalyseur, les ions ammonium sont stables, l'addition d'un catalyseur est capable de convertir l'ammonium en diazote et nitrate. Les sélectivités relatives en N2 et NO3 - dépendent des conditions oxydantes de la réaction (quantité d'azote à traiter par rapport à la quantité de métal actif). De manière générale, le platine se révèle plus sélectif en diazote. Une lixiviation des métaux a été détectée au démarrage des réactions d'OVHC des effluents à cause de l'azote sous forme organique ; elle diminue et disparaît au fur et à mesure de la minéralisation de l'azote et le métal se redépose sur le solide catalytique. Les essais en réacteur continu confirment les observations en réacteur batch / Vinasse is an aqueous effluent originating from ethanol production process from sugarcane. It is a dark brown effluent with an extremely high COD and a low BOD. The treatment of this type of effluent by wet air oxidation (WAO) was the subject of this study using noble metal catalysts supported on TiO2 and ZrO2 at 190-210 ° C under 50-70 bar air. The addition of Ru catalysts allowed the complete mineralization of the organic model pollutants (sucrose, polyethylene glycol, melanoidin) or the real effluents (cognac vinasse and cane vinasse); the Pt catalysts were also very effective, but acetic acid was formed as an intermediate which was difficult to be converted. Under these conditions, the organic nitrogen was converted to ammonium. Whereas in the absence of catalyst, the ammonium ions were stable, the addition of a catalyst was capable of converting ammonium to dinitrogen and nitrate. The selectivity to N2 and NO3 - depended on the oxidizing reaction conditions (molar ratio nitrogen/metal). In general, platinum proved to be more selective to dinitrogen. Metal leaching was detected upon CWAO of effluents containing organic nitrogen. The leaching decreased and disappeared as nitrogen was mineralised and the dissolved metal redeposited on the solid catalyst. The continuous reactor tests confirmed the observations in the batch reactor
37

Flammgespritzte Schichten im System Al2O3-TiO2-ZrO2

Kratschmer, Tim 14 December 2010 (has links)
Beim Flammspritzen von Mischungen im System Al2O3-TiO2-ZrO2 treten vielfältige Effekte auf. Es kommt z.B. zur Ausbildung eines amorphen Anteils, der in Form von amorphen Sublamellen, dem primären amorphen Anteil, und in dendritisch geprägten Bereichen, dem sekundären amorphen Anteil im Gefüge vorliegt. Dieser beeinflusst die mechanischen Eigenschaften deutlich. Bei einer Temperaturbehandlung entstehende Ausscheidungen von ZrO2 oder verschiedenen Zirkoniumtitanaten beeinflussen die mechanischen Eigenschaften ebenfalls signifikant.
38

[en] ISOBUTENE SYNTHESIS FROM ETHANOL EMPLOYING A PHYSICAL MIXTURE OF IN2O3 AND ZRO2 / [pt] SÍNTESE DE ISOBUTENO A PARTIR DO ETANOL EMPREGANDO UMA MISTURA FÍSICA DE IN2O3 E ZRO2

BRUNA JULIANA DA SILVA BRONSATO 26 May 2020 (has links)
[pt] Nos últimos anos, a crescente preocupação com o meio ambiente tem impulsionado o desenvolvimento de processos alternativos e sustentáveis para a obtenção de compostos importantes na indústria química. O isobuteno é um hidrocarboneto, comumente utilizado como intermediário para a síntese de diversos produtos, como polímeros e aditivos de combustíveis. A principal forma de produção desse hidrocarboneto é a partir do craqueamento da nafta, pelo qual é produzido como um coproduto por uma via dependente de fontes fósseis. Para atender à demanda de isobuteno associado a uma produção sustentável, novos estudos têm sugerido a síntese dessa olefina a partir da conversão catalítica de compostos como o etanol, uma matériaprima renovável que pode ser obtida a partir do processamento de diferentes biomassas. Experimentos recentes mostraram que uma mistura física In2O3+ZrO2 apresenta o mesmo desempenho de catalisadores In2O3/ZrO2, sendo ambos promissores para esse tipo de reação química. Assim, o objetivo deste estudo consiste em investigar esta mistura física como catalisador na síntese do isobuteno a partir do etanol. Nesta pesquisa, os catalisadores In2O3, ZrO2 e uma mistura física In2O3+ZrO2 foram avaliados por testes catalíticos em leito fixo e caracterizados pelas técnicas de DRX, XPS, EPR, TPD (CO, CO2, isopropanol, etanol e acetona), Fisissorção de N2, TPR-H2 e espectroscopia de infravermelho com adsorção de piridina. Os resultados revelam que a mistura física apresenta uma atividade catalítica superior ao In2O3 e ao ZrO2 puros, sendo capaz de formar isobuteno com uma seletividade de 36 por cento. O efeito sinérgico desses dois óxidos é verificado, resultando na formação de vacâncias catiônicas e aniônicas no catalisador MF, bem como promovendo as propriedades redox e básicas do sistema. / [en] In recent years, the growing concern with the environment has driven the development of alternative and sustainable processes to obtain important compounds in the chemical industry. Isobutene is a hydrocarbon commonly used as an intermediate for the synthesis of various products such as polymers and fuel additives. The main form of the production of this hydrocarbon is from the cracking of naphtha, by which it is produced as a co-product by a pathway dependent on fossil sources. To meet the demand for isobutene associated with sustainable production, new studies have suggested the synthesis of this olefin from the catalytic conversion of compounds such as ethanol, a renewable raw material that can be obtained from the processing of different biomasses. Recent experiments have shown that an In2O3+ ZrO2 physical mixture (MF) has the same performance as In2O3/ZrO2 catalysts, both of which are promising for this type of chemical reaction. Thus, the aim of this study is to investigate this physical mixture as a catalyst in the synthesis of isobutene from ethanol. In this research, the In2O3, ZrO2 catalysts and an In2O3+ZrO2 physical mixture were evaluated by fixed bed catalytic tests and characterized by the techniques of XRD, XPS, EPR, TPD (CO, CO2, isopropanol, ethanol and acetone), N2 physisorption, TPR-H2 and infrared spectroscopy with pyridine adsorption. The results show that the physical mixture has a catalytic activity superior to pure oxides, In2O3 and ZrO2, being able to form isobutene with a selectivity of 36 percent. The synergistic effect of these two oxides is verified, resulting in the formation of cationic and anionic vacancies in the MF catalyst, as well as promoting the redox and basic properties of the system.
39

Fuel Reforming for Hydrogen Production in Heavy-Duty Vehicle Applications

Granlund, Moa. Z. January 2015 (has links)
The depletion of fossil fuels together with growing environmental concerns have created incitement for developing a more energy-efficient and environmentally-friendly vehicle fleet. The development towards cleaner heavy-duty vehicles started already in the 80’s with the introduction of emission legislations. Initially, engine optimization was enough for reaching the legislated levels of emissions. However, at present engine optimization is not enough but exhaust aftertreatment has become an essential part of heavy-duty vehicles, in order to meet the emission standards. Today, the total emissions are targeted which means that there is an interest in decreasing the idling emissions as well as the emissions during operation. To reduce the overall emissions several states in the USA have introduced idling legislations. Due to the limitations in idling time alternative solutions for power generation during rests are requested. A possible alternative is a fuel cell auxiliary power unit, combining a fuel cell with a fuel reformer (FC-APU).  The focus of this thesis is the development of the fuel reformer for an FC-APU, in which the hydrogen to the fuel cell is generated from diesel in a high-temperature catalytic process. The produced hydrogen can also be used in other heavy-duty vehicle applications i.e. selective catalytic reduction of NOx (HC-SCR), where addition of hydrogen is essential for reaching high conversion at low temperatures. The effect of using hydrogen from a fuel reformer in HC-SCR is included in this work. The catalytic material development is focused on developing promoted materials with lower rhodium content but with catalytic activity comparable to that of materials with higher rhodium content. This includes evaluation and extensive characterization of both fresh and aged promoted materials. The work also includes reactor design where a micro reactor with multiple air inlets is evaluated. This work has contributed to increased knowledge of catalytic materials suitable for reforming of diesel. By changing the support material from the traditionally used alumina to ceria-zirconia, increased H2 yield was achieved. In addition, the ceria-zirconia supported material was less prone to coke. By promoting the material with cobalt or lanthanum it was possible to decrease the rhodium content by 2/3 with enhanced catalytic performance. It was also discovered that promotion with lanthanum decreased the tendency for coking even further. Additionally, the lanthanum-promoted material had higher thermal stability as well as a stable highly dispersed rhodium phase. Furthermore, the work has contributed to an increased knowledge concerning the fuel reformer’s effect on HC-SCR. The work displays clear evidence of benefits with using hydrogen-rich gas from a fuel reformer instead of pure hydrogen. The benefits are derived from the content of low molecular weight hydrocarbons present in the hydrogen-rich gas, which are strong reducing agents increasing the NOx reduction. This finding proves that fuel reforming in combination with HC-SCR is a viable option for NOx abatement. / <p>QC 20150202</p>
40

High quality molecular beam epitaxy growth and characterization of lead titanate zirconate based complex-oxides

Gu, Xing 07 December 2007 (has links)
Research interest in complex oxides has resurged owing to progress in modern epitaxial techniques. Among such oxides, lead-titanate-based thin films such as PbTiO3 (PTO) and Pb(ZrxTi1−x)O3 (PZT) offer attractive advantages for a wide variety of applications. Moreover, integration between functional oxides with compound semiconductors has the potential to realize multi-functional devices which enjoy the properties from both groups of materials. Ferroelectric materials with a perovskite structure (ABO3) and semiconductors such as GaN with a hexagonal structure, require a careful choice of a bridge layer and suitable epitaxial technique. Molecular beam epitaxy (MBE) has been an established technique in providing epitaxial growth with high crystal perfection and precise control over material composition. Single-crystal oxides grown by molecular beam epitaxy (MBE) can in principle avoid grain boundaries and provide a sharp interface as well. In this dissertation, the MBE growth mechanism of PZT was investigated. In-situ RHEED patterns indicate that the growth of PTO and PZT occur in a two-dimensional, layer by layer mode, as confirmed by a streaky pattern. The crystal quality of PTO, PZO, and PZT thin films prepared by MBE are evaluated by X-ray diffraction (XRD), and have a full width at half maximum (FWHM) value of 4 arcmin for an 80nm thick layer. Optical properties of the PTO thin films have been characterized by variable angle spectroscopic ellipsometry (VASE), and well resolved dielectric functions are extracted. The refractive index is determined as 2.605 at 633 nm, and bandgap energy as 3.778eV. The electrical properties of the PTO and PZT are evaluated by the measurement of polarization-field hysteresis loops, give a remanent polarization of 83 μC/cm2 and a coercive field of 77 kV/cm. Lead oxide (PbO), titanium dioxide (TiO2), and zirconium dioxide (ZrO2), on GaN templates for potential PZT/GaN integration. The epitaxial growth of TiO2, PbO, and ZrO2 is realized on GaN templates for the first time by MBE. The PbO epitaxial layer was also used as a nucleation layer to enable single crystalline, perovskite PTO growth on GaN.

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