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BTU
Experimental data on the reaction kinetics of catalytic processes are prerequisite for modeling of such reactions and their output. We investigate the CO oxidation on
some noble metal catalysts, like Iridium(111) and Palladium(111) which is a bistable surface reaction. In a specific range of CO content in the feed gas islands of one or the other adsorbate nucleate and grow, which is recorded with photo electron emission microscopy (PEEM). During these transients the coverage on the surface
changes from predominantly oxygen covered to predominantly CO covered resp. vice versa. But the resolution of PEEM and especially its unknown and nonlinear dependence of coverage of the two adsorbates (oxygen and CO) and image intensity make it impossible to extract the changes in coverage. On the other hand the reaction diffusion model based on the Langmuir-Hinshelwood-mechanism delivers
the coverage of oxygen and carbon monoxide. The shapeand wall velocity of those islands has been connected perfectly to each other [CPL 423 (2006) 39], but not the
absolute coverage and their variation during the reaction. Since the domain wall velocity is small on Iridium(111), this has opened the possibility for a detailed
analysis of the changing coverage inside this domain wallutilizing synchrotron radiation and photo electron spectroscopy at BESSY II. The coverage profile of
oxygen and CO inside a moving domain wall was measured for both cases using XPS spectra at O1s, C1s and the valence band during thereaction. Comparison with the reaction-diffusion-model and other catalytic surfaces, like Palladium(111) are done.
Combining Hardware and Software Based Self Repair Methods for Statically Scheduled Data Paths
(2010)
In the framework of this thesis, synchrotron radiation based spectroscopy methods are applied to study the electronic structures of stoichiometric Rutile single crystals and TiO2 thin films, and the initial stage of chromium and cobalt growth on TiO2 thin films.
Resonance photoemission spectroscopy of clean TiO2 at the Ti L2,3 edges led to Auger-like features, with kinetic energies corresponding to the Ti L2,3M4,5M4,5 Auger decay channels. The presence of these features is assigned to origin from a d2L2 charge transfer state. The resonance of the Ti L3M2,3V Auger channel at the Ti L2 edge is assigned to the L2L3V Coster-Kronig Auger, followed by the normal L3M2,3V Auger decay.
The deposition of chromium on the TiO2 film causes a strong interaction at the interface, in which TiO(2-x) is formed together with chromium in the Cr 3+ state. Besides the oxidized component, contribution of metallic chromium is found as well. In the ultra-low coverage regime, post-deposition oxidation is observed, in which metallic chromium is oxidized to Cr2O3, accompanied by re-oxidation of the substrate to TiO2. The interface reaction is also reflected by the appearance of two defect states in the band gap. Resonant photo-emission at the Cr 2p and Ti 2p edges shows well distinguishable Cr 3d respectively Ti 3d character of the respective states. Indications for self-cleaning properties are found by removal of surface carbon during storage in UHV, but the influence of chromium on these properties is not studied in detail.
The interaction between cobalt and TiO2 is weaker than that of chromium and TiO2. Nevertheless, an interface reaction is found, in which some of the deposited cobalt is oxidized, while the oxide support is partly reduced. The particular oxidation state of Cobalt is identified by means of multiplet calculation including charge transfer and crystal field effects. The calculated XAS and XPS spectra indicate Co 2+ in a tetrahedral coordination with four oxygen atoms. The metallic component of cobalt gives rise to a broad resonance in the valence band down to -20 eV, with a pronounced satellite feature that reflects the oxidized component.
Ein wichtiges Ziel der Bundesregierung ist der Ausbau des Anteils erneuerbarer Energien an der gesamten Stromerzeugung. Die Entwicklung optimierter Wärme- und Kältespeicher stellt einen wichtigen Baustein bei der Erreichung dieser Zielstellung dar. Elektrisch betriebene Wärmepumpen und Kompressionskältemaschinen sowie dezentrale Klein-BHKW bieten in Verbindung mit entsprechend dimensionierten, thermischen Speichern ein großes Potential zum Lastmanagement in Smart Grids und somit zur Netzintegration von Strom aus erneuerbaren Energien. Die im Projekt entwickelte Methodik zur Suche nach neuen Latentspeichermedien kann für ein breites Anwendungsfeld von Heiz- und Kühlanwendungen in Gebäuden bis hin zur Kraftwerkstechnik eingesetzt werden. Innerhalb der Fördermaßnahme „Anwendungsorientierte Forschung und Entwicklung zur nichtnuklearen Energieforschung“ im 6. Energieforschungsprogramm der Bundesregierung wurde durch die Projektarbeiten das Schwerpunktthema Energiespeicher (3.8) adressiert, wobei der Aspekt der Entwicklung neuer Materialien mit reduzierten Kosten für einen wirtschaftlichen Betrieb im Vordergrund stand. Speziell wurden dabei die Unterpunkte 3.8.4 Thermische Speicher zur Weiterentwicklung, Optimierung und Erprobung von PCM sowie 3.8.5 Übergeordnete Themen mit Modellen und Simulationswerkzeugen für die Auswahl und Bewertung neuer Speichermaterialien adressiert.
Die Projektergebnisse besitzen aber auch Berührungspunkte mit den Schwerpunkten 3.12 Energieeffizienz in Industrie, Gewerbe, Handel und Dienstleistungen sowie 3.4 Solarthermische Kraftwerke, da mit der entwickelten Screening-Methode für diese Anwendungsfälle neue Wärmespeichermaterialien auf der Basis wasserfreier Salze mit höheren Prozesstemperaturen gefunden werden können.
Durch den Einsatz von Methoden zur Modellierung und Simulation von Prozessen erfolgt gleichermaßen die Umsetzung einer energie- und ressourcenschonenden Forschungstätigkeit. Das im Projekt entwickelte Vorgehen hilft dabei, einen äußerst sparsamen Einsatz von Chemikalien, eine niedrige Belastung der Umwelt durch verringerten Entsorgungsaufwand der verbrauchten Stoffe sowie einen deutlich geringeren Aufwand und Energieeinsatz für die Messtechnik zu ermöglichen. Damit wurde zugleich das Schwerpunktthema 3.8.5 Modelle und Simulationswerkzeuge für die Auswahl und Bewertung neuer Speichermaterialien angesprochen.
Photovoltaik- und Windenergieanlagen spielen eine Schlüsselrolle für eine klimagerechte Energieversorgung. Zukünftig werden sie einen Großteil des Energiebedarfs decken – auch in den Sektoren Wärme und Verkehr. Studien zeigen: Für Klimaneutralität 2045 muss die Ausbaugeschwindigkeit auf das Drei- bis Vierfache der letzten Jahre erhöht werden. Komplexe und langwierige Planungs- und Genehmigungsverfahren, zu wenig ausgewiesene Flächen und eine unzureichende Bürgerbeteiligung hemmen jedoch den Ausbau.
Das Impulspapier „Vorschläge für einen klimagerechten Ausbau der Photovoltaik und Windenergie“ einer interdisziplinären Arbeitsgruppe des Akademienprojekts Energiesysteme der Zukunft (ESYS) nennt zwölf Handlungsoptionen, um Hemmnisse abzubauen und die Ausbaugeschwindigkeit auf die erforderlichen 15 bis 25 Gigawatt pro Jahr zu beschleunigen.
Small metallic particles deposited on oxide surfaces can serve as heterogeneous catalysts, as for example TiO2 supported cobalt is a known Fischer-Tropsch-Catalyst.
The goal of the presented studies is to investigate the interaction between cobalt and TiO2 in the initial step of growth by synchrotron radiation based spectroscopy.
PES studies of TiO2 supported cobalt show a reduction of the oxide support, accompanied by an oxidation of the deposited material. The oxidation is not complete, but metallic cobalt is found already in the very first step of growth. Uniform decrease of both substrate PES lines indicate very weak interaction between overlayer and TiO2.
An atomic multiplet calculation including charge transfer and crystal field effects is applied to simulate the experimental Co 2p XAS and XPS spectra of the oxidized component. The results allow the identification of the local coordination as well as the identification of the oxidation state of cobalt.
Oxide supported metal films and clusters offer interesting properties with a wide range of possible applications. In this context, Titanium Dioxide is chosen as a model substrate due to its simple electronic structure with a d0 configuration. We study the interaction of ultrathin Chromium films deposited on TiO2 film with focus on the modifications of the valence band and band gap region. Normal photoemission in bulk and surface sensitive modes as well as resonant photoemission at the Cr 2p and Ti 2p edges are used to distinguish the different Cr 3d and Ti 3d contributions to the valence band. In the initial step we find to gap states of distinct character with a sharp resonance of the Cr 3d related state at the Cr 2p edge. With increasing layer thickness we observe that this resonance extends to about 20 eV below the Fermi-Energy. Datasets of valence band spectra measured around the Cr 2p edge show 2 resonant mechanisms in this case i.e. a participator channel for the 3d state accompanied by a spectator channel at fixed kinetic energy.
We investigate the electronic structure of TiO2 thin films by SR-PES, NEXAFS and ResPES. The films are prepared in a combined in-situ/ex-situ process that leads to stoichiometric thin films (≈ 10 nm) in Rutile structure. We focus on ResPES at the Ti 2p edge. When the photon energy is close to the Ti 2p absorption edge we observe additional features about 13 eV below the valence band main features. These features show clear spectator auger decay at the resonance leading to d0 final state. From this, we deduce the existence of the d2L2 initial charge transfer state as this is the only possible channel that enables the corresponding spectator auger decay. These features have the same origin as the satellite structures observed in core level spectra, esp. 2p and 3p.
The initial stages of Chromium growth on Titaniumdioxide-Investigations using synchrotron radiation
(2007)
We investigate the interface of Cr-TiO2 during the initial stages of Cr deposition. Experiments are carried out at BESSY II (BL U49/2-PGM2). Using XPS, XAS and ResPES we obtain information about electronic structure at the interface. We confirm the results of growth studies by Christian Winde obtained by TEM-EELS. In addition, we find that Cr deposition induces two gap states which appear about 1 eV and 3 eV below EF. Using ResPES, these states can be identified as being Cr-like and Ti-like respectively. Core-level-XPS and CIS-spectra of the lower gap state indicate the existence of mainly Cr4+ at low coverage (< 1 ML). At higher coverage (≈ 2.5 ML) metallic Cr is observed as well as metallic Ti. Oxidized Cr occurs mainly as Cr3+. CIS-spectra of higher gap state show metallic behavior with both Cr- and Ti-like character. CIS-spectra of lower gap-state confirm the existence of Cr3+.
Reference: Christian Winde, Herstellung und Charakterisierung von Cr Schichten auf TiO2 (110)Oberflächen, PhD Thesis, University of Stuttgart, 2002