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    Elektronen-induzierte Reaktionen von Koordinationspolymeren zur Nanostrukturierung von Oberflächen
    Electron-induced reactions play a central role in the development of current methods for nanostructuring of surfaces. The basic principle is the decomposition of metal-containing compounds by a focused electron beam. In the present work the electron-induced reactions of three different copper-containing materials, namely, copper(II) oxalate, copper(II) squarate, and copper(II) 1,3,5-benzenetricarboxylate, were examined in detail. Reflection absorption infrared spectroscopy (RAIRS) and X-ray photoelectron spectroscopy (XPS) were used to identify chemical surface species that are formed upon electron exposure. To determine volatile decomposition products the electron-stimulated desorption (ESD) of neutral fragments was monitored with a new designed UHV setup. In addition, morphological changes of the samples were investigated by helium ion microscopy (HIM). It was shown that the molecular structure of the used anions is decisive for the efficiency and the outcome of the electron-induced decomposition. As an example, surface-bound layers of copper(II) oxalate were identified as suitable precursors for the production of metallic nanoparticles.
    doctoral thesis
      338  496
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    Synthese, Charakterisierung und katalytische Untersuchungen an bimetallischen nanoskaligen Systemen
    Synthesis and Characterization of bimetallic nanostructured materials via DRIFT spectroscopy and catalytic performance in CO oxidation and methanol decomposition are the main topics of this work. It is essentiell for the development of new catalysts to characterize them under reaction conditions or at least close to the conditions of the particular technical prozess. Thus for the development of new catalytic active materials two different approaches were chosen. Bimetallic colloidal nanoparticles were synthezised on new routes and tested on their applicability in heterogeneous catalysis. Similar test were performed with nanoporous gold, which represents an inverse system compared to nanoparticles. Furthermore the interactions of the reactants with the catalyst surface were analyzed by DRIFT spectroscopy. Whereas it becomes possible to gain insite into the reaction mechanisms under normal conditions. Under this means bimetallic systems are a matter of particular interest, because of the changing chemical and physical characteristics which occur by the mixture of two metals. This may upgrade the performance of the catalyst.
    doctoral thesis
      250  404
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    Funktionalisierung poröser Goldsysteme
    The controlled functionalization of the surface of nanoporous gold (npAu) was investigated. The npAu was used as a platform for tailored modification with entities such as metal oxides, ad-metals or organic molecules for influencing surface chemistry in heterogeneous catalysis. TiO2 and PrOx were deposited by ALD, CVD and liquid phase impregnation on the npAu. The oxide-npAu material showed remarkable activity (already at 25°C) and stability up to 600 °C with respect to CO oxidation as well as NO reduction. Critical parameters regarding the oxidative coupling of primary alcohols and amines to amides were identified on bare npAu. These insights were used for tuning the surface composition by introducing small quantities of Ag and Ru resulting in an increase of activity by a factor of 2.5. In a 2-step synthetic route npAu was functionalized with a) redox-active entities for electrochemical applications and b) photoactive entities for enhanced photocatalytic conversion of Citronellol.
    doctoral thesis
      330  225