Selectivity in Methanol Oxidation as Studied on Model Systems Involving Vanadium Oxides

Oxidation catalysts are modeled by oxide single crystals, thin oxide films, as well as supported oxide nanoparticles. We characterize the surface of those materials using a variety of surface sensitive techniques including scanning tunneling microscopy and spectroscopy, photoelectron spectroscopy, infrared spectroscopy, and thermal desorption spectroscopy. We find temperature dependent structural transformations from V₂O₅(001) to V₂O₃(0001) via V₆O₁₃(001). V₂O₃(0001) is found to be vanadyl terminated in an oxygen ambient and it loses the vanadyl termination after electron bombardment. It is shown that the concentration of vanadyl groups controls the selectivity of the methanol oxy-dehydrogenation towards formaldehyde. A proposal for the mechanism is made. The results on single crystalline thin films are compared with similar measurements on deposited vanadia nanoparticles. The experimental results are correlated with theoretical calculations and models.     

Preparation of Phase-Pure M1 MoVTeNb Oxide Catalysts by Hydrothermal Synthesis—Influence of Reaction Parameters on Structure and Morphology

This work presents a detailed investigation of the preparation of MoVTeNbO _x catalysts by hydrothermal synthesis. Phase-pure synthesis of M1 has been achieved applying the metals in a molar ratio Mo/V/Te/Nb = 1/0.25/0.23/0.12. Raman, UV/Vis spectroscopy, and SEM/EDX analysis show that the elements are inhomogeneously distributed in the initial suspension that is formed after mixing the metal salts in an aqueous medium. Iso- and heteropoly anions of molybdenum, free telluric acid as well as supra-molecular polyoxometalate clusters are observed in the solution, whereas all metals have been found in the precipitate. Complete rearrangement of molecular building blocks under hydrothermal conditions is essential for formation of phase-pure materials. Optimized synthesis conditions with respect to temperature and time result in the formation of a precursor consisting of nano-structured M1 characterized by an extended periodic organization in the [001] direction and a fairly homogeneous distribution of the elements. Residual ammonium containing supra-molecular species in the precursor result in the formation of phase mixtures during the subsequent crystallization by heat treatment in inert gas. Phase-pure M1 exhibits a distinct degree of flexibility with respect to the chemical composition that becomes obvious by incorporating Nb not exclusively into pentagonal bi-pyramidal units, but also into octahedral coordinated positions as shown by EXAFS. Anisotropic growth of the needle-like M1 crystals has been observed during the final heat treatment performed at 873–923 K in inert atmosphere disclosing a potential method to control the catalytic properties of MoVTeNbO _x catalysts.     

Föderatives Identitätsmanagement am Beispiel der elektronischen Fallakte

Zusammenfassung Für Krankenh?user sind Anwendungen für kooperativ angelegte Behandlungsprozesse wesentliche Werkzeuge um einen zeitnahen einrichtungs- und sektorübergreifenden Austausch patientenbezogener medizinischer Daten zu gew?hrleisten.