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With surface X-ray diffraction (SXRD) using a high-pressure reaction chamber we investigated in-situ the oxidation of the Ru(0001) model catalyst under various reaction conditions, starting from a strongly oxidizing environment to reaction conditions typical for CO oxidation. With a mixture of O(2) and CO (stoichiometry, 2:1) the partial pressure of oxygen has to be increased to 20 mbar to form the catalytically active RuO(2)(110) oxide film, while in pure oxygen environment a pressure of 10(-5) mbar is already sufficient to oxidize the Ru(0001) surface. For preparation temperatures in the range of 550-630 K a self-limiting RuO(2)(110) film is produced with a thickness of 1.6 nm. The RuO(2)(110) film grows self-acceleratedly after an induction period. The RuO(2) films on Ru(0001) can readily be reduced by H(2) and CO exposures at 415 K, without an induction period. 相似文献
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Stierle A Kasper N Dosch H Lundgren E Gustafson J Mikkelsen A Andersen JN 《The Journal of chemical physics》2005,122(4):44706
The oxidation of Pd(100) and the formation of PdO was studied in situ using surface x-ray diffraction. A bulklike, epitaxial PdO film is formed at oxygen partial pressures beyond 1 mbar and sample temperatures exceeding 650 K. The main orientation is PdO(001)/Pd(001), based upon bulk reflections from the PdO film. By comparing with measurements from the Pd crystal truncation rods, we estimate an rms surface roughness of 6 A, in good agreement with previous high pressure scanning tunneling microscopy measurements. Finally, we observed the transformation from the (radical5 x radical5) surface oxide to PdO bulk oxide at 675 K and 50 mbar O(2) pressure. 相似文献
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Mikael Borg Catherine Stampfl Anders Mikkelsen Johan Gustafson Edvin Lundgren Matthias Scheffler Jesper N Andersen 《Chemphyschem》2005,6(9):1923-1928
The structural phases of Al(x)Na(1-x) surface alloys have been investigated theoretically and experimentally. We describe the system using a lattice-gas Hamiltonian, determined from density functional theory, together with Monte Carlo (MC) calculations. The obtained phase diagram reproduces the experiment on a quantitative level. From calculation of the (configurational) density of states by the recently introduced Wang-Landau MC algorithm, we derive thermodynamic quantities, such as the free energy and entropy, which are not directly accessible from conventional MC simulations. We accurately reproduce the stoichiometry, as well as the temperature at which an order-disorder phase transition occurs, and demonstrate the crucial role, and magnitude, of the configurational entropy. 相似文献
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Mark Stradiotto Prof. Dr. Kevin D. Hesp Rylan J. Lundgren 《Angewandte Chemie (International ed. in English)》2010,49(3):494-512
Zwitterionic platinum group metal complexes that feature formal charge separation between a cationic metal fragment and a negatively charged ancillary ligand combine the desirable reactivity profile of related cationic complexes with the broad solubility and solvent tolerance of neutral species. As such, zwitterionic complexes of this type have emerged as attractive candidates for a diversity of applications, most notably involving the breaking and/or forming of E? H and E? C σ bonds involving a main group element E. Important advances in ancillary ligand design are documented that have enabled the construction of platinum group metal zwitterions. Also summarized are the results of stoichiometric and catalytic investigations in which the reactivity of such zwitterions and their more traditionally employed cationic relatives in σ bond activation chemistry are compared and contrasted. 相似文献
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We have investigated the structure and morphology of the InAs(1 1 1)B surface using Low Energy Electron Diffraction (LEED), Scanning Tunneling Microscopy (STM) and Scanning Electron Microscopy (SEM). The surface was prepared by annealing in the presence of an arsenic or atomic hydrogen pressure. A (2 × 2) reconstruction that changes into a (1 × 1) unreconstructed surface after prolonged annealing was observed irrespective of preparation method, while the surface morphology was distinctly different in the two cases. Detailed atomic scale models are proposed to explain the behavior. Deposition of Au aerosol nanoparticles on the sample prior to annealing was found to have no effect on the surface reconstruction. The Au particles were found to sink into the surface. 相似文献
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Extensive new high-temperature, high-resolution FTIR emission spectroscopy measurements for the five common isotopomers of GeO are combined with previous diode laser and microwave measurements in combined isotopomer analyses. New Dunham expansion parameters and an accurate analytical potential energy function are determined for the ground X1Sigma+ state. Copyright 1999 Academic Press. 相似文献