SolidState Effects in Oxidation Catalysis在氧化催化固体状态的影响.pptVIP

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SolidState Effects in Oxidation Catalysis在氧化催化固体状态的影响.ppt

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SolidState Effects in Oxidation Catalysis在氧化催化固体状态的影响

Solid State Aspects of Oxidation Catalysis Paul J. Gellings and Henny J.M. Bouwmeester Contents of lecture Some concepts of solid state chemistry Methods of computational modelling Examples of applications of 1 and 2 to specific catalytic reactions Challenges for extension of use of solid state considerations to catalysis Possibilities for new applications: use of membranes Solid state concepts The solid state concepts considered are: atomic, ionic and electronic defects defect structure defect concentrations type of conduction conductivity crystal structure Defect notation Important types of defects Example of defect equilibrium Kr?ger-Vink or Brouwer diagram for ZrO2 Doping and defect equilibrium Computational modelling:defects Computational modelling:surfaces Defect energies near surface Vanadia: morphology Vanadia: ethene sorption Vanadia: quantum chemical cluster calculations Oxygen exchange Oxidation reactions Methane oxidation oxidative dimerization(oxidative coupling) oxidation to synthesis gas total combustion Other compounds saturated hydrocarbons olefins aromatic hydrocarbons nitrogen oxides Oxidative coupling of methane 1 Oxidative coupling of methane 2 Defect structure of Li-doped MgO 1 Defect structure of Li-doped MgO 2 Solution and oxidation energies Segregation energies Ammoxidation of propane and toluene Active site for selective ammoxidation Partial oxidation of iso-butane Membranes (micro)porous membranes:any oxidic material either intrinsically catalytically active or covered with active (mono)layer dense membranes:ionic or mixed ionic-electronic conductingmaterial Membrane reactors ABO3 perovskite structure Mixed oxygen/ionic conducting dense membrane Oxygen conducting membranes - I Oxygen conducting membranes - II Oxygen conducting membranes - III Proton conduction Predominance diagram for SrCe0.95Yb0.05O3-?Hx Methane coupling with proton conducting membrane Defect equilibria Further experiments Concluding remarks Solid electrolyte mem