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Research Subject 1

Research Subject 1. Development of New Inorganic Membranes. Membranes. – Ceramic membranes for H 2 separation – Ceramic membranes for CO 2 separation – Studies address mechanism of permeation. Prediction of permeation properties. Dense alumina tubing. Porous support. 1 cm.

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Research Subject 1

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  1. Research Subject 1 Development of New Inorganic Membranes • Membranes – Ceramic membranes for H2 separation – Ceramic membranes for CO2 separation – Studies address mechanism of permeation • Prediction of permeation properties

  2. Dense alumina tubing Porous support 1 cm Connected by glass joints New Silica Membranes Si(C2H5O)4 (TEOS) Thermal CVD(873 K) SiO2 membrane (Nanosil) Alumina support(Pall Corporation, pore size 100 nm)

  3. Experimental Equipment for CVD CVD condition : 873 K, 1 atm(0.07 mol % of TEOS) Vent Vent Furnace Temperature Controller Membrane MFC Mass Flow Controller Heating Tape MFC ATSB Balance Gas MFC Oil Bath MFC Oxygen & WaterTrap Carrier Gas TEOS Dilution Gas Water Bath 4 cm

  4. Incomplete coverage Cracking Infiltration Large spaces Larger sol particles Smaller sol particles Approach for a Thin, Defect-free Intermediate Layer Graded layers

  5. Aluminum alkoxide Water Stirring & heating Hydrolysis Acid Peptization Refluxing Calcination Clear Boehmite Sol -Al2O3 Layers Sol Processing & Particle Size Distributions of Sols H+/Al alkoxide Al(OR)3 + H2O Al(OH)3 -(O-Al-O-Al)x AlOOH colloidal particles • Lower acidity produces larger particle sizes

  6. SiO layer 2 High resolution (L = 20 nm) g layer - O Al 2 3 100 nm Scanning Electron Microscopy Silica layer 1000 nm Graded substrate Support

  7. Three-layer membrane Two-layer membrane Permeability and Selectivity ofNanosil Membranes S > 99.9% P = 5 x 10-7 Y. Gu, S. T. Oyama, J. Membr. Sci.2007, 306, 216.

  8. Comparison to Palladium PdMembranes

  9. * = vibrational frequency Δ Ek d = jump distance Permeation equation: S. T. Oyama , D. Lee, P. Hacarlioglu, R. F. Saraf, J. Membr. Sci., 2004, 244, 45.Y. Gu, S. T. Oyama, Adv. Mater.2007, 19, 1636 Statistical Model Permeation occurs by jumps between adjacent solubility sites Key parameters: Ns = number of solubility sites Membrane Membrane P Translation Rotation Vibration

  10. Structure of Pd-Cu Membrane (5 nm) Pd-Cu Intermediate layer Low resolution (20 k X) High resolution (100 k X) Electroless plating of Pd-Cu Dip coating of one intermediate layer - alumina support (5 nm pore)

  11. Diffusion Energy Saddle Point Diffusion Energy Calculation Model: Becke3lyp (DFT) Basis set: 6-311G(2d,p) x z y Normal to the xy plane

  12. Glasses Silica layer Activation Energy vs. Distance to O atoms 4-membered 5-membered 6-membered 7-membered 8-membered Helium Hydrogen P. Hacarlioglu, D. Lee, G.V. Gibbs and S.T. Oyama, J. Membr. Sci. 2008,313, 278-283 .

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