Gas and surface diffusion in modified γ-alumina systems

The transport of pure gases through a microporous membrane is described. The alumina-based membrane (pores 2.5-4 nm) is suitable for Knudsen diffusion separation. To improve the separation factor, interaction with and mobility on the pore wall of one of the gases of a mixture is necessary. To introduce surface diffusion of oxygen and hydrogen, a γ-alumina membrane was impregnated with silver. If temperature and atmosphere are controlled carefully, finely dispersed silver up to 17% by weight can be introduced. At higher loads and under oxidizing conditions, particle growth occurs. In adsorption experiments, little oxygen adsorption on the silver-modified γ-alumina could be detected. This is due to a decrease in accessible surface area of the silver because of particle growth of silver under oxygen. The mobility of hydrogen on the surface was tested by counterdiffusion experiments, of which the theory is given. Hydrogen shows a considerable mobility on the surface at 293 K. At low pressures the flux ratio of hydrogen to nitrogen improved from 3.8 to 8.8. Magnesia was introduced into the γ-alumina membrane to enhance the adsorption and mobility of CO2. It is known that 30% of the CO2 transport on non-modified γ-alumina is surface diffusion. The highest achievable magnesia load was 2.2% by weight. Introduction of magnesia into the γ-alumina surface gives more strong base sites and fewer weak base sites. This results in stronger bonding of CO2 on the surface, but the amount adsorbed is comparable with the amount of CO2 adsorbed on non-modified γ-alumina. The contribution of surface diffusion to the total transport decreases with the introduction of magnesia, as is shown by counterdiffusion. The more strongly bonded CO2 is less mobile, resulting in a smaller surface flux.

[1]  A. J. Burggraaf,et al.  The preparation and characterization of alumina membranes with ultrafine pores: 2. The formation of supported membranes , 1985 .

[2]  A. J. Burggraaf,et al.  The preparation and characterization of alumina membranes with ultra-fine pores: Part 3. The permeability for pure liquids , 1985 .

[3]  K. J. Sladek,et al.  Diffusion on Surfaces. II. Correlation of Diffusivities of Physically and Chemically Adsorbed Species , 1974 .

[4]  K. Haraya,et al.  Separation of H2-CO mixtures with porous glass membranes in the intermediate flow region , 1986 .

[5]  A. J. Burggraaf,et al.  Inorganic, Porous Membranes. Preparation, Structure and Potential Applications , 1984 .

[6]  H. Tamon,et al.  Surface flow phenomenon of adsorbed gases on activa ted alumina. , 1981 .

[7]  M. Hirata,et al.  Measurement and correlation of high pressure vapor-liquid equilibria for the systems ethylene-1-butene and ethylene-propylene. , 1981 .

[8]  J. Watanabé,et al.  COMBINED SURFACE AND GAS PHASE DIFFUSION THROUGH PLUGS OF POROUS ADSORBENT IN TRANSITION DIFFUSION REGION , 1981 .

[9]  A. J. Burggraaf,et al.  The preparation and characterization of alumina membranes with ultra-fine pores : Part 4. Ultrafiltration and hyperfiltration experiments , 1985 .

[10]  A. Khasin,et al.  Adsorption isotherm of oxygen on silver , 1981 .

[11]  K. Jurczyk,et al.  Acid-base properties of modified γ-alumina , 1987 .

[12]  R. D. Present,et al.  Separation of a Gas Mixture Flowing through a Long Tube at Low Pressure , 1949 .

[13]  K. Kammermeyer,et al.  Temperature—separation factor relationships in gaseous diffusion , 1969 .

[14]  A. Burggraaf,et al.  The preparation and characterization of alumina membranes with ultra-fine pores , 1984 .

[15]  K. J. Sladek,et al.  Diffusion on Surfaces. I. Effect of Concentration on the Diffusivity of Physically Adsorbed Gases , 1974 .

[16]  A. Burggraaf,et al.  Gas separation mechanisms in microporous modified γ-al2o3 membranes , 1988 .