Hydrophobic zeolite-silicone rubber mixed matrix membranes for ethanol-water separation: Effect of zeolite and silicone component selection on pervaporation performance

Abstract High-silica ZSM-5 zeolites were incorporated into poly(dimethyl siloxane) (PDMS) polymers to form mixed matrix membranes for ethanol removal from water via pervaporation. Membrane formulation and preparation parameters were varied to determine the effect on pervaporation performance including siloxane chain length, crosslinking agent concentration and density of reactive groups, catalyst level, solvent type, zeolite type and loading, mixing method, and presence of a porous support membrane. Uniform dispersion of zeolite was critical to the achievement of reproducible results and ultrasonication with a probe-type device was found to be effective at particle dispersal. Properties of the vinyl-terminated PDMS and methyl-hydride crosslinking agents in the polymer system had a limited effect on performance while zeolite loading had the greatest effect. The highest observed selectivity of 3.0 was observed with 65 wt% zeolite loading, the highest practicable loading for the polymer system studied. The current results are placed in the context of ZSM-5/PDMS mixed matrix membranes previously reported in the literature for ethanol–water separation.

[1]  J. Smith,et al.  Silicalite, a new hydrophobic crystalline silica molecular sieve , 1978, Nature.

[2]  Ivo F. J. Vankelecom,et al.  Incorporation of nano-sized zeolites in membranes , 2000 .

[3]  Shih‐Yuan Lu,et al.  Pervaporation of acetic acid/water mixtures through silicalite filled polydimethylsiloxane membranes , 2000 .

[4]  Ivo F J Vankelecom,et al.  Zeolite filled polydimethylsiloxane (PDMS) as an improved membrane for solvent-resistant nanofiltration (SRNF). , 2005, Chemical communications.

[5]  Xin Chen,et al.  Separation properties of alcohol–water mixture through silicalite‐I‐filled silicone rubber membranes by pervaporation , 1998 .

[6]  I. Vankelecom,et al.  Sorption and Pervaporation of Aroma Compounds Using Zeolite-Filled PDMS Membranes , 1997 .

[7]  R. Behling,et al.  Preparation and characterization of thin-film zeolite–PDMS composite membranes☆ , 1992 .

[8]  G. Trägårdh,et al.  Mass transport of aliphatic alcohols and esters through hydrophobic pervaporation membranes , 2006 .

[9]  C. A. Smolders,et al.  Zeolite-filled silicone rubber membranes : Part 1. Membrane preparation and pervaporation results , 1987 .

[10]  B. Adnadjevic,et al.  Effect of different physicochemical properties of hydrophobic zeolites on the pervaporation properties of PDMS-membranes , 1997 .

[11]  Ivo F. J. Vankelecom,et al.  Incorporation of Hydrophobic Porous Fillers in PDMS Membranes for Use in Pervaporation , 1997 .

[12]  J Huang,et al.  Pervaporative recovery of n-butanol from aqueous solutions and ABE fermentation broth using thin-film silicalite-filled silicone composite membranes , 2001 .

[13]  M. Galbe,et al.  A review of the production of ethanol from softwood , 2002, Applied Microbiology and Biotechnology.

[14]  Y. Idemoto,et al.  Stabilization of bioethanol recovery with silicone rubber‐coated ethanol‐permselective silicalite membranes by controlling the pH of acidic feed solution , 2005 .

[15]  V. G. Pangarkar,et al.  Recovery of Valuable Tea Aroma Components by Pervaporation , 2003 .

[16]  Leland M. Vane,et al.  A review of pervaporation for product recovery from biomass fermentation processes , 2005 .

[17]  Ivo F. J. Vankelecom,et al.  INFLUENCE OF ZEOLITES IN PDMS MEMBRANES - PERVAPORATION OF WATER/ALCOHOL MIXTURES , 1995 .

[18]  Ivo F. J. Vankelecom,et al.  Parameters Influencing Zeolite Incorporation in PDMS Membranes , 1994 .

[19]  Hiroshi Yanagishita,et al.  Drastic improvement of bioethanol recovery using a pervaporation separation technique employing a silicone rubber‐coated silicalite membrane , 2003 .

[20]  J. G. Wijmans Process performance = membrane properties + operating conditions , 2003 .

[21]  J. Olsson,et al.  The influence of permeant and membrane properties on mass transfer in pervaporation of volatile organic compounds from dilute aqueous solutions , 2002 .

[22]  Hiroshi Yanagishita,et al.  Concentration of fermented ethanol by pervaporation using silicalite membranes coated with silicone rubber , 2002 .

[23]  P. W. Madson,et al.  Recovery of volatile products from dilute high-fouling process streams , 2000 .

[24]  S. Hwang,et al.  Effects of concentration, temperature, and coupling on pervaporation of dilute flavor organics , 2006 .

[25]  R. Lichtenthaler,et al.  Sorption isotherms of alcohols in zeolite-filled silicone rubber and in PVA-composite membranes , 1992 .