Pervaporative recovery of n-butanol from aqueous solutions and ABE fermentation broth using thin-film silicalite-filled silicone composite membranes

Abstract The thin-film silicalite-filled silicone composite membranes were fabricated by incorporating ultrafine silicalite-1 particles, 0.1–0.2 μm, which were synthesized in our laboratory. The effects of membrane thickness and silicalite particle content on membrane properties were studied. It was found that with the increase of silicalite content in the top active layer, the selectivity for n -butanol and n -butanol flux increased, while the total flux decreased. When the silicalite-1 content was over 60%, the active layer appeared to have defects, aggregation of silicalite-1 particles, which effected the separation factor. By controlling the membrane thickness and silicalite-1 content, membranes with the total flux of 600–700 g/m 2  h ( n -butanol flux of 300 g/m 2  h) and selectivity of 90–100 at 70°C using 10 g/l of n -butanol as feed solution were obtained. The effects of operation temperature and feed solution concentration on membrane performances were studied. The structures of the silicalite-1 particles and the composite membranes were analyzed by SEM. Separation properties for acetone n -butanol ethanol (ABE) were also investigated by using model ABE solution and ABE fermentation broth.

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

[2]  F. Mizukami,et al.  Separation of ethanol/water mixture by silicalite membrane on pervaporation , 1994 .

[3]  L. Puigjaner,et al.  Study of butanol extraction through pervaporation in acetobutylic fermentation. , 1987, Biotechnology and bioengineering.

[4]  C. A. Smolders,et al.  EXCLUSION AND TORTUOSITY EFFECTS FOR ALCOHOL/WATER SEPARATION BY ZEOLITE-FILLED PDMS MEMBRANES , 1991 .

[5]  C. Slater,et al.  The Effect of Process Parameters on the Pervaporation of Alcohols through Organophilic Membranes , 1992 .

[6]  C. Stewart Slater,et al.  The Selective Recovery of Alcohols from Fermentation Broths by Pervaporation , 1990 .

[7]  A. Friedl,et al.  Long-Term Continuous Cultivation of Clostridium beijerinckii in a Two-Stage Chemostat with On-Line Solvent Removal , 1996, Applied and environmental microbiology.

[8]  I. Maddox,et al.  The acetone-butanol-ethanol fermentation: recent progress in technology. , 1989, Biotechnology & genetic engineering reviews.

[9]  W. M. Meier,et al.  Structure of synthetic zeolite ZSM-5 , 1978, Nature.

[10]  G. Eigenberger,et al.  Synthesis, characterization and transport properties of a new siloxane-phosphazene copolymer. Extraction of n-butanol from water by pervaporation , 1996 .

[11]  I. Maddox,et al.  The acetone-butanol-ethanol fermentation: a current assessment , 1986 .

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

[13]  N. Qureshi Recovery of alcohol fuels using selective membranes by pervaporation , 1997 .

[14]  Eric Favre,et al.  Extraction of 1-butanol from aqueous solutions by pervaporation , 1996 .

[15]  A. Friedl,et al.  Continuous acetone‐butanol‐ethanol (ABE) fermentation using immobilized cells of Clostridium acetobutylicum in a packed bed reactor and integration with product removal by pervaporation , 1991, Biotechnology and bioengineering.

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

[17]  H. Kataoka,et al.  Continuous butanol/isopropanol fermentation in down‐flow column reactor coupled with pervaporation using supported liquid membrane , 1992, Biotechnology and bioengineering.

[18]  Marcel Mulder,et al.  Basic Principles of Membrane Technology , 1991 .

[19]  Bruce Duffield,et al.  Pervaporation of Model Acetone-Butanol-Ethanol Fermentation Product Solutions Using Polytetrafluoroethylene Membranes , 1993 .

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

[21]  D. Roizard,et al.  Synthesis of novel block siloxane polymers for the removal of butanols from aqueous feed solutions , 1998 .

[22]  D. Bibby,et al.  Silicalite-2, a silica analogue of the aluminosilicate zeolite ZSM-11 , 1979, Nature.

[23]  S. Sikdar,et al.  Pervaporation Using Adsorbent-Filled Membranes , 1996 .

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

[25]  N. Qureshi,et al.  Recovery of butanol from model solutions and fermentation broth using a silicalite/silicone membrane , 1999 .

[26]  Anthony G. Fane,et al.  Filled and unfilled composite GFT PDMS membranes for the recovery of butanols from dilute aqueous solutions: influence of alcohol polarity , 1997 .

[27]  D. Olson,et al.  Chemical and physical properties of the ZSM-5 substitutional series , 1980 .

[28]  Q Geng,et al.  Pervaporative butanol fermentation by Clostridium acetobutylicum B18 , 1994, Biotechnology and bioengineering.

[29]  M. Matsumura,et al.  Separation of dilute aqueous butanol and acetone solutions by pervaporation through liquid membranes , 1987, Biotechnology and bioengineering.

[30]  C. A. Smolders,et al.  Zeolite-filled silicone rubber membranes Experimental determination of concentration profiles , 1994 .

[31]  Michael M. Meagher,et al.  Acetone butanol ethanol (ABE) recovery by pervaporation using silicalite–silicone composite membrane from fed-batch reactor of Clostridium acetobutylicum , 2001 .

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