skip to main content


Title: Single‐Step Scalable Fabrication of Zeolite MFI Hollow Fiber Membranes for Hydrocarbon Separations
Abstract

Despite the high potential of zeolite MFI membranes for the separation of important hydrocarbons, their impact on industrial hydrocarbon separations has been limited by challenges in scalable fabrication methods and use of high‐cost membrane supports. Here a one‐step method for fabrication of highly selective and thin (<1 µm) MFI zeolite membranes on low‐cost α‐alumina hollow fiber supports is demonstrated. This is enabled by use of a highly concentrated silicate precursor gel containing MFI nanocrystals that induces a compact membrane layer at the support surface in a single‐step membrane synthesis. These one‐step crystallized MFI hollow fiber membranes show excellent characteristics for butane isomer separation (n‐butane permeance > 10−7mol m−2s−1Pa−1andn‐butane/i‐butane separation factors > 50 ), as well as for removal of natural gas liquids (butane, propane, and ethane) from methane at elevated feed pressures up to 9 bar. It is further demonstrated that the scalability of the current strategy by successful fabrication of a high‐quality ten‐membrane module in a single synthesis batch.

 
more » « less
NSF-PAR ID:
10378953
Author(s) / Creator(s):
 ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Materials Interfaces
Volume:
7
Issue:
19
ISSN:
2196-7350
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    High‐quality 2D MFI nanosheet coatings were prepared on α‐alumina hollow fiber supports by vacuum filtration and then transformed into molecular sieving membranes by two sequential hydrothermal treatments. This processing method eliminates the need for specially engineered silica‐based support materials that have so far been necessary to allow the formation of functional membranes from 2D MFI nanosheets. The sequential steps enhance adhesion of the membrane on the fiber support, fill in nanoscale gaps between the 2D nanosheets, and preserve the desirable (0k0) out‐of‐plane orientation without the need of any support engineering or modification. The membrane exhibits high performance for separation ofn‐butane fromi‐butane, and for other technologically important hydrocarbon separations. The present findings have strong implications on strategies for obtaining thin, highly selective zeolite membranes from 2D zeolites in a technologically scalable manner.

     
    more » « less
  2. Abstract

    High‐quality 2D MFI nanosheet coatings were prepared on α‐alumina hollow fiber supports by vacuum filtration and then transformed into molecular sieving membranes by two sequential hydrothermal treatments. This processing method eliminates the need for specially engineered silica‐based support materials that have so far been necessary to allow the formation of functional membranes from 2D MFI nanosheets. The sequential steps enhance adhesion of the membrane on the fiber support, fill in nanoscale gaps between the 2D nanosheets, and preserve the desirable (0k0) out‐of‐plane orientation without the need of any support engineering or modification. The membrane exhibits high performance for separation ofn‐butane fromi‐butane, and for other technologically important hydrocarbon separations. The present findings have strong implications on strategies for obtaining thin, highly selective zeolite membranes from 2D zeolites in a technologically scalable manner.

     
    more » « less
  3. Abstract

    Separation of higher hydrocarbons from methane is an important and energy‐intensive operation in natural gas processing. We present a detailed investigation of thin and oriented MFI zeolite membranes fabricated from 2D MFI nanosheets on inexpensive α‐alumina hollow fiber supports, particularly for separation ofn‐butane, propane, and ethane (“natural gas liquids”) from methane. These membranes display high permeances and selectivities for C2–C4hydrocarbons over methane, driven primarily by stronger adsorption of C2–C4hydrocarbons. We study the separation characteristics under unary, binary, ternary, and quaternary mixture conditions at 298 K and 100–900 kPa feed pressures. The membranes are highly effective in quaternary mixture separation at elevated feed pressures, for example allowingn‐butane/methane separation factors of 170–280 andn‐butane permeances of 710–2,700 GPU over the feed pressure range. We parametrize and apply multicomponent Maxwell–Stefan transport equations to predict the main trends in separation behavior over a range of operating conditions.

     
    more » « less
  4. Abstract

    Zeolite membranes show great potential for gas and hydrocarbon separations, but high manufacturing cost has been one of the main hurdles in their industrial application. Here we demonstrate a method termed viscosity‐confined dry gel conversion (VCDGC) for zeolite hollow fiber membrane fabrication. We demonstrate in detail the VCDGC synthesis of small‐pore CHA zeolite membranes. Extensive permeation measurements reveal that dry gel‐processed CHA zeolite hollow fiber membranes have excellent gas and hydrocarbon separation characteristics well exceeding or comparable to current membranes. Medium‐pore MFI membranes are also fabricated, and their favorable hydrocarbon separation characteristics indicate the versatility and reliability of the VCDGC method.

     
    more » « less
  5. Abstract

    Zeolite membranes show great potential for gas and hydrocarbon separations, but high manufacturing cost has been one of the main hurdles in their industrial application. Here we demonstrate a method termed viscosity‐confined dry gel conversion (VCDGC) for zeolite hollow fiber membrane fabrication. We demonstrate in detail the VCDGC synthesis of small‐pore CHA zeolite membranes. Extensive permeation measurements reveal that dry gel‐processed CHA zeolite hollow fiber membranes have excellent gas and hydrocarbon separation characteristics well exceeding or comparable to current membranes. Medium‐pore MFI membranes are also fabricated, and their favorable hydrocarbon separation characteristics indicate the versatility and reliability of the VCDGC method.

     
    more » « less