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Title: Superhydrophobic or Hydrophilic Porous Metallic/Ceramic Tubular Membranes for Continuous Separations of Biodiesel–Water W/O and O/W Emulsions

Abstract

This study reports the effective surface effect of porous inorganic membranes on improving the emulsion separations (i.e., perm-selective extraction of either oil phase or aqueous phase from the emulsions). A novel tubular form of superwetting, porous, stainless steel/ceramic membranes were demonstrated for enabling continuous separations of oil–water emulsions, extracting either oil phase or aqueous phase from the flowing emulsions. The superhydrophobic membranes consist of macroporous (4 μm) stainless-steel SS434 tube with inner wall surface modified with superhydrophobicity (>150° contact angle) via perfluoro-silane grafting functionalization. The (super)hydrophilic membranes consist of 4-μm porous stainless-steel SS434 tube without/with inner wall coated with nanoporous alumina (6 nm average pore size), the surface of which was further modified with superhydrophilicity via Hydrophil-S solution deposition. With the cross-flow membrane filtration setup, the surface-engineered tubular membranes were studied for perm-selective extraction of aqueous or oil phase from oil–water emulsions (water-in-oil W/O and oil-in-water O/W) that are relevant to a real industrial biodiesel (FAME) production process. The superhydrophobic membrane (4 μm pore size) has demonstrated capability of extracting nearly 100% pure oil while rejecting water phase when either W/O or O/W emulsions were tested as feed. The superhydrophobic membrane showed distinct advantage of 2-orders-of-magnitude-higher flux extraction of oilmore » at 100 times higher “break-through” pressures. On the other hand, the super/hydrophilic nanoporous membranes (6 nm) have shown selective water permeation (separation factor up to 35) when biodiesel-relevant W/O emulsions were tested. Finally, the membrane function is discussed from the perspective of improving industrial biodiesel processing yield by overcoming equilibrium limitations during the biodiesel formation reactions. Future work on in situ reaction–separation experiments are envisioned.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Prenexus Health, Inc., Gilbert, AZ (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1509559
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 58; Journal Issue: 2; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hu, Michael Z., Bischoff, Brian L., Morales-Rodriguez, Marissa E., Gray, Kevin A., and Davison, Brian H.. Superhydrophobic or Hydrophilic Porous Metallic/Ceramic Tubular Membranes for Continuous Separations of Biodiesel–Water W/O and O/W Emulsions. United States: N. p., 2019. Web. doi:10.1021/acs.iecr.8b04888.
Hu, Michael Z., Bischoff, Brian L., Morales-Rodriguez, Marissa E., Gray, Kevin A., & Davison, Brian H.. Superhydrophobic or Hydrophilic Porous Metallic/Ceramic Tubular Membranes for Continuous Separations of Biodiesel–Water W/O and O/W Emulsions. United States. https://doi.org/10.1021/acs.iecr.8b04888
Hu, Michael Z., Bischoff, Brian L., Morales-Rodriguez, Marissa E., Gray, Kevin A., and Davison, Brian H.. 2019. "Superhydrophobic or Hydrophilic Porous Metallic/Ceramic Tubular Membranes for Continuous Separations of Biodiesel–Water W/O and O/W Emulsions". United States. https://doi.org/10.1021/acs.iecr.8b04888. https://www.osti.gov/servlets/purl/1509559.
@article{osti_1509559,
title = {Superhydrophobic or Hydrophilic Porous Metallic/Ceramic Tubular Membranes for Continuous Separations of Biodiesel–Water W/O and O/W Emulsions},
author = {Hu, Michael Z. and Bischoff, Brian L. and Morales-Rodriguez, Marissa E. and Gray, Kevin A. and Davison, Brian H.},
abstractNote = {This study reports the effective surface effect of porous inorganic membranes on improving the emulsion separations (i.e., perm-selective extraction of either oil phase or aqueous phase from the emulsions). A novel tubular form of superwetting, porous, stainless steel/ceramic membranes were demonstrated for enabling continuous separations of oil–water emulsions, extracting either oil phase or aqueous phase from the flowing emulsions. The superhydrophobic membranes consist of macroporous (4 μm) stainless-steel SS434 tube with inner wall surface modified with superhydrophobicity (>150° contact angle) via perfluoro-silane grafting functionalization. The (super)hydrophilic membranes consist of 4-μm porous stainless-steel SS434 tube without/with inner wall coated with nanoporous alumina (6 nm average pore size), the surface of which was further modified with superhydrophilicity via Hydrophil-S solution deposition. With the cross-flow membrane filtration setup, the surface-engineered tubular membranes were studied for perm-selective extraction of aqueous or oil phase from oil–water emulsions (water-in-oil W/O and oil-in-water O/W) that are relevant to a real industrial biodiesel (FAME) production process. The superhydrophobic membrane (4 μm pore size) has demonstrated capability of extracting nearly 100% pure oil while rejecting water phase when either W/O or O/W emulsions were tested as feed. The superhydrophobic membrane showed distinct advantage of 2-orders-of-magnitude-higher flux extraction of oil at 100 times higher “break-through” pressures. On the other hand, the super/hydrophilic nanoporous membranes (6 nm) have shown selective water permeation (separation factor up to 35) when biodiesel-relevant W/O emulsions were tested. Finally, the membrane function is discussed from the perspective of improving industrial biodiesel processing yield by overcoming equilibrium limitations during the biodiesel formation reactions. Future work on in situ reaction–separation experiments are envisioned.},
doi = {10.1021/acs.iecr.8b04888},
url = {https://www.osti.gov/biblio/1509559}, journal = {Industrial and Engineering Chemistry Research},
issn = {0888-5885},
number = 2,
volume = 58,
place = {United States},
year = {2019},
month = {1}
}

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Works referenced in this record:

Glycerol removal from biodiesel using membrane separation technology
journal, September 2010


Separation of biodiesel and glycerol using ceramic membranes
journal, April 2010


Separation of water droplets from water-in-diesel dispersion using superhydrophobic polypropylene fibrous membranes
journal, April 2014


Superhydrophobic and superhydrophilic surface-enhanced separation performance of porous inorganic membranes for biomass-to-biofuel conversion applications
journal, October 2016


Rational design of materials interface at nanoscale towards intelligent oil–water separation
journal, January 2018


Characterization of fouling processes in ceramic membranes used for the recovery and recycle of oil sands produced water
journal, October 2017


Preparation and characterization of tubular ceramic membranes for treatment of oil emulsions
journal, July 2005


Membrane technology enhancement in oil–water separation. A review
journal, February 2015


Cross-Flow Microfiltration of Oily Water using a Ceramic Membrane: Flux Decline and Oil Adsorption
journal, October 2009


Separation of glycerol from FAME using ceramic membranes
journal, July 2011


Works referencing / citing this record: