Highly Selective Supported Graphene Oxide Membranes for Water-Ethanol Separation

Shin, Yongsoon; Taufique, Mohammad Fuad Nur; Devanathan, Ram; Cutsforth, Erika C.; Lee, Jaewon; Liu, Wei; Fifield, Leonard S.; Gotthold, David W.

doi:10.1038/s41598-019-38485-y

Title: Highly Selective Supported Graphene Oxide Membranes for Water-Ethanol Separation

Journal Article · 18 February 2019 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-019-38485-y · OSTI ID:1507524

Shin, Yongsoon ^[1]; Taufique, Mohammad Fuad Nur ^[1];

^[1]; Cutsforth, Erika C. ^[1]; Lee, Jaewon ^[1]; Liu, Wei ^[1];

^[1];

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Polyethersulfone (PES)-supported graphene oxide (GO) membrane has been developed by a simple casting approach. This stable membrane is applied for ethanol/water separation at different temperatures. The 5.0 µm thick GO film coated on PES membrane showed a long-term stability over a testing period of one month and excellent water/ethanol selectivity at elevated temperatures. The water/ethanol selectivity is dependent on the ethanol weight percentage in the water/ethanol feed mixtures and the operating temperature. The water/ethanol selectivity was enhanced with an increase of ethanol weight percentage in water/ethanol mixtures and from below 100 at RT to close to 874 at 90 ºC for 90% ethanol/10% water mixture. Molecular simulations of water-ethanol mixtures in graphene bilayers that are considered to play a key role in transport revealed that molecular transport is negligible for layer spacing below 1 nm. The differences in the diffusion of ethanol and water in the bilayer are not consistent with the large selectivity value experimentally observed. The entry of water and ethanol into the interlayer space may be the crucial step controlling the selectivity.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1507524

Report Number(s):: PNNL-SA-130472

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 9; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (61)

Parameterization of OPLS-AA force field for the conformational analysis of macrocyclic polyketides Kahn, Kalju; Bruice, Thomas C. Journal of Computational Chemistry, Vol. 23, Issue 10 https://doi.org/10.1002/jcc.10051	journal	May 2002
Graphene oxide membrane for liquid phase organic molecular separation Liu, Renlong; Arabale, Girish; Kim, Jinseon Carbon, Vol. 77 https://doi.org/10.1016/j.carbon.2014.06.007	journal	October 2014
Graphene oxide membranes with high permeability and selectivity for dehumidification of air Shin, Yongsoon; Liu, Wei; Schwenzer, Birgit Carbon, Vol. 106 https://doi.org/10.1016/j.carbon.2016.05.023	journal	September 2016
Molecular dynamics simulation of ethanol/water mixtures for structure and diffusion properties Zhang, Cuijuan; Yang, Xiaoning Fluid Phase Equilibria, Vol. 231, Issue 1 https://doi.org/10.1016/j.fluid.2005.03.018	journal	April 2005
Engineering process and cost model for a conventional corn wet milling facility Ramirez, Edna C.; Johnston, David B.; McAloon, Andrew J. Industrial Crops and Products, Vol. 27, Issue 1 https://doi.org/10.1016/j.indcrop.2007.08.002	journal	January 2008
Thin porous metal sheet-supported NaA zeolite membrane for water/ethanol separation Zhang, Jian; Liu, Wei Journal of Membrane Science, Vol. 371, Issue 1-2 https://doi.org/10.1016/j.memsci.2011.01.032	journal	April 2011
Free-standing graphene oxide thin films assembled by a pressurized ultrafiltration method for dehydration of ethanol Tang, Yu Pan; Paul, Donald R.; Chung, Tai Shung Journal of Membrane Science, Vol. 458 https://doi.org/10.1016/j.memsci.2014.01.062	journal	May 2014
Physical Properties and Hydrogen-Bonding Network of Water–Ethanol Mixtures from Molecular Dynamics Simulations Ghoufi, A.; Artzner, F.; Malfreyt, P. The Journal of Physical Chemistry B, Vol. 120, Issue 4 https://doi.org/10.1021/acs.jpcb.5b11776	journal	January 2016
Molecular Dynamics Study of the Aggregation Process of Graphene Oxide in Water Tang, Huan; Liu, Dongmei; Zhao, Ying The Journal of Physical Chemistry C, Vol. 119, Issue 47 https://doi.org/10.1021/acs.jpcc.5b07345	journal	November 2015
Water Confined in Nanotubes and between Graphene Sheets: A First Principle Study Cicero, Giancarlo; Grossman, Jeffrey C.; Schwegler, Eric Journal of the American Chemical Society, Vol. 130, Issue 6 https://doi.org/10.1021/ja074418+	journal	January 2008
Non-Annealed Graphene Paper as a Binder-Free Anode for Lithium-Ion Batteries Abouimrane, Ali; Compton, Owen C.; Amine, Khalil The Journal of Physical Chemistry C, Vol. 114, Issue 29 https://doi.org/10.1021/jp103704y	journal	June 2010
Graphitic Carbon–Water Nonbonded Interaction Parameters Wu, Yanbin; Aluru, N. R. The Journal of Physical Chemistry B, Vol. 117, Issue 29 https://doi.org/10.1021/jp402051t	journal	July 2013
Calibration and Testing of a Water Model for Simulation of the Molecular Dynamics of Proteins and Nucleic Acids in Solution Levitt, Michael; Hirshberg, Miriam; Sharon, Ruth The Journal of Physical Chemistry B, Vol. 101, Issue 25 https://doi.org/10.1021/jp964020s	journal	June 1997
Super-stretchable Graphene Oxide Macroscopic Fibers with Outstanding Knotability Fabricated by Dry Film Scrolling Cruz-Silva, Rodolfo; Morelos-Gomez, Aaron; Kim, Hyung-ick ACS Nano, Vol. 8, Issue 6, p. 5959-5967 https://doi.org/10.1021/nn501098d	journal	May 2014
Water conduction through the hydrophobic channel of a carbon nanotube Hummer, G.; Rasaiah, J. C.; Noworyta, J. P. Nature, Vol. 414, Issue 6860 https://doi.org/10.1038/35102535	journal	November 2001
On the origin of the stability of graphene oxide membranes in water Yeh, Che-Ning; Raidongia, Kalyan; Shao, Jiaojing Nature Chemistry, Vol. 7, Issue 2 https://doi.org/10.1038/nchem.2145	journal	January 2015
Strain-induced room-temperature ferroelectricity in SrTiO3 membranes Xu, Ruijuan; Huang, Jiawei; Barnard, Edward S. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16912-3	journal	June 2020
Molecular Dynamics Simulations Reveal that Water Diffusion between Graphene Oxide Layers is Slow Devanathan, Ram; Chase-Woods, Dylan; Shin, Yongsoon Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep29484	journal	July 2016
Pressure and temperature dependence of self-diffusion in water Krynicki, Kazimierz; Green, Christopher D.; Sawyer, David W. Faraday Discussions of the Chemical Society, Vol. 66 https://doi.org/10.1039/dc9786600199	journal	January 1978
Interfacial slip friction at a fluid-solid cylindrical boundary Kannam, Sridhar Kumar; Todd, B. D.; Hansen, J. S. The Journal of Chemical Physics, Vol. 136, Issue 24 https://doi.org/10.1063/1.4730167	journal	June 2012
Effect of molecular shape and electrostatic interactions on the water layer around polar and apolar groups in solution Sidhu, K. S.; Goodfellow, J. M.; Turner, J. Z. The Journal of Chemical Physics, Vol. 110, Issue 16 https://doi.org/10.1063/1.478699	journal	April 1999
Molecular dynamics study on water self-diffusion in aqueous mixtures of methanol, ethylene glycol and glycerol: investigations from the point of view of hydrogen bonding Zhang, Ning; Li, Weizhong; Chen, Cong Molecular Physics, Vol. 111, Issue 7 https://doi.org/10.1080/00268976.2012.760050	journal	April 2013
Precise and Ultrafast Molecular Sieving Through Graphene Oxide Membranes Joshi, R. K.; Carbone, P.; Wang, F. C. Science, Vol. 343, Issue 6172 https://doi.org/10.1126/science.1245711	journal	February 2014
Selective Molecular Sieving through Porous Graphene Koenig, Steven P.; Wang, Luda; Pellegrino, John arXiv https://doi.org/10.48550/arxiv.1208.4135	text	January 2012
Tuneable Sieving of Ions Using Graphene Oxide Membranes Abraham, J.; Vasu, K. S.; Williams, C. D. arXiv https://doi.org/10.48550/arxiv.1701.05519	text	January 2017
Separation technologies for the recovery and dehydration of alcohols from fermentation broths Vane, Leland M. Biofuels, Bioproducts and Biorefining, Vol. 2, Issue 6 https://doi.org/10.1002/bbb.108	journal	November 2008
Parameterization of OPLS-AA force field for the conformational analysis of macrocyclic polyketides Kahn, Kalju; Bruice, Thomas C. Journal of Computational Chemistry, Vol. 23, Issue 10 https://doi.org/10.1002/jcc.10051	journal	May 2002
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Temperature and concentration polarization in membrane distillation of aqueous salt solutions Martı́nez-Dı́ez, L.; Vázquez-González, M. I. Journal of Membrane Science, Vol. 156, Issue 2 https://doi.org/10.1016/S0376-7388(98)00349-4	journal	April 1999
Graphene oxide membrane for liquid phase organic molecular separation Liu, Renlong; Arabale, Girish; Kim, Jinseon Carbon, Vol. 77 https://doi.org/10.1016/j.carbon.2014.06.007	journal	October 2014
Graphene oxide membranes with high permeability and selectivity for dehumidification of air Shin, Yongsoon; Liu, Wei; Schwenzer, Birgit Carbon, Vol. 106 https://doi.org/10.1016/j.carbon.2016.05.023	journal	September 2016
Molecular dynamics simulation of ethanol/water mixtures for structure and diffusion properties Zhang, Cuijuan; Yang, Xiaoning Fluid Phase Equilibria, Vol. 231, Issue 1 https://doi.org/10.1016/j.fluid.2005.03.018	journal	April 2005
Engineering process and cost model for a conventional corn wet milling facility Ramirez, Edna C.; Johnston, David B.; McAloon, Andrew J. Industrial Crops and Products, Vol. 27, Issue 1 https://doi.org/10.1016/j.indcrop.2007.08.002	journal	January 2008
Thin porous metal sheet-supported NaA zeolite membrane for water/ethanol separation Zhang, Jian; Liu, Wei Journal of Membrane Science, Vol. 371, Issue 1-2 https://doi.org/10.1016/j.memsci.2011.01.032	journal	April 2011
Free-standing graphene oxide thin films assembled by a pressurized ultrafiltration method for dehydration of ethanol Tang, Yu Pan; Paul, Donald R.; Chung, Tai Shung Journal of Membrane Science, Vol. 458 https://doi.org/10.1016/j.memsci.2014.01.062	journal	May 2014
Physical Properties and Hydrogen-Bonding Network of Water–Ethanol Mixtures from Molecular Dynamics Simulations Ghoufi, A.; Artzner, F.; Malfreyt, P. The Journal of Physical Chemistry B, Vol. 120, Issue 4 https://doi.org/10.1021/acs.jpcb.5b11776	journal	January 2016
Molecular Dynamics Study of the Aggregation Process of Graphene Oxide in Water Tang, Huan; Liu, Dongmei; Zhao, Ying The Journal of Physical Chemistry C, Vol. 119, Issue 47 https://doi.org/10.1021/acs.jpcc.5b07345	journal	November 2015
Swelling of Graphene Oxide Membranes in Aqueous Solution: Characterization of Interlayer Spacing and Insight into Water Transport Mechanisms Zheng, Sunxiang; Tu, Qingsong; Urban, Jeffrey J. ACS Nano, Vol. 11, Issue 6 https://doi.org/10.1021/acsnano.7b02999	journal	May 2017
Water Confined in Nanotubes and between Graphene Sheets: A First Principle Study Cicero, Giancarlo; Grossman, Jeffrey C.; Schwegler, Eric Journal of the American Chemical Society, Vol. 130, Issue 6 https://doi.org/10.1021/ja074418+	journal	January 2008
Non-Annealed Graphene Paper as a Binder-Free Anode for Lithium-Ion Batteries Abouimrane, Ali; Compton, Owen C.; Amine, Khalil The Journal of Physical Chemistry C, Vol. 114, Issue 29 https://doi.org/10.1021/jp103704y	journal	June 2010
Graphitic Carbon–Water Nonbonded Interaction Parameters Wu, Yanbin; Aluru, N. R. The Journal of Physical Chemistry B, Vol. 117, Issue 29 https://doi.org/10.1021/jp402051t	journal	July 2013
Calibration and Testing of a Water Model for Simulation of the Molecular Dynamics of Proteins and Nucleic Acids in Solution Levitt, Michael; Hirshberg, Miriam; Sharon, Ruth The Journal of Physical Chemistry B, Vol. 101, Issue 25 https://doi.org/10.1021/jp964020s	journal	June 1997
Super-stretchable Graphene Oxide Macroscopic Fibers with Outstanding Knotability Fabricated by Dry Film Scrolling Cruz-Silva, Rodolfo; Morelos-Gomez, Aaron; Kim, Hyung-ick ACS Nano, Vol. 8, Issue 6, p. 5959-5967 https://doi.org/10.1021/nn501098d	journal	May 2014
Graphene Oxide Papers Modified by Divalent Ions—Enhancing Mechanical Properties via Chemical Cross-Linking Park, Sungjin; Lee, Kyoung-Seok; Bozoklu, Gulay ACS Nano, Vol. 2, Issue 3 https://doi.org/10.1021/nn700349a	journal	March 2008
Water conduction through the hydrophobic channel of a carbon nanotube Hummer, G.; Rasaiah, J. C.; Noworyta, J. P. Nature, Vol. 414, Issue 6860 https://doi.org/10.1038/35102535	journal	November 2001
On the origin of the stability of graphene oxide membranes in water Yeh, Che-Ning; Raidongia, Kalyan; Shao, Jiaojing Nature Chemistry, Vol. 7, Issue 2 https://doi.org/10.1038/nchem.2145	journal	January 2015
Selective molecular sieving through porous graphene Koenig, Steven P.; Wang, Luda; Pellegrino, John Nature Nanotechnology, Vol. 7, Issue 11 https://doi.org/10.1038/nnano.2012.162	journal	October 2012
Tunable sieving of ions using graphene oxide membranes Abraham, Jijo; Vasu, Kalangi S.; Williams, Christopher D. Nature Nanotechnology, Vol. 12, Issue 6 https://doi.org/10.1038/nnano.2017.21	journal	April 2017
Energy penalty for excess baggage Devanathan, Ram Nature Nanotechnology, Vol. 12, Issue 6 https://doi.org/10.1038/nnano.2017.53	journal	April 2017
Molecular Dynamics Simulations Reveal that Water Diffusion between Graphene Oxide Layers is Slow Devanathan, Ram; Chase-Woods, Dylan; Shin, Yongsoon Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep29484	journal	July 2016
The chemistry of graphene oxide Dreyer, Daniel R.; Park, Sungjin; Bielawski, Christopher W. Chem. Soc. Rev., Vol. 39, Issue 1 https://doi.org/10.1039/B917103G	journal	January 2010
Pressure and temperature dependence of self-diffusion in water Krynicki, Kazimierz; Green, Christopher D.; Sawyer, David W. Faraday Discussions of the Chemical Society, Vol. 66 https://doi.org/10.1039/dc9786600199	journal	January 1978
Interfacial slip friction at a fluid-solid cylindrical boundary Kannam, Sridhar Kumar; Todd, B. D.; Hansen, J. S. The Journal of Chemical Physics, Vol. 136, Issue 24 https://doi.org/10.1063/1.4730167	journal	June 2012
Effect of molecular shape and electrostatic interactions on the water layer around polar and apolar groups in solution Sidhu, K. S.; Goodfellow, J. M.; Turner, J. Z. The Journal of Chemical Physics, Vol. 110, Issue 16 https://doi.org/10.1063/1.478699	journal	April 1999
Molecular dynamics study on water self-diffusion in aqueous mixtures of methanol, ethylene glycol and glycerol: investigations from the point of view of hydrogen bonding Zhang, Ning; Li, Weizhong; Chen, Cong Molecular Physics, Vol. 111, Issue 7 https://doi.org/10.1080/00268976.2012.760050	journal	April 2013
Unimpeded Permeation of Water Through Helium-Leak-Tight Graphene-Based Membranes Nair, R. R.; Wu, H. A.; Jayaram, P. N. Science, Vol. 335, Issue 6067, p. 442-444 https://doi.org/10.1126/science.1211694	journal	January 2012
Precise and Ultrafast Molecular Sieving Through Graphene Oxide Membranes Joshi, R. K.; Carbone, P.; Wang, F. C. Science, Vol. 343, Issue 6172 https://doi.org/10.1126/science.1245711	journal	February 2014
Unimpeded permeation of water through helium-leak-tight graphene-based membranes Nair, R. R.; Wu, H. A.; Jayaram, P. N. arXiv https://doi.org/10.48550/arxiv.1112.3488	text	January 2011
Selective Molecular Sieving through Porous Graphene Koenig, Steven P.; Wang, Luda; Pellegrino, John arXiv https://doi.org/10.48550/arxiv.1208.4135	text	January 2012
Precise and ultrafast molecular sieving through graphene oxide membranes Joshi, R. K.; Carbone, P.; Wang, F. C. arXiv https://doi.org/10.48550/arxiv.1401.3134	text	January 2014
Tuneable Sieving of Ions Using Graphene Oxide Membranes Abraham, J.; Vasu, K. S.; Williams, C. D. arXiv https://doi.org/10.48550/arxiv.1701.05519	text	January 2017

Cited By (1)

Exfoliation and stabilization mechanism of graphene in carbon dioxide expanded organic solvents: molecular dynamics simulations Cai, Lu; Hou, Sensheng; Wei, Xiangyu Physical Chemistry Chemical Physics, Vol. 22, Issue 4 https://doi.org/10.1039/c9cp05924e	journal	January 2020

Similar Records

Catalytic Reduction of Graphene Oxide Membranes and Water Selective Channel Formation in Water–Alcohol Separations

Journal Article · 2021 · Membranes · OSTI ID:1806194

Zang, Yushi; Peek, Alex; Shin, Yongsoon; +2 more

Correlating Interlayer Spacing and Separation Capability of Graphene Oxide Membranes in Organic Solvents

Journal Article · 2020 · ACS Nano · OSTI ID:1619183

Zheng, Sunxiang; Tu, Qingsong; Wang, Monong; +2 more

Molecular dynamics simulations reveal that water diffusion between graphene oxide layers is slow

Journal Article · 2016 · Scientific Reports · OSTI ID:1290377

Devanathan, Ram; Chase-Woods, Dylan; Shin, Yongsoon; +1 more

Related Subjects

36 MATERIALS SCIENCE
ethanol-water separation
graphene oxide
membrane

Title: Highly Selective Supported Graphene Oxide Membranes for Water-Ethanol Separation

Citation Formats

References (61)

Cited By (1)

Similar Records

Related Subjects