Catalytic Reduction of Graphene Oxide Membranes and Water Selective Channel Formation in Water–Alcohol Separations
Abstract
Graphene oxide (GO) is a promising membrane system for chemical separation applications due to its 2-D nanofluidics properties and an ability to control interplanar spacing for selectivity. The permeance of water, methanol (MeOH) and isopropyl alcohol (IPA) through 5 µm thick membranes was found to be 0.38 ± 0.15, 0.33 ± 0.16 and 0.42 ± 0.31 LMH/bar (liter/m2·h·bar), respectively. Interestingly, the permeance of a water–alcohol mixture was found to be dramatically lower (~0.01 LMH/bar) than any of its components. Upon removing the solvent mixture, the transmembrane flux of the pure solvent was recovered to near the original permeance. The interlayer space of a dried GO membrane was found to be 8.52 Å, which increased to 12.19 Å. 13.26 Å and 16.20 Å upon addition of water, MeOH and IPA. A decrease in d-space, about 2 Å, was consistently observed when adding alcohol to water wetted GO membrane and an optical color change and reduction in permeance. A newly proposed mechanism of a partial reduction of GO through a catalytic reaction with the water–alcohol mixture is consistent with experimental observations.
- Authors:
-
[2];
- Univ. of Washington, Seattle, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
- OSTI Identifier:
- 1806194
- Report Number(s):
- PNNL-SA-157058
Journal ID: ISSN 2077-0375
- Grant/Contract Number:
- AC05-76RL01830; CBET-1460922
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Membranes
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 5; Journal ID: ISSN 2077-0375
- Publisher:
- MDPI
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalytic membranes; nanofluidics; biofuel separations
Citation Formats
Zang, Yushi, Peek, Alex, Shin, Yongsoon, Gotthold, David W., and Hinds, Bruce. Catalytic Reduction of Graphene Oxide Membranes and Water Selective Channel Formation in Water–Alcohol Separations. United States: N. p., 2021.
Web. doi:10.3390/membranes11050317.
Zang, Yushi, Peek, Alex, Shin, Yongsoon, Gotthold, David W., & Hinds, Bruce. Catalytic Reduction of Graphene Oxide Membranes and Water Selective Channel Formation in Water–Alcohol Separations. United States. https://doi.org/10.3390/membranes11050317
Zang, Yushi, Peek, Alex, Shin, Yongsoon, Gotthold, David W., and Hinds, Bruce. Mon .
"Catalytic Reduction of Graphene Oxide Membranes and Water Selective Channel Formation in Water–Alcohol Separations". United States. https://doi.org/10.3390/membranes11050317. https://www.osti.gov/servlets/purl/1806194.
@article{osti_1806194,
title = {Catalytic Reduction of Graphene Oxide Membranes and Water Selective Channel Formation in Water–Alcohol Separations},
author = {Zang, Yushi and Peek, Alex and Shin, Yongsoon and Gotthold, David W. and Hinds, Bruce},
abstractNote = {Graphene oxide (GO) is a promising membrane system for chemical separation applications due to its 2-D nanofluidics properties and an ability to control interplanar spacing for selectivity. The permeance of water, methanol (MeOH) and isopropyl alcohol (IPA) through 5 µm thick membranes was found to be 0.38 ± 0.15, 0.33 ± 0.16 and 0.42 ± 0.31 LMH/bar (liter/m2·h·bar), respectively. Interestingly, the permeance of a water–alcohol mixture was found to be dramatically lower (~0.01 LMH/bar) than any of its components. Upon removing the solvent mixture, the transmembrane flux of the pure solvent was recovered to near the original permeance. The interlayer space of a dried GO membrane was found to be 8.52 Å, which increased to 12.19 Å. 13.26 Å and 16.20 Å upon addition of water, MeOH and IPA. A decrease in d-space, about 2 Å, was consistently observed when adding alcohol to water wetted GO membrane and an optical color change and reduction in permeance. A newly proposed mechanism of a partial reduction of GO through a catalytic reaction with the water–alcohol mixture is consistent with experimental observations.},
doi = {10.3390/membranes11050317},
journal = {Membranes},
number = 5,
volume = 11,
place = {United States},
year = {Mon Apr 26 00:00:00 EDT 2021},
month = {Mon Apr 26 00:00:00 EDT 2021}
}
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Works referenced in this record:
Carbonyl Addition Reactions: Factors Affecting the Hydrate–Hemiacetal and Hemiacetal–Acetal Equilibrium Constants
journal, March 1975
- Guthrie, J. Peter
- Canadian Journal of Chemistry, Vol. 53, Issue 6
Insights on the mechanism of water-alcohol separation in multilayer graphene oxide membranes: Entropic versus enthalpic factors
journal, February 2018
- Damasceno Borges, Daiane; Woellner, Cristiano F.; Autreto, Pedro A. S.
- Carbon, Vol. 127
Enhanced flow in carbon nanotubes
journal, November 2005
- Majumder, Mainak; Chopra, Nitin; Andrews, Rodney
- Nature, Vol. 438, Issue 7064
Fast Mass Transport Through Sub-2-Nanometer Carbon Nanotubes
journal, May 2006
- Holt, J. K.
- Science, Vol. 312, Issue 5776
Large-area graphene-based nanofiltration membranes by shear alignment of discotic nematic liquid crystals of graphene oxide
journal, March 2016
- Akbari, Abozar; Sheath, Phillip; Martin, Samuel T.
- Nature Communications, Vol. 7, Issue 1
Slip length of water on graphene: Limitations of non-equilibrium molecular dynamics simulations
journal, January 2012
- Kumar Kannam, Sridhar; Todd, B. D.; Hansen, J. S.
- The Journal of Chemical Physics, Vol. 136, Issue 2
Direct observation of oxygen configuration on individual graphene oxide sheets
journal, February 2018
- Liu, Zilong; Nørgaard, Kasper; Overgaard, Marc H.
- Carbon, Vol. 127
The chemistry of graphene oxide
journal, January 2010
- Dreyer, Daniel R.; Park, Sungjin; Bielawski, Christopher W.
- Chem. Soc. Rev., Vol. 39, Issue 1
Molecular Dynamics Simulations Reveal that Water Diffusion between Graphene Oxide Layers is Slow
journal, July 2016
- Devanathan, Ram; Chase-Woods, Dylan; Shin, Yongsoon
- Scientific Reports, Vol. 6, Issue 1
Functionalized Graphene Sheets Embedded in Chitosan Nanocomposite Membranes for Ethanol and Isopropanol Dehydration via Pervaporation
journal, September 2014
- Dharupaneedi, Suhas P.; Anjanapura, Raghu V.; Han, Jeong M.
- Industrial & Engineering Chemistry Research, Vol. 53, Issue 37
Carbon-based building blocks for alcohol dehydration membranes with disorder-enhanced water permeability
journal, July 2017
- Boffa, V.; Etmimi, H.; Mallon, P. E.
- Carbon, Vol. 118
Programmable carbon nanotube membrane-based transdermal nicotine delivery with microdialysis validation assay
journal, January 2017
- Gulati, Gaurav Kumar; Chen, Tao; Hinds, Bruce Jackson
- Nanomedicine: Nanotechnology, Biology and Medicine, Vol. 13, Issue 1
Molecular transport through capillaries made with atomic-scale precision
journal, September 2016
- Radha, B.; Esfandiar, A.; Wang, F. C.
- Nature, Vol. 538, Issue 7624
Unimpeded Permeation of Water Through Helium-Leak-Tight Graphene-Based Membranes
journal, January 2012
- Nair, R. R.; Wu, H. A.; Jayaram, P. N.
- Science, Vol. 335, Issue 6067, p. 442-444
Water conduction through the hydrophobic channel of a carbon nanotube
journal, November 2001
- Hummer, G.; Rasaiah, J. C.; Noworyta, J. P.
- Nature, Vol. 414, Issue 6860
Graphene oxide as an acid catalyst for the room temperature ring opening of epoxides
journal, January 2012
- Dhakshinamoorthy, Amarajothi; Alvaro, Mercedes; Concepción, Patricia
- Chemical Communications, Vol. 48, Issue 44
Why Are Carbon Nanotubes Fast Transporters of Water?
journal, February 2008
- Joseph, Sony; Aluru, N. R.
- Nano Letters, Vol. 8, Issue 2
Highly Selective Supported Graphene Oxide Membranes for Water-Ethanol Separation
journal, February 2019
- Shin, Yongsoon; Taufique, Mohammad Fuad Nur; Devanathan, Ram
- Scientific Reports, Vol. 9, Issue 1
Solvent Transport Behavior of Shear Aligned Graphene Oxide Membranes and Implications in Organic Solvent Nanofiltration
journal, January 2018
- Akbari, Abozar; Meragawi, Sally E.; Martin, Samuel T.
- ACS Applied Materials & Interfaces, Vol. 10, Issue 2
A Nuclear Magnetic Resonance Study of the Reversible Hydration of Aliphatic Aldehydes and Ketones. I. Oxygen-17 and Proton Spectra and Equilibrium Constants
journal, February 1967
- Greenzaid, P.; Luz, Z.; Samuel, David.
- Journal of the American Chemical Society, Vol. 89, Issue 4
Enabling Graphene Oxide Nanosheets as Water Separation Membranes
journal, April 2013
- Hu, Meng; Mi, Baoxia
- Environmental Science & Technology, Vol. 47, Issue 8
Precise and Ultrafast Molecular Sieving Through Graphene Oxide Membranes
journal, February 2014
- Joshi, R. K.; Carbone, P.; Wang, F. C.
- Science, Vol. 343, Issue 6172
Understanding Water Permeation in Graphene Oxide Membranes
journal, April 2014
- Wei, Ning; Peng, Xinsheng; Xu, Zhiping
- ACS Applied Materials & Interfaces, Vol. 6, Issue 8
Carbon membranes for efficient water-ethanol separation
journal, September 2016
- Gravelle, Simon; Yoshida, Hiroaki; Joly, Laurent
- The Journal of Chemical Physics, Vol. 145, Issue 12
Impact of Carboxyl Groups in Graphene Oxide on Chemoselective Alcohol Oxidation with Ultra-Low Carbocatalyst Loading
journal, June 2017
- Cui, Yan; Lee, Young Hee; Yang, Jung Woon
- Scientific Reports, Vol. 7, Issue 1
Aldehyde functionalized graphene oxide frameworks as robust membrane materials for pervaporative alcohol dehydration
journal, April 2017
- Hua, Dan; Rai, Rajesh Kumar; Zhang, Yu
- Chemical Engineering Science, Vol. 161
Graphene oxide gas separation membranes intercalated by UiO-66-NH 2 with enhanced hydrogen separation performance
journal, October 2017
- Jia, Mingmin; Feng, Yi; Liu, Shichang
- Journal of Membrane Science, Vol. 539
Nitrogen-Doped Graphene as Efficient Metal-Free Electrocatalyst for Oxygen Reduction in Fuel Cells
journal, February 2010
- Qu, Liangti; Liu, Yong; Baek, Jong-Beom
- ACS Nano, Vol. 4, Issue 3, p. 1321-1326
Cross-Linking with Diamine Monomers To Prepare Composite Graphene Oxide-Framework Membranes with Varying d -Spacing
journal, April 2014
- Hung, Wei-Song; Tsou, Chi-Hui; De Guzman, Manuel
- Chemistry of Materials, Vol. 26, Issue 9
2D graphene oxide channel for water transport
journal, January 2018
- Mi, Baoxia; Zheng, Sunxiang; Tu, Qingsong
- Faraday Discussions, Vol. 209
Swelling of Graphene Oxide Membranes in Aqueous Solution: Characterization of Interlayer Spacing and Insight into Water Transport Mechanisms
journal, May 2017
- Zheng, Sunxiang; Tu, Qingsong; Urban, Jeffrey J.
- ACS Nano, Vol. 11, Issue 6
High-Flux Graphene Oxide Nanofiltration Membrane Intercalated by Carbon Nanotubes
journal, April 2015
- Han, Yi; Jiang, Yanqiu; Gao, Chao
- ACS Applied Materials & Interfaces, Vol. 7, Issue 15
Synthesis of graphene oxide membranes and their behavior in water and isopropanol
journal, May 2017
- Aher, Ashish; Cai, Yuguang; Majumder, Mainak
- Carbon, Vol. 116
A Graphene Oxide Membrane with Highly Selective Molecular Separation of Aqueous Organic Solution
journal, May 2014
- Huang, Kang; Liu, Gongping; Lou, Yueyun
- Angewandte Chemie International Edition, Vol. 53, Issue 27
A Highly Active, Readily Synthesized and Easily Separated Graphene Oxide (GO)/Polyethersulfone (PES) Catalytic Membrane for Biodiesel Production
journal, February 2020
- Tian, Fengyu; Xu, Baiqing; Li, Yingjie
- ChemistrySelect, Vol. 5, Issue 5
Ultrathin graphene-based membrane with precise molecular sieving and ultrafast solvent permeation
journal, November 2017
- Yang, Q.; Su, Y.; Chi, C.
- Nature Materials, Vol. 16, Issue 12
Metal-free graphene-based catalytic membrane for degradation of organic contaminants by persulfate activation
journal, August 2019
- Pedrosa, Marta; Drazic, Goran; Tavares, Pedro B.
- Chemical Engineering Journal, Vol. 369
Structure of mammalian endolysosomal TRPML1 channel in nanodiscs
journal, October 2017
- Chen, Qingfeng; She, Ji; Zeng, Weizhong
- Nature, Vol. 550, Issue 7676
Graphene oxide based membrane intercalated by nanoparticles for high performance nanofiltration application
journal, September 2018
- Chen, Long; Li, Na; Wen, Ziyan
- Chemical Engineering Journal, Vol. 347
Reduced Graphene Oxide Membranes for Ultrafast Organic Solvent Nanofiltration
journal, August 2016
- Huang, Liang; Chen, Ji; Gao, Tiantian
- Advanced Materials, Vol. 28, Issue 39
Mechanism of water transport in graphene oxide laminates
journal, January 2017
- Deng, Junjiao; You, Yi; Bustamante, Heriberto
- Chemical Science, Vol. 8, Issue 3
Selective Intercalation of Graphite Oxide by Methanol in Water/Methanol Mixtures
journal, January 2013
- You, Shujie; Yu, Junchun; Sundqvist, Bertil
- The Journal of Physical Chemistry C, Vol. 117, Issue 4
Free-standing graphene oxide thin films assembled by a pressurized ultrafiltration method for dehydration of ethanol
journal, May 2014
- Tang, Yu Pan; Paul, Donald R.; Chung, Tai Shung
- Journal of Membrane Science, Vol. 458
Square ice in graphene nanocapillaries
journal, March 2015
- Algara-Siller, G.; Lehtinen, O.; Wang, F. C.
- Nature, Vol. 519, Issue 7544
Effect of microstructure of graphene oxide fabricated through different self-assembly techniques on 1-butanol dehydration
journal, March 2015
- Tsou, Chi-Hui; An, Quan-Fu; Lo, Shen-Chuan
- Journal of Membrane Science, Vol. 477
Tunable sieving of ions using graphene oxide membranes
journal, April 2017
- Abraham, Jijo; Vasu, Kalangi S.; Williams, Christopher D.
- Nature Nanotechnology, Vol. 12, Issue 6
Pressure-assisted self-assembly technique for fabricating composite membranes consisting of highly ordered selective laminate layers of amphiphilic graphene oxide
journal, March 2014
- Hung, Wei-Song; An, Quan-Fu; De Guzman, Manuel
- Carbon, Vol. 68
Inside Cover: Graphene Oxide: A Convenient Carbocatalyst for Facilitating Oxidation and Hydration Reactions (Angew. Chem. Int. Ed. 38/2010)
journal, July 2010
- Dreyer, Daniel R.; Jia, Hong-Peng; Bielawski, Christopher W.
- Angewandte Chemie International Edition, Vol. 49, Issue 38