On the origin of the stability of graphene oxide membranes in water

Che Ning Yeh; Kalyan Raidongia; Jiaojing Shao; Quan Hong Yang; Jiaxing Huang

doi:10.1038/nchem.2145

On the origin of the stability of graphene oxide membranes in water

Che Ning Yeh, Kalyan Raidongia, Jiaojing Shao, Quan Hong Yang, Jiaxing Huang^*

^*Corresponding author for this work

Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

876 Scopus citations

Abstract

Graphene oxide (GO) films are known to be highly stable in water and this property has made their use in membrane applications in solution possible. However, this state of affairs is somewhat counterintuitive because GO sheets become negatively charged on hydration and the membrane should disintegrate owing to electrostatic repulsion. We have now discovered a long-overlooked reason behind this apparent contradiction. Our findings show that neat GO membranes do, indeed, readily disintegrate in water, but the films become stable if they are crosslinked by multivalent cationic metal contaminants. Such metal contaminants can be introduced unintentionally during the synthesis and processing of GO, most notably on filtration with anodized aluminium oxide filter discs that corrode to release significant amounts of aluminium ions. This finding has wide implications in interpreting the processing-structure-property relationships of GO and other lamellar membranes. We also discuss strategies to avoid and mitigate metal contamination and demonstrate that this effect can be exploited to synthesize new membrane materials.

Original language	English (US)
Pages (from-to)	166-170
Number of pages	5
Journal	Nature chemistry
Volume	7
Issue number	2
DOIs	https://doi.org/10.1038/nchem.2145
State	Published - Jan 2015

Funding

This work was primarily funded by the National Science Foundation (DMR-CAREER 0955612) and the Office of Naval Research (ONRN000141310556). C-N.Y. acknowledges 3M for a graduate fellowship, and the International Institute for Nanotechnology at Northwestern University for a Ryan Fellowship. J.S. acknowledges the China Scholarship Council for an exchange student fellowship. J.H. acknowledges the John Simon Guggenheim Memorial Foundation for a Guggenheim Fellowship. Q-H.Y. thanks the National Basic Research Program of China (2014CB932403) and National Natural Science Foundation of China (No. 51372167) for support. The work made use of experimental facilities at the Quantitative Bioelemental Imaging Center (QBIC) supported by the National Aeronautics and Space Administration Ames Research Center (NNA06CB93G), the Northwestern University Atomic and Nanoscale Characterization Experimental Center (NUANCE, Keck-II) and the J.B. Cohen X-Ray Diffraction Facility supported by the National Science Foundation Materials Research Science and Engineering Centers program (DMR-1121262). We thank C. L. Brinson for letting us use her mechanical analyser.

ASJC Scopus subject areas

General Chemical Engineering
General Chemistry

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10.1038/nchem.2145

Cite this

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title = "On the origin of the stability of graphene oxide membranes in water",

abstract = "Graphene oxide (GO) films are known to be highly stable in water and this property has made their use in membrane applications in solution possible. However, this state of affairs is somewhat counterintuitive because GO sheets become negatively charged on hydration and the membrane should disintegrate owing to electrostatic repulsion. We have now discovered a long-overlooked reason behind this apparent contradiction. Our findings show that neat GO membranes do, indeed, readily disintegrate in water, but the films become stable if they are crosslinked by multivalent cationic metal contaminants. Such metal contaminants can be introduced unintentionally during the synthesis and processing of GO, most notably on filtration with anodized aluminium oxide filter discs that corrode to release significant amounts of aluminium ions. This finding has wide implications in interpreting the processing-structure-property relationships of GO and other lamellar membranes. We also discuss strategies to avoid and mitigate metal contamination and demonstrate that this effect can be exploited to synthesize new membrane materials.",

author = "Yeh, {Che Ning} and Kalyan Raidongia and Jiaojing Shao and Yang, {Quan Hong} and Jiaxing Huang",

note = "Funding Information: This work was primarily funded by the National Science Foundation (DMR-CAREER 0955612) and the Office of Naval Research (ONRN000141310556). C-N.Y. acknowledges 3M for a graduate fellowship, and the International Institute for Nanotechnology at Northwestern University for a Ryan Fellowship. J.S. acknowledges the China Scholarship Council for an exchange student fellowship. J.H. acknowledges the John Simon Guggenheim Memorial Foundation for a Guggenheim Fellowship. Q-H.Y. thanks the National Basic Research Program of China (2014CB932403) and National Natural Science Foundation of China (No. 51372167) for support. The work made use of experimental facilities at the Quantitative Bioelemental Imaging Center (QBIC) supported by the National Aeronautics and Space Administration Ames Research Center (NNA06CB93G), the Northwestern University Atomic and Nanoscale Characterization Experimental Center (NUANCE, Keck-II) and the J.B. Cohen X-Ray Diffraction Facility supported by the National Science Foundation Materials Research Science and Engineering Centers program (DMR-1121262). We thank C. L. Brinson for letting us use her mechanical analyser.",

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N2 - Graphene oxide (GO) films are known to be highly stable in water and this property has made their use in membrane applications in solution possible. However, this state of affairs is somewhat counterintuitive because GO sheets become negatively charged on hydration and the membrane should disintegrate owing to electrostatic repulsion. We have now discovered a long-overlooked reason behind this apparent contradiction. Our findings show that neat GO membranes do, indeed, readily disintegrate in water, but the films become stable if they are crosslinked by multivalent cationic metal contaminants. Such metal contaminants can be introduced unintentionally during the synthesis and processing of GO, most notably on filtration with anodized aluminium oxide filter discs that corrode to release significant amounts of aluminium ions. This finding has wide implications in interpreting the processing-structure-property relationships of GO and other lamellar membranes. We also discuss strategies to avoid and mitigate metal contamination and demonstrate that this effect can be exploited to synthesize new membrane materials.

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On the origin of the stability of graphene oxide membranes in water

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