Chemical and Physical Drivers for Improvement in Permeance and Stability of Linker-Free Graphene Oxide Membranes

Jatin J. Patil, Zhengmao Lu, Michael J. Zachman, Ningxin Chen, Kimberly S. Reeves, Asmita Jana, Griselda Revia, Brandon MacDonald, Brent D. Keller, Edgar Lara-Curzio, Jeffrey C. Grossman, Nicola Ferralis

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

Graphene oxide (GO) is a promising membrane material for chemical separations, including water treatment. However, GO has often required postsynthesis chemical modifications, such as linkers or intercalants, to improve either the permeability, performance, or mechanical integrity of GO membranes. In this work, we explore two different feedstocks of GO to investigate chemical and physical differences, where we observe up to a 100× discrepancy in the permeability-mass loading trade-off while maintaining nanofiltration capacity. GO membranes also show structural stability and chemical resilience to harsh pH conditions and bleach treatment. We probe GO and the resulting assembled membranes through a variety of characterization approaches, including a novel scanning-transmission-electron-microscopy-based visualization approach, to connect differences in sheet stacking and oxide functional groups to significant improvements in permeability and chemical stability.

Original languageEnglish
Pages (from-to)6414-6423
Number of pages10
JournalNano Letters
Volume23
Issue number14
DOIs
StatePublished - Jul 26 2023

Funding

We would like to acknowledge the United States Department of Energy, National Energy Technology Laboratory for providing the coal tar pitch samples and for useful discussions about this material. J.J.P. is supported by the Exponent Fellowship awarded through the MIT School of Engineering. N.C. is supported by the MIT Undergraduate Research Opportunities Program Office at MIT. This work made use of the MRSEC Shared Experimental Facilities at MIT, supported by the National Science Foundation under Award DMR-1419807. This work was carried out in part through the use of MIT.nano’s facilities. This work was performed in part at the Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF Award 1541959. CNS is part of Harvard University. The scanning transmission electron microscopy portion of this research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This project was funded by NETL, in part, through a site support contract. Neither the United States Government nor any agency thereof, nor any of their employees, nor the support contractor, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Activities at ORNL were supported under contract DE-AC05-00OR22725 with the US Department of Energy (DOE), through DOE’s Fossil Energy & Carbon Management Program’s CoalMat project. We would like to acknowledge the United States Department of Energy, National Energy Technology Laboratory for providing the coal tar pitch samples and for useful discussions about this material. J.J.P. is supported by the Exponent Fellowship awarded through the MIT School of Engineering. N.C. is supported by the MIT Undergraduate Research Opportunities Program Office at MIT. This work made use of the MRSEC Shared Experimental Facilities at MIT, supported by the National Science Foundation under Award DMR-1419807. This work was carried out in part through the use of MIT.nano’s facilities. This work was performed in part at the Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF Award 1541959. CNS is part of Harvard University. The scanning transmission electron microscopy portion of this research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This project was funded by NETL, in part, through a site support contract. Neither the United States Government nor any agency thereof, nor any of their employees, nor the support contractor, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Activities at ORNL were supported under contract DE-AC05–00OR22725 with the US Department of Energy (DOE), through DOE’s Fossil Energy & Carbon Management Program’s CoalMat project.

FundersFunder number
Center for Nanophase Materials Sciences
MIT Undergraduate Research Opportunities Program Office
National Science FoundationDMR-1419807, 1541959
U.S. Department of Energy
Office of Science
Oak Ridge National LaboratoryDE-AC05–00OR22725
Massachusetts Institute of Technology
Harvard University
National Energy Technology Laboratory
School of Engineering, Monash University Malaysia

    Keywords

    • Graphene oxide
    • chemical separations
    • filtration
    • membrane
    • stability
    • transmission electron microscopy

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