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Title: The parameter space for scalable integration of atomically thin graphene with Nafion for proton exchange membrane (PEM) applications

Abstract

Selective proton permeation through atomically thin graphene while maintaining impermeability to even small gas atoms i.e. He or hydrated ions, presents potential for advancing proton exchange membranes (PEMs) across a range of energy conversion and storage applications. The incorporation of graphene into state-of-the-art proton conducting polymers e.g. Nafion can enable improvements in PEM selectivity as well as mitigate reactant crossover. The development of facile integration approaches are hence imperative. Here, we systematically study the parameters influencing the integration of monolayer graphene synthesized via scalable chemical vapor deposition (CVD) on polycrystalline Cu foils with a model proton conducting polymer (Nafion) via a facile hot-press process. The hot-press time (t), temperature (T) and pressure (P) are found to not only influence the quality of graphene transfer but can also introduce additional defects in the CVD graphene. Graphene transfers to Nafion performed below the optimum temperature (Topt ~ 115 °C) remain patchy with ruptures, while transfers above Topt showed defect features, and transfers near Topt show minimal ruptures and defect features. We demonstrate Nafion|graphene|Nafion sandwich membranes using the optimal transfer conditions that allow for ~50% reduction in hydrogen crossover (~0.17 mA cm–2) in comparison to Nafion control membranes (~0.33 mA cm–2) while maintainingmore » comparable proton area specific resistance < 0.25 Ω cm2 (areal conductance ~ 4–5 S cm–2), that are adequate to enable practical PEM applications such as fuel cells, redox flow batteries, and beyond.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [5]; ORCiD logo [6]
  1. Chemical and Biomolecular Engineering Department, Vanderbilt University, Nashville, TN, 37212, USA
  2. Chemical and Biomolecular Engineering Department, Vanderbilt University, Nashville, TN, 37212, USA, Interdisciplinary Graduate Program in Materials Science, Vanderbilt University, Nashville, TN, 37235, USA, Vanderbilt Institute of Nanoscale Science and Engineering, Nashville, TN, 37212, USA
  3. Department of Chemistry, Vanderbilt University, Nashville, TN, 37235, USA
  4. Interdisciplinary Graduate Program in Materials Science, Vanderbilt University, Nashville, TN, 37235, USA, Vanderbilt Institute of Nanoscale Science and Engineering, Nashville, TN, 37212, USA
  5. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, USA
  6. Chemical and Biomolecular Engineering Department, Vanderbilt University, Nashville, TN, 37212, USA, Interdisciplinary Graduate Program in Materials Science, Vanderbilt University, Nashville, TN, 37235, USA, Vanderbilt Institute of Nanoscale Science and Engineering, Nashville, TN, 37212, USA, Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, USA, Mechanical Engineering Department, Vanderbilt University, Nashville, TN, 37212, USA
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Vanderbilt Univ., Nashville, TN (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Office of Isotope R&D and Production (IRP); National Science Foundation (NSF)
OSTI Identifier:
1992378
Alternate Identifier(s):
OSTI ID: 1997611; OSTI ID: 2324831
Grant/Contract Number:  
SC0022237; AC05-00OR22725; 1944134; SC0022915
Resource Type:
Published Article
Journal Name:
Materials Advances
Additional Journal Information:
Journal Name: Materials Advances Journal Volume: 4 Journal Issue: 16; Journal ID: ISSN 2633-5409
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chaturvedi, Pavan, Moehring, Nicole K., Knight, Thomas, Shah, Rahul, Vlassiouk, Ivan, and Kidambi, Piran R. The parameter space for scalable integration of atomically thin graphene with Nafion for proton exchange membrane (PEM) applications. United Kingdom: N. p., 2023. Web. doi:10.1039/D3MA00180F.
Chaturvedi, Pavan, Moehring, Nicole K., Knight, Thomas, Shah, Rahul, Vlassiouk, Ivan, & Kidambi, Piran R. The parameter space for scalable integration of atomically thin graphene with Nafion for proton exchange membrane (PEM) applications. United Kingdom. https://doi.org/10.1039/D3MA00180F
Chaturvedi, Pavan, Moehring, Nicole K., Knight, Thomas, Shah, Rahul, Vlassiouk, Ivan, and Kidambi, Piran R. Mon . "The parameter space for scalable integration of atomically thin graphene with Nafion for proton exchange membrane (PEM) applications". United Kingdom. https://doi.org/10.1039/D3MA00180F.
@article{osti_1992378,
title = {The parameter space for scalable integration of atomically thin graphene with Nafion for proton exchange membrane (PEM) applications},
author = {Chaturvedi, Pavan and Moehring, Nicole K. and Knight, Thomas and Shah, Rahul and Vlassiouk, Ivan and Kidambi, Piran R.},
abstractNote = {Selective proton permeation through atomically thin graphene while maintaining impermeability to even small gas atoms i.e. He or hydrated ions, presents potential for advancing proton exchange membranes (PEMs) across a range of energy conversion and storage applications. The incorporation of graphene into state-of-the-art proton conducting polymers e.g. Nafion can enable improvements in PEM selectivity as well as mitigate reactant crossover. The development of facile integration approaches are hence imperative. Here, we systematically study the parameters influencing the integration of monolayer graphene synthesized via scalable chemical vapor deposition (CVD) on polycrystalline Cu foils with a model proton conducting polymer (Nafion) via a facile hot-press process. The hot-press time (t), temperature (T) and pressure (P) are found to not only influence the quality of graphene transfer but can also introduce additional defects in the CVD graphene. Graphene transfers to Nafion performed below the optimum temperature (Topt ~ 115 °C) remain patchy with ruptures, while transfers above Topt showed defect features, and transfers near Topt show minimal ruptures and defect features. We demonstrate Nafion|graphene|Nafion sandwich membranes using the optimal transfer conditions that allow for ~50% reduction in hydrogen crossover (~0.17 mA cm–2) in comparison to Nafion control membranes (~0.33 mA cm–2) while maintaining comparable proton area specific resistance < 0.25 Ω cm2 (areal conductance ~ 4–5 S cm–2), that are adequate to enable practical PEM applications such as fuel cells, redox flow batteries, and beyond.},
doi = {10.1039/D3MA00180F},
journal = {Materials Advances},
number = 16,
volume = 4,
place = {United Kingdom},
year = {Mon Aug 14 00:00:00 EDT 2023},
month = {Mon Aug 14 00:00:00 EDT 2023}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/D3MA00180F

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