Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability

Zulfi Al Rasyid Gautama; Yasir Arafat Hutapea; Byungchan Hwang; Junko Matsuda; Albert Mufundirwa; Takeharu Sugiyama; Miho Ariyoshi; Shigenori Fujikawa; Stephen Matthew Lyth; Akari Hayashi; Kazunari Sasaki; Masamichi Nishihara

doi:10.1016/j.memsci.2022.120734

Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability

Zulfi Al Rasyid Gautama, Yasir Arafat Hutapea, Byungchan Hwang, Junko Matsuda, Albert Mufundirwa, Takeharu Sugiyama, Miho Ariyoshi, Shigenori Fujikawa, Stephen Matthew Lyth, Akari Hayashi, Kazunari Sasaki, Masamichi Nishihara^*

^*Corresponding author for this work

Chemical And Process Engineering

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Abstract

Decomposition of polymer electrolyte membranes (PEMs) by radical species is a significant issue related to the chemical durability of polymer electrolyte fuel cells (PEFCs). A major contributor to radical formation is the oxygen crossover through the membrane from cathode to anode. Therefore, suppression of oxygen diffusion through the PEM is predicted to effectively mitigate the chemical degradation via radical formation. To confirm this, a simple high oxygen barrier PEM is prepared by sandwiching a thin gas barrier interlayer in between two Nafion 211 membranes. The interlayer consists of poly (vinyl alcohol) (PVA) and poly (vinyl sulfonic acid) (PVS) with various molar ratio. The sandwich PEM can show 286 times lower oxygen permeability than Nafion 212 membrane, which corresponds to 1.7 times longer survival time than Nafion 212 in a chemically accelerated stress test for PEMs known as open circuit voltage (OCV) holding test. Furthermore, the SEM image of the sandwich PEM cross-section shows that the interlayer could survive the OCV holding test despite its lower resistance against radical attack. The results in this study indicate that the addition of high oxygen barrier interlayer can reduce radical formation in PEFC and improve chemical durability.

Original language	English
Article number	120734
Number of pages	23
Journal	Journal of Membrane Science
Volume	658
Early online date	19 Jun 2022
DOIs	https://doi.org/10.1016/j.memsci.2022.120734
Publication status	Published - 15 Sept 2022

Funding

Furthermore, the PVA/PVS interlayer undergoes severe decomposition after 333 h, supporting the drastic increase in cell resistance (Fig. 8 (d)). This may occur due to reasons such as radical attack to the interlayer, weakened Nafion-interlayer boundary (due to dissolution of PVA and PVS in water), or degradation near the Pt band.The authors gratefully acknowledge financial support by the research grant of the Toyota Mobility Foundation 2019 and “Center of Innovation Science and Technology based Radical Innovation and Entrepreneurship Program (COI Program), JST Japan. The SAXS experiments were performed at Kyushu University Beamline (SAGA-LS/BL06) with the proposals of No. 2020IIIK003 and 2021IK001. The authors gratefully acknowledge financial support by the research grant of the Toyota Mobility Foundation 2019 and “ Center of Innovation Science and Technology based Radical Innovation and Entrepreneurship Program (COI Program), JST Japan. The SAXS experiments were performed at Kyushu University Beamline (SAGA-LS/BL06) with the proposals of No. 2020IIIK003 and 2021IK001 .

Keywords

fuel cell
OCV holding test
oxygen permeability
polymer electrolyte membrane
polyvinyl alcohol

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10.1016/j.memsci.2022.120734

Gautama-etal-JMS-2022-Suppression-of-radical-attack-in-polymer-electrolyteAccepted author manuscript, 3.87 MBLicence: CC BY-NC-ND 4.0

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Gautama, Z. A. R., Hutapea, Y. A., Hwang, B., Matsuda, J., Mufundirwa, A., Sugiyama, T., Ariyoshi, M., Fujikawa, S., Lyth, S. M., Hayashi, A., Sasaki, K., & Nishihara, M. (2022). Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability. Journal of Membrane Science, 658, Article 120734. https://doi.org/10.1016/j.memsci.2022.120734

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title = "Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability",

abstract = "Decomposition of polymer electrolyte membranes (PEMs) by radical species is a significant issue related to the chemical durability of polymer electrolyte fuel cells (PEFCs). A major contributor to radical formation is the oxygen crossover through the membrane from cathode to anode. Therefore, suppression of oxygen diffusion through the PEM is predicted to effectively mitigate the chemical degradation via radical formation. To confirm this, a simple high oxygen barrier PEM is prepared by sandwiching a thin gas barrier interlayer in between two Nafion 211 membranes. The interlayer consists of poly (vinyl alcohol) (PVA) and poly (vinyl sulfonic acid) (PVS) with various molar ratio. The sandwich PEM can show 286 times lower oxygen permeability than Nafion 212 membrane, which corresponds to 1.7 times longer survival time than Nafion 212 in a chemically accelerated stress test for PEMs known as open circuit voltage (OCV) holding test. Furthermore, the SEM image of the sandwich PEM cross-section shows that the interlayer could survive the OCV holding test despite its lower resistance against radical attack. The results in this study indicate that the addition of high oxygen barrier interlayer can reduce radical formation in PEFC and improve chemical durability.",

keywords = "fuel cell, OCV holding test, oxygen permeability, polymer electrolyte membrane, polyvinyl alcohol",

author = "Gautama, {Zulfi Al Rasyid} and Hutapea, {Yasir Arafat} and Byungchan Hwang and Junko Matsuda and Albert Mufundirwa and Takeharu Sugiyama and Miho Ariyoshi and Shigenori Fujikawa and Lyth, {Stephen Matthew} and Akari Hayashi and Kazunari Sasaki and Masamichi Nishihara",

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Gautama, ZAR, Hutapea, YA, Hwang, B, Matsuda, J, Mufundirwa, A, Sugiyama, T, Ariyoshi, M, Fujikawa, S, Lyth, SM, Hayashi, A, Sasaki, K & Nishihara, M 2022, 'Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability', Journal of Membrane Science, vol. 658, 120734. https://doi.org/10.1016/j.memsci.2022.120734

TY - JOUR

T1 - Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability

AU - Gautama, Zulfi Al Rasyid

AU - Hutapea, Yasir Arafat

AU - Hwang, Byungchan

AU - Matsuda, Junko

AU - Mufundirwa, Albert

AU - Sugiyama, Takeharu

AU - Ariyoshi, Miho

AU - Fujikawa, Shigenori

AU - Lyth, Stephen Matthew

AU - Hayashi, Akari

AU - Sasaki, Kazunari

AU - Nishihara, Masamichi

PY - 2022/9/15

Y1 - 2022/9/15

N2 - Decomposition of polymer electrolyte membranes (PEMs) by radical species is a significant issue related to the chemical durability of polymer electrolyte fuel cells (PEFCs). A major contributor to radical formation is the oxygen crossover through the membrane from cathode to anode. Therefore, suppression of oxygen diffusion through the PEM is predicted to effectively mitigate the chemical degradation via radical formation. To confirm this, a simple high oxygen barrier PEM is prepared by sandwiching a thin gas barrier interlayer in between two Nafion 211 membranes. The interlayer consists of poly (vinyl alcohol) (PVA) and poly (vinyl sulfonic acid) (PVS) with various molar ratio. The sandwich PEM can show 286 times lower oxygen permeability than Nafion 212 membrane, which corresponds to 1.7 times longer survival time than Nafion 212 in a chemically accelerated stress test for PEMs known as open circuit voltage (OCV) holding test. Furthermore, the SEM image of the sandwich PEM cross-section shows that the interlayer could survive the OCV holding test despite its lower resistance against radical attack. The results in this study indicate that the addition of high oxygen barrier interlayer can reduce radical formation in PEFC and improve chemical durability.

AB - Decomposition of polymer electrolyte membranes (PEMs) by radical species is a significant issue related to the chemical durability of polymer electrolyte fuel cells (PEFCs). A major contributor to radical formation is the oxygen crossover through the membrane from cathode to anode. Therefore, suppression of oxygen diffusion through the PEM is predicted to effectively mitigate the chemical degradation via radical formation. To confirm this, a simple high oxygen barrier PEM is prepared by sandwiching a thin gas barrier interlayer in between two Nafion 211 membranes. The interlayer consists of poly (vinyl alcohol) (PVA) and poly (vinyl sulfonic acid) (PVS) with various molar ratio. The sandwich PEM can show 286 times lower oxygen permeability than Nafion 212 membrane, which corresponds to 1.7 times longer survival time than Nafion 212 in a chemically accelerated stress test for PEMs known as open circuit voltage (OCV) holding test. Furthermore, the SEM image of the sandwich PEM cross-section shows that the interlayer could survive the OCV holding test despite its lower resistance against radical attack. The results in this study indicate that the addition of high oxygen barrier interlayer can reduce radical formation in PEFC and improve chemical durability.

KW - fuel cell

KW - OCV holding test

KW - oxygen permeability

KW - polymer electrolyte membrane

KW - polyvinyl alcohol

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DO - 10.1016/j.memsci.2022.120734

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VL - 658

JO - Journal of Membrane Science

JF - Journal of Membrane Science

M1 - 120734

ER -

Suppression of radical attack in polymer electrolyte membranes using a vinyl polymer blend interlayer with low oxygen permeability

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