High protonic resistance of hydrocarbon-based cathodes in PEM fuel cells under low humidity conditions: Origin, implication, and mitigation

Liepold, Hannes; Bird, Ashley; Heizmann, Philipp A.; Fadlullah, Hassan; Nguyen, Hien; Klose, Carolin; Holdcroft, Steven; Kusoglu, Ahmet; Vierrath, Severin; Münchinger, Andreas

doi:10.1016/j.jpowsour.2024.235537

Title: High protonic resistance of hydrocarbon-based cathodes in PEM fuel cells under low humidity conditions: Origin, implication, and mitigation

Journal Article · 30 September 2024 · Journal of Power Sources

DOI: https://doi.org/10.1016/j.jpowsour.2024.235537 · OSTI ID:2449631

^[1]; Bird, Ashley ^[2];

^[1]; Fadlullah, Hassan ^[3]; Nguyen, Hien ^[3]; Klose, Carolin ^[1];

^[4]; Kusoglu, Ahmet ^[2]; Vierrath, Severin ^[1];

^[5]

Univ. of Freiburg (Germany)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Hahn-Schickard, Freiburg (Germany)
Simon Fraser Univ., Burnaby, BC (Canada)
Univ. of Freiburg (Germany); Hahn-Schickard, Freiburg (Germany)

Hydrocarbon-based electrodes for proton-exchange membrane fuel cells face challenges in closing the performance gap with electrodes based on perfluorosulfonic acid ionomers, particularly under low humidity conditions. Alongside increased oxygen transport resistance and higher kinetic-induced overpotentials, the protonic resistance of these fluorine-free electrodes is the primary hurdle to improved performance. This study systematically investigates the origin and impact of the cathode protonic resistance on fuel cell performance, utilizing sulfonated phenylated polyphenylenes as hydrocarbon ionomers. Electrochemical characterization at low relative humidity (≤50 %) reveal a high protonic resistance arising from both lower conductivity of the hydrocarbon thin film compared to the bulk membrane and increased cathode tortuosity at a gas transport-optimized ionomer to carbon (I/C) ratio of 0.2. The poor protonic resistance at low relative humidities leads to a non-homogeneous current distribution across the thickness of the cathode electrode, resulting in lower catalyst utilization. To address this issue, reducing the thickness of the cathode CL while maintaining a constant Pt loading (i.e., increasing the Pt on carbon ratio) significantly reduces protonic resistance. This improvement compensates for the kinetic disadvantages of highly loaded carbon particles and results in a considerable performance increase by 40 % at 0.75 V under low relative humidities.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2449631

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 624; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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