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Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode

Author

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  • Hernan Sanchez Casalongue

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Joint Center for Artificial Photosynthesis (JCAP) Energy Innovation Hub, LBNL)

  • Sarp Kaya

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Joint Center for Artificial Photosynthesis (JCAP) Energy Innovation Hub, LBNL)

  • Venkatasubramanian Viswanathan

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    SUNCAT Center for Interface Science and Catalysis, Stanford University)

  • Daniel J. Miller

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory)

  • Daniel Friebel

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Joint Center for Artificial Photosynthesis (JCAP) Energy Innovation Hub, LBNL)

  • Heine A. Hansen

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    SUNCAT Center for Interface Science and Catalysis, Stanford University)

  • Jens K. Nørskov

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    SUNCAT Center for Interface Science and Catalysis, Stanford University)

  • Anders Nilsson

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Joint Center for Artificial Photosynthesis (JCAP) Energy Innovation Hub, LBNL
    Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory)

  • Hirohito Ogasawara

    (SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
    Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory)

Abstract

The performance of polymer electrolyte membrane fuel cells is limited by the reduction at the cathode of various oxygenated intermediates in the four-electron pathway of the oxygen reduction reaction. Here we use ambient pressure X-ray photoelectron spectroscopy, and directly probe the correlation between the adsorbed species on the surface and the electrochemical potential. We demonstrate that, during the oxygen reduction reaction, hydroxyl intermediates on the cathode surface occur in several configurations with significantly different structures and reactivities. In particular, we find that near the open-circuit potential, non-hydrated hydroxyl is the dominant surface species. On the basis of density functional theory calculations, we show that the removal of hydration enhances the reactivity of oxygen species. Tuning the hydration of hydroxyl near the triple phase boundary will be crucial for designing more active fuel cell cathodes.

Suggested Citation

  • Hernan Sanchez Casalongue & Sarp Kaya & Venkatasubramanian Viswanathan & Daniel J. Miller & Daniel Friebel & Heine A. Hansen & Jens K. Nørskov & Anders Nilsson & Hirohito Ogasawara, 2013. "Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode," Nature Communications, Nature, vol. 4(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:4:y:2013:i:1:d:10.1038_ncomms3817
    DOI: 10.1038/ncomms3817
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    Cited by:

    1. Panpan Xu & Xingyu Guo & Binglei Jiao & Jinxing Chen & Minghao Zhang & Haodong Liu & Xiaolu Yu & Maura Appleberry & Zhenzhen Yang & Hongpeng Gao & Fan Yang & Xuefei Weng & Yanbin Shen & Jing Gu & Ying, 2024. "Proton-exchange induced reactivity in layered oxides for lithium-ion batteries," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    2. Ivan S. Zhidkov & Azat F. Akbulatov & Liana N. Inasaridze & Andrey I. Kukharenko & Lyubov A. Frolova & Seif O. Cholakh & Chu-Chen Chueh & Pavel A. Troshin & Ernst Z. Kurmaev, 2021. "Influence of Oxygen Ion Migration from Substrates on Photochemical Degradation of CH 3 NH 3 PbI 3 Hybrid Perovskite," Energies, MDPI, vol. 14(16), pages 1-9, August.
    3. Benedikt Axel Brandes & Yogeshwaran Krishnan & Fabian Luca Buchauer & Heine Anton Hansen & Johan Hjelm, 2024. "Unifying the ORR and OER with surface oxygen and extracting their intrinsic activities on platinum," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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