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

Hernan Sanchez Casalongue, Sarp Kaya, Venkatasubramanian Viswanathan, Daniel J. Miller, Daniel Friebel, Heine A. Hansen, Jens K. Nørskov, Anders Nilsson and Hirohito Ogasawara ()
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Hernan Sanchez Casalongue: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Sarp Kaya: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Venkatasubramanian Viswanathan: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
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
Heine A. Hansen: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Jens K. Nørskov: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Anders Nilsson: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Hirohito Ogasawara: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory

Nature Communications, 2013, vol. 4, issue 1, 1-6

Abstract: 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.

Date: 2013
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DOI: 10.1038/ncomms3817

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