In Situ X-Ray Probing Reveals Fingerprints of Surface Platinum Oxide

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In situ x-ray absorption spectroscopy (XAS) at the Pt L{sub 3} edge is a useful probe for Pt-O interactions at polymer electrolyte membrane fuel cell (PEMFC) cathodes. We show that XAS using the high energy resolution fluorescence detection (HERFD) mode, applied to a well-defined monolayer Pt/Rh(111) sample where the bulk penetrating hard x-rays probe only surface Pt atoms, provides a unique sensitivity to structure and chemical bonding at the Pt-electrolyte interface. Ab initio multiple-scattering calculations using the FEFF8 code and complementary extended x-ray absorption fine structure (EXAFS) results indicate that the commonly observed large increase of the white-line at high ... continued below

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Friebel, Daniel August 24, 2011.

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In situ x-ray absorption spectroscopy (XAS) at the Pt L{sub 3} edge is a useful probe for Pt-O interactions at polymer electrolyte membrane fuel cell (PEMFC) cathodes. We show that XAS using the high energy resolution fluorescence detection (HERFD) mode, applied to a well-defined monolayer Pt/Rh(111) sample where the bulk penetrating hard x-rays probe only surface Pt atoms, provides a unique sensitivity to structure and chemical bonding at the Pt-electrolyte interface. Ab initio multiple-scattering calculations using the FEFF8 code and complementary extended x-ray absorption fine structure (EXAFS) results indicate that the commonly observed large increase of the white-line at high electrochemical potentials on PEMFC cathodes originates from platinum oxide formation, whereas previously proposed chemisorbed oxygen-containing species merely give rise to subtle spectral changes.

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  • Journal Name: Submitted to Physical Chemistry Chemical Physics

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  • Report No.: SLAC-PUB-13855
  • Grant Number: AC02-76SF00515
  • Office of Scientific & Technical Information Report Number: 1023233
  • Archival Resource Key: ark:/67531/metadc837430

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  • August 24, 2011

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  • May 19, 2016, 3:16 p.m.

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  • Nov. 29, 2016, 2:53 p.m.

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Friebel, Daniel. In Situ X-Ray Probing Reveals Fingerprints of Surface Platinum Oxide, article, August 24, 2011; United States. (digital.library.unt.edu/ark:/67531/metadc837430/: accessed October 23, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.