Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 1, Pages 197-200Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja210465x
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Funding
- U.S. DOE [DE-FG02-05ER46260, DE-FG02-03ER15476]
- Synchrotron Catalysis Consortium (U.S. DOE) [DE-FG02-05ER15688]
- U.S. Department of Energy (DOE) [DE-FG02-05ER46260] Funding Source: U.S. Department of Energy (DOE)
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An in situ electrochemical X-ray absorption spectroscopy (XAS) cell has been fabricated that enables high oxygen flux to the working electrode by utilizing a thin poly(dimethylsiloxane) (PDMS) window. This cell design enables in situ XAS investigations of the oxygen reduction reaction (ORR) at high operating current densities greater than 1 mA in an oxygen-purged environment. When the cell was used to study the ORR for a Pt on carbon electrocatalyst, the data revealed a progressive evolution of the electronic structure of the metal clusters that is both potential-dependent and strongly current-dependent. The trends establish a direct correlation to d-state occupancies that directly tracks the character of the Pt-O bonding present.
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