In situ electrochemical X-ray absorption spectroscopy of oxygen reduction electrocatalysis with high oxygen flux |
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| Authors: | Erickson Evan M Thorum Matthew S Vasić Relja Marinković Nebojša S Frenkel Anatoly I Gewirth Andrew A Nuzzo Ralph G |
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| Institution: | Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA. |
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| Abstract: | 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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