In situ electrochemical X-ray absorption spectroscopy of oxygen reduction electrocatalysis with high oxygen flux

Evan M. Erickson; Matthew S. Thorum; Relja Vasić; Nebojŝa S. Marinković; Anatoly I. Frenkel; Andrew A. Gewirth; Ralph G. Nuzzo

doi:10.1021/ja210465x

In situ electrochemical X-ray absorption spectroscopy of oxygen reduction electrocatalysis with high oxygen flux

Evan M. Erickson, Matthew S. Thorum, Relja Vasić, Nebojŝa S. Marinković, Anatoly I. Frenkel, Andrew A. Gewirth, Ralph G. Nuzzo

Research output: Contribution to journal › Article › peer-review

80 Scopus citations

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.

Original language	English
Pages (from-to)	197-200
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	134
Issue number	1
DOIs	https://doi.org/10.1021/ja210465x
State	Published - 11 Jan 2012
Externally published	Yes

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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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AU - Erickson, Evan M.

AU - Thorum, Matthew S.

AU - Vasić, Relja

AU - Marinković, Nebojŝa S.

AU - Frenkel, Anatoly I.

AU - Gewirth, Andrew A.

AU - Nuzzo, Ralph G.

PY - 2012/1/11

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N2 - 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.

AB - 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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In situ electrochemical X-ray absorption spectroscopy of oxygen reduction electrocatalysis with high oxygen flux

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