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

Materials Science and Engineering

Stony Brook University

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

82 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 - Jan 11 2012

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title = "In situ electrochemical X-ray absorption spectroscopy of oxygen reduction electrocatalysis with high oxygen flux",

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.",

author = "Erickson, \{Evan M.\} and Thorum, \{Matthew S.\} and Relja Vasi{\'c} and Marinkovi{\'c}, \{Nebojŝa S.\} and Frenkel, \{Anatoly I.\} and Gewirth, \{Andrew A.\} and Nuzzo, \{Ralph G.\}",

year = "2012",

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doi = "10.1021/ja210465x",

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T1 - In situ electrochemical X-ray absorption spectroscopy of oxygen reduction electrocatalysis with high oxygen flux

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

Y1 - 2012/1/11

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.

UR - https://www.scopus.com/pages/publications/84855658133

U2 - 10.1021/ja210465x

DO - 10.1021/ja210465x

M3 - Article

SN - 0002-7863

VL - 134

SP - 197

EP - 200

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 1

ER -

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

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