In Situ Electrochemical X-ray Absorption Spectroscopy of Oxygen Reduction Electrocatalysis with High Oxygen Flux

被引：78

作者：

Erickson, Evan M. ^{[2
]}

Thorum, Matthew S. ^{[2
]}

Vasic, Relja ^{[1
]}

Marinkovic, Nebojsa S. ^{[3
]}

Frenkel, Anatoly I. ^{[1
]}

Gewirth, Andrew A. ^{[2
]}

Nuzzo, Ralph G. ^{[2
]}

机构：

[1] Yeshiva Univ, Dept Phys, New York, NY 10016 USA

[2] Univ Illinois, Dept Chem, Urbana, IL 61801 USA

[3] Univ Delaware, Ctr Catalyt Sci & Technol, Newark, DE 19716 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2012年 / 134卷 / 01期

关键词：

FUEL-CELL; SURFACE-PROPERTIES; WATER ACTIVATION; PLATINUM; CATALYSTS; ALLOYS; ELECTROREDUCTION; PERFORMANCE; ENVIRONMENT; KINETICS;

D O I：

10.1021/ja210465x

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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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收藏

页码：197 / 200

页数：4

相关论文

共 34 条

[1] Optimization of a permeation-based microfluidic direct formic acid fuel cell (DFAFC) [J].

Erickson, Evan M. ;

Mitrovski, Svetlana M. ;

Gewirth, Andrew A. ;

Nuzzo, Ralph G. .

ELECTROPHORESIS, 2011, 32 (08) :947-956

[2] Thermodynamic guidelines for the design of bimetallic catalysts for oxygen electroreduction and rapid screening by scanning electrochemical microscopy.: M-Co (M: Pd, Ag, Au) [J].

Fernández, JL ;

Walsh, DA ;

Bard, AJ .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (01) :357-365

[3] Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs [J].

Gasteiger, HA ;

Kocha, SS ;

Sompalli, B ;

Wagner, FT .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 56 (1-2) :9-35

[4] Electroreduction of Dioxygen for Fuel-Cell Applications: Materials and Challenges [J].

Gewirth, Andrew A. ;

Thorum, Matthew S. .

INORGANIC CHEMISTRY, 2010, 49 (08) :3557-3566

[5]

Greeley J, 2009, NAT CHEM, V1, P552, DOI [10.1038/nchem.367, 10.1038/NCHEM.367]

[6] INSITU STUDIES OF A DISPERSED PLATINUM ON CARBON ELECTRODE USING X-RAY ABSORPTION-SPECTROSCOPY [J].

HERRON, ME ;

DOYLE, SE ;

PIZZINI, S ;

ROBERTS, KJ ;

ROBINSON, J ;

HARDS, G ;

WALSH, FC .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1992, 324 (1-2) :243-258

[7] INSTRUMENTATION AND CELL DESIGN FOR INSITU STUDIES OF ELECTRODE SURFACES USING X-RAY SYNCHROTRON RADIATION [J].

HERRON, ME ;

DOYLE, SE ;

ROBERTS, KJ ;

ROBINSON, J ;

WALSH, FC .

REVIEW OF SCIENTIFIC INSTRUMENTS, 1992, 63 (01) :950-955

[8] Effect of loading level in platinum-dispersed carbon black electrocatalysts on oxygen reduction activity evaluated by rotating disk electrode [J].

Higuchi, E ;

Uchida, H ;

Watanabe, M .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2005, 583 (01) :69-76

[9] EFFECT OF CHEMICAL ENVIRONMENT ON MAGNITUDE OF X-RAY ABSORPTION RESONANCE AT LLLL EDGES - STUDIES ON METALLIC ELEMENTS, COMPOUNDS, AND CATALYSTS [J].

LYTLE, FW ;

WEI, PSP ;

GREEGOR, RB ;

VIA, GH ;

SINFELT, JH .

JOURNAL OF CHEMICAL PHYSICS, 1979, 70 (11) :4849-4855

[10] QUANTITATIVE TECHNIQUE FOR THE DETERMINATION OF THE NUMBER OF UNOCCUPIED D-ELECTRON STATES IN A PLATINUM CATALYST USING THE L2,3 X-RAY ABSORPTION-EDGE SPECTRA [J].

MANSOUR, AN ;

COOK, JW ;

SAYERS, DE .

JOURNAL OF PHYSICAL CHEMISTRY, 1984, 88 (11) :2330-2334

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