In situ EXAFS study to probe active centers of Ru chalcogenide electrocatalysts during oxygen reduction reaction

被引：57

作者：

Malakhov, IV

Nikitenko, SG

Savinova, ER

Kochubey, DI

Alonso-Vante, N

机构：

[1] Univ Poitiers, CNRS, UMR 6503, Lab Electrocatalysis, F-86022 Poitiers, France

[2] Boreskov Inst Catalysis, Novosibirsk 630090, Russia

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2002年 / 106卷 / 07期

关键词：

D O I：

10.1021/jp011295l

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Novel cluster Ru chalcogenide materials MoxRuySez and RuxTey were studied in situ using EXAFS in the transmission mode during the oxygen reduction reaction. Reversible changes in the structure of the active center were revealed for the electrochemical reaction as a function of the applied electrode potential. The shift of the potential in the anodic direction from 0.08 to 0.78 V versus rhe (reference hydrogen electrode) in the presence of oxygen resulted in an increase of the Ru-O and simultaneous decrease of the Ru-Ru coordination numbers in the first coordination shell of Ru. Along with the variation of the coordination numbers, we observed reversible changes of the coordination distances: a decrease of the Ru-O and an increase of the Ru-Ru distance with the positive polarization. These changes witness the distortion of the catalytic center upon oxygen adsorption. A tentative mechanism of oxygen activation on RuxXy cluster materials is proposed on the basis of the in situ EXAFS data.

引用

页码：1670 / 1676

页数：7

共 39 条

[11] Kinetics of oxygen reduction at RuO2-coated titanium electrode in alkaline solution
Chang, CC
Wen, TC
[J]. JOURNAL OF APPLIED ELECTROCHEMISTRY, 1997, 27 (03) : 355 - 363
[12] Chrzanowski W, 1999, INTERFACIAL ELECTROCHEMISTRY, P937
[13] In-situ XAFS studies of Br adsorption on the silver(111) electrode
Endo, O
Matsumura, D
Kohdate, K
Kiguchi, M
Yokoyama, T
Ohta, T
[J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2000, 494 (02) : 121 - 126
[14] ANION EFFECTS AND THE MECHANISM OF CU UPD ON PT(111) - X-RAY AND ELECTROCHEMICAL STUDIES
GOMEZ, R
YEE, HS
BOMMARITO, GM
FELIU, JM
ABRUNA, HD
[J]. SURFACE SCIENCE, 1995, 335 (1-3) : 101 - 109
[15] GURMAN SJ, 1986, J PHYS C SOLID STATE, V19, P1845, DOI 10.1088/0022-3719/19/11/021
[16] IN-SITU EXAMINATION OF ANODIC SILVER-OXIDE FILMS BY EXAFS IN THE REFLECTION MODE
HECHT, D
BORTHEN, P
STREHBLOW, HH
[J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1995, 381 (1-2): : 113 - 121
[17] INVESTIGATION OF ELECTROCHEMISTRY OF A SERIES OF METAL DIOXIDES WITH RUTILE-TYPE STRUCTURE - MOO2, WO2, REO2, RUO2, OSO2, AND IRO2
HORKANS, J
SHAFER, MW
[J]. JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1977, 124 (08) : 1202 - 1207
[18] Chemical state of ruthenium submonolayers on a Pt(111) electrode
Kim, H
de Moraes, IR
Tremiliosi-Filho, G
Haasch, R
Wieckowski, A
[J]. SURFACE SCIENCE, 2001, 474 (1-3) : L203 - L212
[19] The structure of amorphous bulk and silica-supported copper(II) hydroxides
Kriventsov, VV
Kochubey, DI
Elizarova, GL
Matvienko, LG
Parmon, VN
[J]. JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1999, 215 (01) : 23 - 27
[20] Electrocatalysis on nanoscale ruthenium-based material manufactured by carbonyl decomposition
Le Rhun, V
Garnier, E
Pronier, S
Alonso-Vante, N
[J]. ELECTROCHEMISTRY COMMUNICATIONS, 2000, 2 (07) : 475 - 479

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