Appearance of an oscillation through the autocatalytic mechanism by control of the atomic-level structure of electrode surfaces in electrochemical H2O2 reduction at Pt electrodes

被引:46
作者
Nakanishi, S
Mukouyama, Y
Karasumi, K
Imanishi, A
Furuya, N
Nakato, Y [1 ]
机构
[1] Osaka Univ, Grad Sch Engn Sci, Dept Chem, Toyonaka, Osaka 5608531, Japan
[2] Univ Yamanashi, Fac Engn, Dept Appl Chem, Yamanashi 4008510, Japan
来源
JOURNAL OF PHYSICAL CHEMISTRY B | 2000年 / 104卷 / 17期
关键词
D O I
10.1021/jp993961c
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
The influence of the atomic-level structure of electrode surfaces on electrochemical oscillations has been studied in a system of H2O2 reduction on Pt electrodes in acidic solutions. A current oscillation of another type, named oscillation E, has been found to appear for an atomically flat single-crystal Pt(111) electrode, in addition to previously reported oscillations, named oscillations A and B. Oscillation E does not appear for atomically flat Pt(100), Pt(110), polycrystalline Pt, and Pt(111) with atomically nonflat surfaces. Mathematical simulation by use of a model including an autocatalytic effect of adsorbed OH for dissociative adsorption of H2O2, as a possible explanation, has reproduced the appearance of oscillation E, as well as observed correlations between the appearance of oscillation E and the magnitudes of H2O2-reduction current and "negative" resistance. It is discussed that an efficient autocatalytic mechanism works at the atomically flat Pt(111) surface, which is responsible for the appearance of oscillation E at this surface.
引用
收藏
页码:4181 / 4188
页数:8
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