期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 112, 期 42, 页码 16663-16667出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp802873e
关键词
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资金
- University Development Fund on Molecular Functional Materials
- University of Hong Kong and CERG
- Hong Kong Special Administrative Region, China [HKU 7061/04P, HKU 7059/05P]
We describe the effects of electrochemical pretreatment of glassy carbon electrodes (GCEs) on the electrogenerated chemiluminescence (ECL) of the Ru(bpy)(3)(2+) (bpy = 2,2'-bipyridine)/tri-n-propylamine (TPrA) system. It has been found that the oxidation of TPrA at the anodically pretreated GCEs became more facile, while the intensity of ECL could be greatly suppressed. The contravention between the electrochemical reaction kinetics and the light emission intensity of the coreactant ECL system was reported for the first time and has been attributed to the rapid deprotonation of TPrA(center dot+) cation radicals by the aid of oxygen-containing surface species formed on the GCE during the pretreatment. Because the lifetime of TPrA(center dot+) was reduced, the products of the deprotonation reaction, TPrA(center dot) free radicals, would be more subject to oxidative consumption on the electrode subsequently, leading to weaker ECL signals. When the ECL was produced mainly following a catalytic route, however, the electrode surface effect was much less significant. This study suggests that the long lifetime of TPrA(center dot+) cation radicals may be crucial for the intense light emission, which allows a sufficient amount of highly reducing intermediate radicals, TPrA(center dot), to participate in the ECL process within a relatively thick reaction layer before being destroyed by the electrode.
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