The modification of glassy carbon and gold electrodes with aryl diazonium salt:: The impact of the electrode materials on the rate of heterogeneous electron transfer

The modification of glassy carbon and gold electrodes with aryl diazonium salt:: The impact of the electrode materials on the rate of heterogeneous electron transfer
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DOI:
10.1016/j.chemphys.2005.03.033
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发表时间:
2005-12-07
期刊:
影响因子:
2.3
通讯作者:
Gooding, JJ
Gooding, JJ
中科院分区:
化学3区
文献类型:
--
作者:
Liu, GZ;Liu, JQ;Gooding, JJ

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用循环伏安法研究了二茂铁乙胺与4-羧基苯基/苯基混合单分子膜在玻碳(GC)和金电极上的非均相电子转移性质。电极在逐步过程中衍生化。4-羧基苯基和苯基重氮盐的混合物在电极表面的电化学还原产生稳定的单分子膜。通过X射线光电子能谱验证了表面上的羧酸部分的引入。随后,使用水溶性碳二亚胺和N-羟基琥珀酰亚胺活化4-羧基苯基部分,并与二茂铁甲胺反应。使用电子转移的Marcus理论,由循环伏安图确定通过单层系统的电子转移速率常数,并且发现在金上的二茂铁改性的单层系统的速率常数比在GC电极上的速率常数高一个数量级。结果表明,电极材料对电子转移速率有重要影响。(c)2005 Elsevier B. V.保留所有权利。
The heterogeneous electron-transfer properties of ferrocenemethylamine coupled to a series of mixed 4-carboxyphenyl/phenyl monolayers on glassy carbon (GC) and gold electrodes were investigated, by cyclic voltammetry, in aqueous buffer solutions. The electrodes were derivatized in a step-wise process. Electrochemical reduction of mixtures of 4-carboxyphenyl and phenyl diazonium salts on the electrode surfaces yielded stable monolayers. The introduction of carboxylic acid moieties onto the surfaces was verified by X-ray photoelectron spectroscopy. Subsequently the 4-carboxyphenyl moieties were activated using water-soluble carbodiimide and N-hydroxysuccinimide and reacted with ferrocenernethylamine. the rate constants of electron transfer through the monolayer systems were determined from cyclic voltammograms, using the Marcus theory for electron transfer and were found to be an order of magnitude higher for the ferrocene-modified monolayer systems on gold than those on GC electrodes. The results suggest the electrode material has an important influence on the rate of electron transfer. (c) 2005 Elsevier B.V. All rights reserved.