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Which mechanism operates in the electron-transfer process at liquid/liquid interfaces?

We present a more general expression for the relationship of potential dependence, which implies that a change in the interfacial drop across the interface has little effect on the free energy of the reaction, but mainly affects the surface concentration of reactant in each phase. Abundant experimen... Full description

Journal Title: Physical chemistry chemical physics : PCCP February 21, 2011, Vol.13(7), pp.2774-2779
Main Author: Zhou, Min
Other Authors: Gan, Shiyu , Zhong, Lijie , Dong, Xiandui , Niu, Li
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: E-ISSN: 1463-9084 ; DOI: 10.1039/c0cp01692f
Link: http://search.proquest.com/docview/849433578/?pq-origsite=primo
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title: Which mechanism operates in the electron-transfer process at liquid/liquid interfaces?
format: Article
creator:
  • Zhou, Min
  • Gan, Shiyu
  • Zhong, Lijie
  • Dong, Xiandui
  • Niu, Li
subjects:
  • Chemistry
ispartof: Physical chemistry chemical physics : PCCP, February 21, 2011, Vol.13(7), pp.2774-2779
description: We present a more general expression for the relationship of potential dependence, which implies that a change in the interfacial drop across the interface has little effect on the free energy of the reaction, but mainly affects the surface concentration of reactant in each phase. Abundant experimental results from several well-known groups are analyzed in great detail to confirm our conclusion. At the same time, we define a new parameter named Frumkin correction factor to describe this relationship of potential dependence, which expresses the thermodynamic effect of double diffuse layers within both phases in contrast with the so often suggested kinetic electron-transfer (ET) coefficient; we also find that it depends on two intimately related aspects: the charges of reactive species and the ratio of the diffuse layer potential to the total potential within each phase, so it is quite arbitrary to ignore the diffuse layer effect in the aqueous phase just because of its relatively small values. In addition, a fascinating question on the inverted region at liquid/liquid interfaces has been successfully interpreted by an opposite surface concentration effect, which was often considered as a kinetic Marcus inverse by most groups.
language: eng
source:
identifier: E-ISSN: 1463-9084 ; DOI: 10.1039/c0cp01692f
fulltext: fulltext
issn:
  • 14639084
  • 1463-9084
url: Link


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descriptionWe present a more general expression for the relationship of potential dependence, which implies that a change in the interfacial drop across the interface has little effect on the free energy of the reaction, but mainly affects the surface concentration of reactant in each phase. Abundant experimental results from several well-known groups are analyzed in great detail to confirm our conclusion. At the same time, we define a new parameter named Frumkin correction factor to describe this relationship of potential dependence, which expresses the thermodynamic effect of double diffuse layers within both phases in contrast with the so often suggested kinetic electron-transfer (ET) coefficient; we also find that it depends on two intimately related aspects: the charges of reactive species and the ratio of the diffuse layer potential to the total potential within each phase, so it is quite arbitrary to ignore the diffuse layer effect in the aqueous phase just because of its relatively small values. In addition, a fascinating question on the inverted region at liquid/liquid interfaces has been successfully interpreted by an opposite surface concentration effect, which was often considered as a kinetic Marcus inverse by most groups.
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