By Jean-Michel Savéant
This booklet relies at the George Fisher Baker Lecture given by means of Jean-Michel Savéant at Cornell college in Fall 2002.The first publication concentrating on molecular electrochemistryRelates to different fields, together with photochemistry and biochemistryOutlines truly the relationship among thoughts, experimental illustrations, proofs and helping methodsAppendixes to supply rigorous demonstrations to avoid an overload of algebra often textApplications-oriented, excited by examining the consequences bought instead of the method
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Additional info for Elements of Molecular and Biomolecular Electrochemistry: An Electrochemical Approach to Electron Transfer Chemistry
1. Introduction Continuing the study of simple outer-sphere electron transfer reactions, AzA þ eÀ Ð BzA À1 attention is now focused on the kinetics of the reaction and how it can be characterized by an electrochemical technique such as cyclic voltammetry. The case of a reduction continues to be taken as an example, transposition to oxidation requiring obvious changes of signs. The electrochemical responses now depend on both the rate of electron transfer and either the rate of diffusion, for freely moving reactants, or the potential scan rate, for immobilized reactants.
37 ELECTRON TRANSFER KINETICS also means that the transfer coefficient is a linear function of the driving force rather than independent of it as in the Butler–Volmer case: 6¼ a¼X ¼ 6 Yj¼ ð8jÞ ¼ 0:5 1 þ ! ÁG0 4ÁG6¼ 0 ¼ 0:5 1 þ E À E0 4ÁG6¼ 0 ! 4, where the experimental detection of this variation is discussed. So far, only the nuclear reorganization energy attending electron transfer has been discussed, yielding the expressions above of the free energy of activation in the framework of classical transition state theory.
It follows that RDEV cannot compete with transient techniques such as cyclic voltammetry in the kinetic characterization of fast processes. One attractive feature of RDEV is nonetheless the simplicity of the relationship between the current flowing through the electrode and the concentrations of the reactants at the electrode surface. 10a. 10b) according to ðCA Þx¼0 i ¼1À 0 il C ðCB Þx¼0 i ¼ il C0 ð1:15Þ where C 0 is the bulk concentration of A, and il ¼ FSC 0 DAB 2=3 1=2 ¼ 0:62FSC 0 DAB nÀ1=6 oR d ð1:16Þ is the plateau current (amperes) reached when the potential is negative enough for the concentration of A at the electrode surface to be nil, or, equivalently, the concentration of B to equal C 0 .
Elements of Molecular and Biomolecular Electrochemistry: An Electrochemical Approach to Electron Transfer Chemistry by Jean-Michel Savéant