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Proton-coupled intervalence charge transfer: concerted processes.

Ramachandran Balasubramanian1, Geneviève Blondin, Juan Carlos Canales

  • 1Université Paris Diderot , Sorbonne Paris Cité, Laboratoire d'Electrochimie Moléculaire, Unité Mixte de Recherche Université - CNRS 7591, Bâtiment Lavoisier, 15 rue Jean de Baïf, 75205 Paris Cedex 13, France.

Journal of the American Chemical Society
|January 21, 2012
PubMed
Summary

Electrochemical methods reveal proton-induced intervalence charge transfer (IVCT) kinetics. Analysis of a diiron complex suggests a concerted pathway is favored over stepwise routes, opening avenues for reactivity studies.

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Area of Science:

  • Electrochemistry
  • Chemical Kinetics
  • Inorganic Chemistry

Background:

  • Proton-induced intervalence charge transfer (IVCT) is crucial in various chemical and biological systems.
  • Understanding the kinetics and mechanisms of IVCT is essential for controlling reactivity.
  • Electrochemical techniques offer a powerful tool for probing fast electron transfer processes.

Purpose of the Study:

  • To develop and apply an electrochemical method for studying proton-induced IVCT kinetics.
  • To elucidate the dominant reaction pathway (concerted vs. stepwise) in proton-induced IVCT.
  • To establish a foundation for systematic kinetic investigations of IVCT reactions.

Main Methods:

  • In situ electrochemical generation of one IVCT couple member.
  • Monitoring the conversion via the electrochemical signature of the other couple member.
  • Kinetic analysis incorporating the H/D isotope effect.

Main Results:

  • A novel electrochemical approach was successfully employed to measure proton-induced IVCT kinetics.
  • Kinetic analysis, including the H/D isotope effect, strongly supports a concerted proton-IVCT pathway.
  • Stepwise pathways were found to be less prevalent under the studied conditions.

Conclusions:

  • The study demonstrates a viable electrochemical strategy for investigating proton-induced IVCT kinetics.
  • Concerted proton-transfer coupled with intervalence charge transfer is identified as a key mechanism.
  • This work paves the way for detailed studies on factors governing IVCT pathway selectivity.