Journal of the American Chemical Society p. 4790 - 4798 (1980)
Update date:2022-08-11
Topics:
Klingler, R. J.
Kochi, J. K.
The anodic peak potentials in the irreversible cyclic voltammograms of various homoleptic alkylmetals in acetonitrile show a striking linear correlation with their ionization potentials ID determined in the gas phase.Application of various transient electrochemical techniques proves that the electrode process arises from a totally irreversible ECE sequence in which the peak potential is determined solely by the kinetics of heterogeneous electron transfer and diffusion-uncomplicated by any follow-up chemical reaction.As a result, the anodic peak potential Ep can be directly related to the activation free energy for electron transfer, and the correlation of EP and ID represents a linear free-energy relationship.The mechanism of heterogeneous electron transfer is described as an outer-sphere process, dependent only on the driving force for one-electron oxidation and independent of steric effects of the alkylmetal.The close relationship between the activated compexes for heterogeneous and homogeneous electron transfer is emphasized in a direct comparison of the electrochemical process with the oxidation of the same alkylmetals by a series of poly(pyridine)iron(III) complexes in solution.
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