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pH-induced, long-range electron transfer across a thin polymeric film

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j100402a001· OSTI ID:5497002

A bilayer of thin polymeric films on a glassy carbon electrode was prepared by electropolymerizing ((bpy)/sub 2/Os(vpy)/sub 2/)(PF/sub 6/)/sub 2/ (bpy = 2,2'-bipyridine, vpy = 4-vinylpyridine), to form the inner layer, and adding as an outer layer Nafion into which the complex ((bpy)/sub 2/(py)Ru(OH)/sub 2/))/sup 2 +/ (py = pyridine) was ion exchanged. The Os(III)/(II) couple is pH independent with E/sub 1/2/ = 0.55 V while E/sub 1/2/ for the Ru(III)/(II) couple varies from 0.76 to 0.20 V over the pH range 1 to 10, (bpy)/sub 2/(py)Ru/sup III/-OH/sup 2 +/ + e/sup -/ + H/sup +/ ..-->.. (bpy)/sub 2/(py)Ru/sup II/-OH/sub 2//sup 2 +/. At pH 5.0 the potentials of the couples in the inner and outer films are the same. By decreasing the pH in the external solution to pH 2.0 with the electrode potential held at 0.60 V (i.e., both films initially as M(III)), a long-range electron transfer occurs from the electrode through the intervening Os film to Ru(III) sites in the outer film. Upon returning the pH in the external solution to 5.0, the reverse process occurs, and long-range electron transfer from Ru(II) to the electrode is mediated by the inner film.

Research Organization:
Univ. of North Carolina, Chapel Hill
OSTI ID:
5497002
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 90:11; ISSN JPCHA
Country of Publication:
United States
Language:
English