Journal of Physical Chemistry p. 6383 - 6389 (1991)
Update date:2022-08-11
Topics:
Dalton, E. F.
Murray, Royce W.
A analysis is given of the electron-self-exchange reactions responsible for the steady-state redox conductivity of thin films of the electropolymerized monomer N,N'-bis(3-pyrrol-1-yl-propyl)-4,4'-bipyridinium tetrafluoroborate, sandwiched between two electrodes.Concentration-gradient-driven electron self-exchange in the liquid-acetonitrile-bathed viologen(2+/1+) mixed-valent state of this polymer, kex = 8 x 103 M-1 s-1, is much slower than that for the viologen (1+/0) mixed valent-state, kex = 1.6 x 105 M-1 s-1, which has a smaller activation barrier.Neither self-exchange reaction responds to use of alternative counterions except that both rates decrease in polymer containing tosylate counterions.The rate constant found for the electrical-gradient-driven viologen (1+/0) electron self-exchange, kex = 1.1 x 105 M-1 s-1, observed in dry, N2-bathed polymer where ClO4(1-) counterion mobility is quenched, is nearly the same as the acetonitrile-bathed value.The rate constants appear to be dominated by characteristics of the polymer phase rather than the bathing environment of the polymer.Estimates are made of the counteranion diffusivity in acetonitrile-bathed films and of how it affects transient electron transport measurements.
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