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Ion Modulated Electroactivity in Thin Film Metallopolymers
NORTHWESTERN UNIV EVANSTON IL DEPT OF CHEMISTRY
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Electroactivity in thin-film redox polymers derived from Fe2, 2bipyridine332 and Fephenanthroline332 can be tremendously modulated by replacing conventional counter ions such as perchlorate with alkylsulfonates CH3CH2 nSO3, n0-11. With large n species, the amount of charge passed during metal oxidation decreases reversibly by nearly an order of magnitude, while the rate of charge flow as measured transiently by chronocoulometry similarly decreases, again reversibly. Redox thermodynamic effects systematic shifts in film-based formal potentials are also seen. The unusual coupling of redox and ionic conductivity processes uncovered here appears to be related to 1 the large free-volume demands of the alkylsulfonates, and 2 fundamental limitations on the ability of the metallopolymer to meet those demands.
APPROVED FOR PUBLIC RELEASE