Abstract
A novel electrode coating material was synthesized by bulk, radical copolymerization of acrylamide, bisacrylamide and vinylpyridine in aqueous solutions. Highly swelled, porous gels were obtained. Sections of the copolymeric gels, a fraction of a micrometer in thickness, were cut with a microtome and deposited on glassy carbon disk electrodes. Electrochemical measurements involving chronocoulometry, cyclic voltammetry and rotating disk methods were used to characterize these electrode coatings in terms of their physical structure and ion-exchange properties. After ion-exchange incorporation of ferricyanide ions, mediated electrooxidation of ascorbic acid was investigated in an acidic electrolyte. The kinetics of the processes involved in this electrocatalysis were analyzed according to the Savéant-Andrieux theory. All electrocatalytic systems behaved according to the R + S case. Detailed analysis of the electrocatalysis data allowed us to relate the key parameters determining the system's performance to the structure and the composition of the gel films. Self-segregation of vinylpyridine groups during polymerization of a gel in acidic solution was revealed and related to its superior ion-exchange properties and the high catalytic activity of the bound ferricyanide ions.
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