Conducting polymers have attracted much attention for a number of applications, such as batteries, sensors, selective membranes, and electronic devices. 1 The major problem of these materials, however, has been their inherent intractability as they are insoluble in most solvents. With this respect, there has been increasing interest in soluble submicron conducting-polymer particles, which further suggest other potential applications, such as soluble ion exchangers, microcapsules, energy storage materials, corrosion resistant coatings and catalysts, the properties of which can be controlled externally by the potential. [2][3][4][5] The conducting polymer particles are synthesized in the presence of a polymeric stabilizer, which adsorbs onto polymer nuclei and prevents their further aggregation via a steric stabilization mechanism. [6][7][8][9][10][11][12] We have recently examined the ion exchange properties of polyaniline particles for analytical purposes. 2,3,13-16 The composite particles consisting of polyaniline and polystyrene sulfonate can quantitatively take up many organic anions in the emeraldine-based form and eject them by reduction or deprotonation. Such particles can be used as intelligent ion-exchange microcapsules, the exchange capacity of which can be controlled by the potential in solution. However, during these studies, we found that the quantitative ejection of organic anions by reducing the particles was often difficult, especially in the case of electrochemical reduction, which was carried out in anaerobic condition. This is partly due to incomplete reduction of the polypyrrole core, which may be caused by an insulation effect of the stabilizer or of reduced polymer created at the core surface. Thus, we focus here on the improvement in the redox activity to have complete control for uptake and ejection with the potential.The electroactivity is also important for applications to energy storage. The reduced particles can store electrical energy as a condensed lightweight form, which is obtained by centrifugation or filtration and redispersed in solution as they are required. This would solve a current problem of redox-flow energy-storage systems, which require huge reservoirs to store electroactive materials in solutions. If atmospheric oxygen and the dehydrated and reduced colloidal particles, which are redispersed in water in situ, can be used to generate the electric power, then the reservoir capacities can be much smaller than those required for the redox-flow systems based on the current design.Experimental Chemicals.-Pyrrole (Wako Chemical Co., Saitama, Japan) was used without further purification. Poly(vinylpyrrolidone) K90 (PVP; Mw ϭ 1.2 ϫ 10 6 ) and poly(vinyl alcohol) (PVA; Mw ϭ 2.2 ϫ 10 4 ; degree of hydrolyzation, 88%) were purchased from Wako Chemicals. All the other chemicals used here were of reagent grade, and Milli-Q water (12-18 M⍀ cm) was used throughout. Reagent grade 9,10-anthraquinone-2-sulfonate (AQS Ϫ ) was added as its sodium salt.Preparation of colloidal particles.-Bul...