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I. INTRODUCTION The structure and dynamics of the liquid/liquid interface have been the focus of considerable research activity (for review of the electrochemistry of ITIES, see Ref. 1). In addition to fundamental interest, the charge-transfer (CT) reactions occurring at the liquid/liquid interface, i.e., electron transfer (ET), simple ion transfer (IT), and facilitated IT, are relevant to important technological systems from chemical sensors to drug delivery in pharmacology to solvent extraction in hydrometallurgy (1,2). At the interface between two immiscible electrolyte solutions (ITIES), one can conduct reactions that cannot occur at solid electrodes, e.g., reactions involving species of very different polarities. These reactions find applications in electrochemical catalyses and synthesis (for examples, see Ref. 3). The liquid/liquid interface has been suggested as a simple model for biological and artificial membranes (4).