The results and discussion are presented in the following order. In Section I, we provide a brief overview of the electrochemical reduction of S2O8 2-and oxidation of C2O4 2-. In Section II, we demonstrate that the heterogeneous reduction of S2O8 2-at a glassy carbon (GC) electrode in the presence of only C2O4 2-does not lead to autocatalysis, a consequence of the direct reduction of SO4 •-at the GC electrode. In Section III, the mediated reduction of S2O8 2-using the Ru(NH3)6 3+/2+ couple is shown using cyclic voltammetry to initiate rapid autocatalysis in the presence of C2O4 2-. DEMS results monitoring CO2 production after the initiation step is terminated are also presented in this section. In Section IV, CPE experiments are used to determine the electrical charge passed during electrolysis of bulk solutions of S2O8