In this article, it is proposed that a membrane with tunable ionic conductivity can be used as a separator between the electrodes of a supercapacitor to both allow normal charge/discharge operation and minimize self-discharge when not in use. It is shown that the redox active conducting polymer PPy(DBS), when polymerized on a porous substrate, will span across the pores of the membrane. PPy(DBS) is also shown to function as an ionic redox transistor, in which the transmembrane ionic conductivity of the polymer membrane is a function of its redox state. The PPy(DBS) ionic redox transistor is applied between the electrodes in a supercapacitor as a smart membrane separator. It is demonstrated that the maximum tunable ionic conductivity of the smart membrane separator is comparable in operation to an industry standard separator at maximum ionic conductivity, with a self-discharge leakage current of ∼0.12mA/cm2 at 1V. The minimum tunable ionic conductivity of the smart membrane separator is shown to decrease the supercapacitor self-discharge when not in use by a factor of 10, with a leakage current of 0.012mA/cm2 at 1V. This range of tunable ionic conductivity could lead to the emergence of redox transistor batteries with high energy density and low self-discharge for short and long-term storage applications.

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