Multiple oxidation-state metal oxide has presented a promising charge storage capability for aqueous supercapacitors (SCs); however, the ion insert/deinsert behavior in the bulk phase generally gives a sluggish reaction kinetic and considerable volume effect. Herein, iron oxide/poly(3,4-ethylenedioxythiophene) (FeO/PEDOT) heterointerface was constructed and enabled boosted Faradaic pseudocapacitance by dual-ion-involved redox reactions in NaSO electrolytes. The FeO/PEDOT interface served as a "bridge" to couple electrode and anion SO and exhibited a strong force and stable bonding with SO, thus providing an additional Faradaic charge storage contribution for SCs. Significantly, the PEDOT-capsulated FeO nanorod array (FeO@PEDOT) electrode presented a specific capacitance of 338 mF cm at 1 mA cm with 1 M NaSO electrolyte, which was twice that of the pristine FeO nanorod electrode. The boosted interfaced Faradaic reaction of SO partially hindered the intercalation of Na in the FeO bulk phase, efficiently favoring the electrochemical stability.
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