window (around 3 V) are more favorable for practical applications. Up to date, only an ultrafast OEC based on CNT films has been reported in literature. [10] However, the preparation of CNT electrodes involved complicated processes of vacuum filtration and expensive chemical vapor deposition. Therefore, a facile and scalable method to fabricate OECs with excellent AC line-filtering performances still remains as a challenge.In this paper, we report the fabrication of OECs based on electrochemically reduced less defective graphene oxide (ERLGO) films with oriented 3D interconnected porous structures. For optimizing the performance of ERLGO electrode, LGO sheets with a small average size of 0.7 µm (sLGO) were used and the resulting ERsLGO electrode was further deeply reduced in an organic electrolyte. The typical OEC exhibited high areal specific energy density, excellent electrochemical stability, and superior rate capability, promising for AC line filtering. These OECs can also be connected in series or parallel to meet various demands in industrial levels.
Results and DiscussionThe graphene electrode (Figure 1a) was prepared by electrochemical reduction of LGO or sLGO sheets in their aqueous dispersion (3 mg mL −1 ) at −1.1 V for 4 s, then further deeply reduced in an organic electrolyte at −2.0 V for 20 s. The organic electrolyte was 1 mol L −1 acetonitrile (AN) solution of tetraethylammonium-tetrafluoroborate (TEABF 4 ). LGO sheets were prepared by oxidation of graphite flakes at a low temperature of 0 °C. [19] They have an average lateral dimension of 7 µm (Figure 1b, Figure S1, Supporting Information). During the electrodeposition process, LGO sheets were selfassembled onto the surface of substrate electrode upon the driving by directional electric field. [20] Simultaneously, they were electrochemically reduced to ERLGO sheets to form a porous network because of π-π stacking and hydrophobic interactions. However, the ERLGO electrode has a relatively disordered porous structure ( Figure S2, Supporting Information) because of the steric obstacles of these large graphene sheets during their self-assembling process. Therefore, we pulverized LGO sheets in their aqueous dispersion by sonication, significantly reducing their average size to around 0.7 µm (Figure 1c, Less-defective graphene oxide sheets with a small average size of 0.7 µm are electrochemically reduced to form a hydrogel film with highly oriented porous structure. It is applied as the electrode of organic electrochemical capacitor (OEC) after solvent change with organic electrolyte and deep reduction in this organic medium. At 120 Hz, the typical OEC exhibits a high areal specific energy density of 472 µF V 2 cm −2 with a wide workable voltage window of 2.5 V, a phase angle of −80.5°, a resistor-capacitor time constant (τ RC ) of 0.219 ms, and an excellent electrochemical stability. Thus, it is promising to replace aluminum electrolytic capacitors for AC line filtering. Furthermore, two identical OECs connected in series keep the performance of single...