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There is strong interest in developing high-frequency (HF) supercapacitors or electrochemical capacitors (ECs), which can work at the hundreds to kilo hertz range for line-frequency alternating current (AC) filtering in the substitution of bulky aluminum electrolytic capacitors, with broad applications in the power and electronic fields. Although great progress has been achieved in the studies of electrode materials for ECs, most of them are not suitable to work in this high frequency range because of the slow electrochemical processes involved. Edge-oriented vertical graphene (VG) networks on 3D scaffolds have a unique structure that offers straightforward pore configuration, reasonable surface area, and high electronic conductivity, thus allowing the fabrication of HF-ECs. Comparatively, highly conductive freestanding cross-linked carbon nanofibers (CCNFs), derived from bacterial cellulose in a rapid plasma pyrolysis process, can also provide a large surface area but free of rate-limiting micropores, and are another good candidate for HF-ECs. In this mini review, advances in these fields are summarized, with emphasis on our recent contributions in the study of these materials and their electrochemical properties including preliminary demonstrations of HF-ECs for AC line filtering and pulse power storage applications. 

There is a strong interest in increasing the frequency response of electrochemical capacitors (ECs) from typically less than 1 Hz to the hundreds or the kilo Hz range, so that such high-frequency ECs (HF-ECs) could replace conventional capacitors for AC line-frequency filtering and other capacitor applications. The development of such HF-ECs is hindered by their typically low capacitance density and operation voltage. Herein, by treating ZIF-67 particulate films in CH 4 /H 2 plasma, edge-oriented graphene (EOG) formed around the carbonized ZIF-67 particulate skeleton, and this EOG was coupled with carbon nanotubes (CNTs) that were grown with the aid of Co catalyst nanoparticles, which were generated by reducing the Co 2+ ions associated with ZIF in the plasma. Used as electrodes, these EOG/CNT/carbonized ZIF-67 composites exhibited a large electrode areal capacitance of 1.0 mF cm −2 and an excellent frequency response of −84° phase angle at 120 Hz in aqueous electrolyte cells, whereas values of 0.67 mF cm −2 and −78° for the electrode areal capacitance and the phase angle at 120 Hz, respectively, were obtained in organic electrolyte cells with the operation voltage of 2.5 V. Using three pairs of electrodes stacked together, a single integrated cell operating at 7.5 V and having a characteristic frequency of ∼3.8 kHz at −45° phase angle, was demonstrated. These results suggest the potential to use this EOG/CNT/carbonized ZIF-67 composite structure for developing HF-ECs. 

ABSTRACT Compact-size kilohertz (kHz) AC-supercapacitors are being pursued for ripple current filtering and pulsed energy storage. However, their development is limited by a small areal capacitance density due to very thin electrode used for meeting frequency requirement. In our work, crosslinked carbon nanofiber aerogel (CCNFA) was investigated as freestanding electrode for kHz AC-supercapacitors with an areal capacitance density as large as 4.5 mF cm -2 at 120 Hz, 5-10 times larger than most reports. The CCNFA was obtained in a rapid plasma carbonization process of bacterial cellulose. The fabrication route adopted here is simple and straightforward, and the produced CCNFA electrode was found to be very suitable for high-frequency AC-supercapacitors. The operating voltage range of CCNFA based AC-supercapacitors can be expanded to 3 V by utilizing an organic electrolyte. In addition to AC-Supercapacitor performance, the morphology and material properties of bacterial cellulose aerogel and CCNFA were also reported.