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Many transition-metal-oxide-based catalysts have been investigated to chemically bind soluble lithium polysulfides and accelerate their redox kinetics in lithium-sulfur (Li-S) battery chemistry. However, the intrinsic poor electrical conductivities of these oxides restrict their catalytic performance, consequently limiting the sulfur utilization and the rate performance of Li-S batteries. Herein, we report a freestanding electrocatalytic sulfur host consisting of hydrogen-treated VO2 nanoparticles (H-VO2) anchored on nitrogen-doped carbonized bacterial cellulose aerogels (N-CBC). The hydrogen treatment enables the formation and stabilization of the rutile VO2(R) phase with metallic conductivity at room temperature, significantly enhancing its catalytic capability compared to the as-synthesized insulative VO2(M) phase. Several measurements characterize the electrocatalytic performance of this unique H-VO2@N-CBC structure. In particular, the two kinetic barriers between S8, polysulfides, and Li2S are largely reduced by 28.2 and 43.3 kJ/mol, respectively. Accordingly, the Li-S battery performance, in terms of sulfur utilization and charge/discharge rate, is greatly improved. This work suggests an effective strategy to develop conductive catalysts based on a typical transition metal oxide (VO2) for Li-S batteries. 

An ultra‐fast electrochemical capacitor (EC) designed for efficient ripple current smoothing was fabricated using vertically oriented MoS₂(VOM) nanoflakes deposited on freestanding carbonized cellulose (CC) sheets as electrodes. The daily used cellulose tissue sheets were transformed into electrode scaffolds through a rapid pyrolysis process within a preheated furnace, on which VOM nanoflakes were formed in a conventional hydrothermal process. With these ~10 μm thick VOM‐CC electrodes, ultrafast ECs with tunable frequency response and specific capacitance density were fabricated. The ECs with a cell‐level areal capacitance density of 0.8 mF/cm²at 120 Hz were demonstrated for ripple current filtering from 60 Hz to 60 kHz. At a lower frequency response level, EC cell with a large capacitance density of 4.8 mF/cm²was also demonstrated. With the facile and easily scaled up process to producing the nanostructured electrode, the miniaturized VOM‐CC based ECs have the potential to substitute the bulky aluminum electrolytic capacitors for current smoothing and pulse power applications.

 

Polysulfide shuttle effect, causing extremely low Coulombic efficiency and cycling stability, is one of the toughest challenges hindering the development of practical lithium sulfur batteries (LSBs). Introducing catalytic nanostructures to stabilize the otherwise soluble polysulfides and promote their conversion to solids has been proved to be an effective strategy in attacking this problem, but the heavy mass of catalysts often results in a low specific energy of the whole electrode. Herein, by designing and synthesizing a free-standing edge-oriented NiCo 2 S 4 /vertical graphene functionalized carbon nanofiber (NCS/EOG/CNF) thin film as a catalytic overlayer incorporated in the sulfur cathode, the polysulfide shuttle effect is largely alleviated, revealed by the enhanced electrochemical performance measurements and the catalytic function demonstration. Different from other reports, the NiCo 2 S 4 nanosheets synthesized here have a 3-D edge-oriented structure with fully exposed edges and easily accessible in-plane surfaces, thus providing a high density of active sites even with a small mass. The EOG/CNF scaffold further renders the high conductivity in the catalytic structure. Combined, this novel structure, with high sulfur loading and high sulfur fraction, leads to high-performance sulfur cathodes toward a practical LSB technology. 

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.