Electrochemical capacitors (i.e. supercapacitors) include electrochemical double-layer capacitors that depend on the charge storage of ion adsorption and pseudo-capacitors that are based on charge storage involving fast surface redox reactions. The energy storage capacities of supercapacitors are several orders of magnitude higher than those of conventional dielectric capacitors, but are much lower than those of secondary batteries. They typically have high power density, long cyclic stability and high safety, and thus can be considered as an alternative or complement to rechargeable batteries in applications that require high power delivery or fast energy harvesting. This article reviews the latest progress in supercapacitors in charge storage mechanisms, electrode materials, electrolyte materials, systems, characterization methods, and applications. In particular, the newly developed charge storage mechanism for intercalative pseudocapacitive behaviour, which bridges the gap between battery behaviour and conventional pseudocapacitive behaviour, is also clarified for comparison. Finally, the prospects and challenges associated with supercapacitors in practical applications are also discussed.

Electrochemical capacitors: mechanism, materials, systems, characterization and applications

Electrospinning is a versatile and viable technique for generating ultrathin fibers. Remarkable progress has been made with regard to the development of electrospinning methods and engineering of electrospun nanofibers to suit or enable various applications. We aim to provide a comprehensive overview of electrospinning, including the principle, methods, materials, and applications. We begin with a brief introduction to the early history of electrospinning, followed by discussion of its principle and typical apparatus. We then discuss its renaissance over the past two decades as a powerful technology for the production of nanofibers with diversified compositions, structures, and properties. Afterward, we discuss the applications of electrospun nanofibers, including their use as "smart" mats, filtration membranes, catalytic supports, energy harvesting/conversion/storage components, and photonic and electronic devices, as well as biomedical scaffolds. We highlight the most relevant and recent advances related to the applications of electrospun nanofibers by focusing on the most representative examples. We also offer perspectives on the challenges, opportunities, and new directions for future development. At the end, we discuss approaches to the scale-up production of electrospun nanofibers and briefly discuss various types of commercial products based on electrospun nanofibers that have found widespread use in our everyday life.

Electrospinning and Electrospun Nanofibers: Methods, Materials, and Applications

Due to their high energy density and low material cost, lithium–sulfur batteries represent a promising energy storage system for a multitude of emerging applications, ranging from stationary grid storage to mobile electric vehicles. This review aims to summarize major developments in the field of lithium–sulfur batteries, starting from an overview of their electrochemistry, technical challenges and potential solutions, along with some theoretical calculation results to advance our understanding of the material interactions involved. Next, we examine the most extensively-used design strategy: encapsulation of sulfur cathodes in carbon host materials. Other emerging host materials, such as polymeric and inorganic materials, are discussed as well. This is followed by a survey of novel battery configurations, including the use of lithium sulfide cathodes and lithium polysulfide catholytes, as well as recent burgeoning efforts in the modification of separators and protection of lithium metal anodes. Finally, we conclude with an outlook section to offer some insight on the future directions and prospects of lithium–sulfur batteries.

Designing high-energy lithium–sulfur batteries

Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable electronics, and to mitigate environmental problems. However, the application of Li–S batteries is challenged by several obstacles, including their short life and low sulfur utilization, which become more serious when sulfur loading is increased to the practically accepted level above 3–5 mg cm−2. More and more efforts have been made recently to overcome the barriers toward commercially viable Li–S batteries with a high sulfur loading. This review highlights the recent progress in high-sulfur-loading Li–S batteries enabled by hierarchical design principles at multiscale. Particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are under specific concerns. Hierarchy in the multiscale design is proposed to guide the future development of high-sulfur-loading Li–S batteries.

Review on High-Loading and High-Energy Lithium–Sulfur Batteries

Lithium-sulfur (Li-S) batteries have attracted tremendous interest because of their high theoretical energy density and cost effectiveness. The target of Li-S battery research is to produce batteries with a high useful energy density that at least outperforms state-of-the-art lithium-ion batteries. However, due to an intrinsic gap between fundamental research and practical applications, the outstanding electrochemical results obtained in most Li-S battery studies indeed correspond to low useful energy densities and are not really suitable for practical requirements. The Li-S battery is a complex device and its useful energy density is determined by a number of design parameters, most of which are often ignored, leading to the failure to meet commercial requirements. The purpose of this review is to discuss how to pave the way for reliable Li-S batteries. First, the current research status of Li-S batteries is briefly reviewed based on statistical information obtained from literature. This includes an analysis of how the various parameters influence the useful energy density and a summary of existing problems in the current Li-S battery research. Possible solutions and some concerns regarding the construction of reliable Li-S batteries are comprehensively discussed. Finally, insights are offered on the future directions and prospects in Li-S battery field.

More Reliable Lithium-Sulfur Batteries: Status, Solutions and Prospects.

Owing to the overwhelming advantage in energy density, lithium-sulfur (Li-S) battery is a promising next-generation electrochemical energy storage system. Despite many efforts in pursuing long cycle life, relatively little emphasis has been placed on increasing the areal energy density. Herein, we have designed and developed a 'pie' structured electrode, which provides an excellent balance between gravimetric and areal energy densities. Combining lotus root-like multichannel carbon nanofibers 'filling' and amino-functionalized graphene 'crust', the free-standing paper electrode (S mass loading: 3.6 mg cm(-2)) delivers high specific capacity of 1,314 mAh g(-1) (4.7 mAh cm(-2)) at 0.1 C (0.6 mA cm(-2)) accompanied with good cycling stability. Moreover, the areal capacity can be further boosted to more than 8 mAh cm(-2) by stacking three layers of paper electrodes with S mass loading of 10.8 mg cm(-2).

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Pie-like electrode design for high-energy density lithium–sulfur batteries

Hierarchical tubular structures composed of Co3O4 hollow nanoparticles and carbon nanotubes (CNTs) have been synthesized by an efficient multi-step route. Starting from polymer-cobalt acetate (Co(Ac)2) composite nanofibers, uniform polymer-Co(Ac)2@zeolitic imidazolate framework-67 (ZIF-67) core–shell nanofibers are first synthesized via partial phase transformation with 2-methylimidazole in ethanol. After the selective dissolution of polymer-Co(Ac)2 cores, the resulting ZIF-67 tubular structures can be converted into hierarchical CNTs/Co-carbon hybrids by annealing in Ar/H2 atmosphere. Finally, the hierarchical CNT/Co3O4 microtubes are obtained by a subsequent thermal treatment in air. Impressively, the as-prepared nanocomposite delivers a high reversible capacity of 1281 mAh g−1 at 0.1 A g−1 with exceptional rate capability and long cycle life over 200 cycles as an anode material for lithium-ion batteries.

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Hierarchical Tubular Structures Composed of Co3O4 Hollow Nanoparticles and Carbon Nanotubes for Lithium Storage

Molybdenum disulfide (MoS2), a typical two-dimensional material, is a promising anode material for lithium-ion batteries because it has three times the theoretical capacity of graphite. The main challenges associated with MoS2 anodes are the structural degradation and the low rate capability caused by the low intrinsic electric conductivity and large strain upon cycling. Here, we design hierarchical MoS2 tubular structures internally wired by carbon nanotubes (CNTs) to tackle these problems. These porous MoS2 tubular structures are constructed from building blocks of ultrathin nanosheets, which are believed to benefit the electrochemical reactions. Benefiting from the unique structural and compositional characteristics, these CNT-wired MoS2 tubular structures deliver a very high specific capacity of ~1320 mAh g−1 at a current density of 0.1 A g−1, exceptional rate capability, and an ultralong cycle life of up to 1000 cycles. This work may inspire new ideas for constructing high-performance electrodes for electrochemical energy storage.

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Hierarchical MoS2 tubular structures internally wired by carbon nanotubes as a highly stable anode material for lithium-ion batteries

A simple and versatile method for general synthesis of uniform one-dimensional (1D) MxCo3−xS4 (M=Ni, Mn, Zn) hollow tubular structures (HTSs), using soft polymeric nanofibers as a template, is described. Fibrous core–shell polymer@M-Co acetate hydroxide precursors with a controllable molar ratio of M/Co are first prepared, followed by a sulfidation process to obtain core–shell polymer@MxCo3−xS4 composite nanofibers. The as-made MxCo3−xS4 HTSs have a high surface area and exhibit exceptional electrochemical performance as electrode materials for hybrid supercapacitors. For example, the MnCo2S4 HTS electrode can deliver specific capacitance of 1094 F g−1 at 10 A g−1, and the cycling stability is remarkable, with only about 6 % loss over 20 000 cycles.

Yu Ming Chen

Papers

Pie-like electrode design for high-energy density lithium–sulfur batteries

Hierarchical Tubular Structures Composed of Co3O4 Hollow Nanoparticles and Carbon Nanotubes for Lithium Storage

Hierarchical MoS2 tubular structures internally wired by carbon nanotubes as a highly stable anode material for lithium-ion batteries

General Formation of MxCo3−xS4 (M=Ni, Mn, Zn) Hollow Tubular Structures for Hybrid Supercapacitors