Electrolytes have been identified as some of the most influential components in the performance of electrochemical supercapacitors (ESs), which include: electrical double-layer capacitors, pseudocapacitors and hybrid supercapacitors. This paper reviews recent progress in the research and development of ES electrolytes. The electrolytes are classified into several categories, including: aqueous, organic, ionic liquids, solid-state or quasi-solid-state, as well as redox-active electrolytes. Effects of electrolyte properties on ES performance are discussed in detail. The principles and methods of designing and optimizing electrolytes for ES performance and application are highlighted through a comprehensive analysis of the literature. Interaction among the electrolytes, electro-active materials and inactive components (current collectors, binders, and separators) is discussed. The challenges in producing high-performing electrolytes are analyzed. Several possible research directions to overcome these challenges are proposed for future efforts, with the main aim of improving ESs' energy density without sacrificing existing advantages (e.g., a high power density and a long cycle-life) (507 references).

A review of electrolyte materials and compositions for electrochemical supercapacitors

The science and technology of ultracapacitors are reviewed for a number of electrode materials, including carbon, mixed metal oxides, and conducting polymers. More work has been done using microporous carbons than with the other materials and most of the commercially available devices use carbon electrodes and an organic electrolytes. The energy density of these devices is 3¯5 Wh/kg with a power density of 300¯500 W/kg for high efficiency (90¯95%) charge/discharges. Projections of future developments using carbon indicate that energy densities of 10 Wh/kg or higher are likely with power densities of 1¯2 kW/kg. A key problem in the fabrication of these advanced devices is the bonding of the thin electrodes to a current collector such the contact resistance is less than 0.1 cm2. Special attention is given in the paper to comparing the power density characteristics of ultracapacitors and batteries. The comparisons should be made at the same charge/discharge efficiency.

Ultracapacitors: Why, How, and Where is the Technology

https://cyberleninka.org/article/n/768408.pdf

Mechanical properties of graphene and graphene-based nanocomposites

Notably, many significant breakthroughs for a new generation of supercapacitors have been reported in recent years, related to theoretical understanding, material synthesis and device designs. Herein, we summarize the state-of-the-art progress toward mechanisms, new materials, and novel device designs for supercapacitors. Firstly, fundamental understanding of the mechanism is mainly focused on the relationship between the structural properties of electrode materials and their electrochemical performances based on some in situ characterization techniques and simulations. Secondly, some emerging electrode materials are discussed, including metal–organic frameworks (MOFs), covalent organic frameworks (COFs), MXenes, metal nitrides, black phosphorus, LaMnO3, and RbAg4I5/graphite. Thirdly, the device innovations for the next generation of supercapacitors are provided successively, mainly emphasizing flow supercapacitors, alternating current (AC) line-filtering supercapacitors, redox electrolyte enhanced supercapacitors, metal ion hybrid supercapacitors, micro-supercapacitors (fiber, plane and three-dimensional) and multifunctional supercapacitors including electrochromic supercapacitors, self-healing supercapacitors, piezoelectric supercapacitors, shape-memory supercapacitors, thermal self-protective supercapacitors, thermal self-charging supercapacitors, and photo self-charging supercapacitors. Finally, the future developments and key technical challenges are highlighted regarding further research in this thriving field.

Latest advances in supercapacitors: from new electrode materials to novel device designs.

Flexible solid-state supercapacitors (FSSCs) are frontrunners in energy storage device technology and have attracted extensive attention owing to recent significant breakthroughs in modern wearable electronics In this study, we review the state-of-the-art advancements in FSSCs to provide new insights on mechanisms, emerging electrode materials, flexible gel electrolytes and novel cell designs The review begins with a brief introduction on the fundamental understanding of charge storage mechanisms based on the structural properties of electrode materials The next sections briefly summarise the latest progress in flexible electrodes (ie, freestanding and substrate-supported, including textile, paper, metal foil/wire and polymer-based substrates) and flexible gel electrolytes (ie, aqueous, organic, ionic liquids and redox-active gels) Subsequently, a comprehensive summary of FSSC cell designs introduces some emerging electrode materials, including MXenes, metal nitrides, metal–organic frameworks (MOFs), polyoxometalates (POMs) and black phosphorus Some potential practical applications, such as the development of piezoelectric, photo-, shape-memory, self-healing, electrochromic and integrated sensor-supercapacitors are also discussed The final section highlights current challenges and future perspectives on research in this thriving field

Towards flexible solid-state supercapacitors for smart and wearable electronics

High-energy yarn supercapacitors are desirable for safe and wearable electronics. Here, Kou et al. use a coaxial wet-spinning assembly method to fabricate core-sheath fibres of polymer-wrapped carbon nanomaterials and demonstrate high-performance supercapacitor applications.

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Coaxial wet-spun yarn supercapacitors for high-energy density and safe wearable electronics

Two dimensional MXene materials have demonstrated attractive electrical and electrochemical properties for various applications, particularly in energy storage, benefiting from their intrinsic 2D atomic thick topological structures. However, assembling MXene into macroscopic fibers with regular alignment still remains a huge challenge, inherently due to the insufficient interlaminar interaction between MXene sheets and the lack of well-developed assembling techniques. Herein, we report a wet-spinning assembly strategy for the continuous fabrication of MXene-based fibers through a synergistic effect between graphene oxides liquid crystals and MXene sheets. MXene sheets are orderly aligned between graphene oxides liquid crystalline templates and assembled into hybrid fibers with the highest MXene mass ratio achieving 95 w/w%. An excellent overall fiber electrical conductivity (2.9 × 104 S m−1) and superior volumetric capacitance (586.4 F cm−3) of the integrated fiber-constructed supercapacitor exceeding those of neat reduced graphene fibers were achieved.

MXene/graphene hybrid fibers for high performance flexible supercapacitors

Rechargeable aluminum-ion batteries are promising in high-power density but still face critical challenges of limited lifetime, rate capability, and cathodic capacity. We design a "trihigh tricontinuous" (3H3C) graphene film cathode with features of high quality, orientation, and channeling for local structures (3H) and continuous electron-conducting matrix, ion-diffusion highway, and electroactive mass for the whole electrode (3C). Such a cathode retains high specific capacity of around 120 mAh g-1 at ultrahigh current density of 400 A g-1 (charged in 1.1 s) with 91.7% retention after 250,000 cycles, surpassing all the previous batteries in terms of rate capability and cycle life. The assembled aluminum-graphene battery works well within a wide temperature range of -40 to 120°C with remarkable flexibility bearing 10,000 times of folding, promising for all-climate wearable energy devices. This design opens an avenue for a future super-batteries.

https://advances.sciencemag.org/content/advances/3/12/eaao7233.full.pdf

Ultrafast all-climate aluminum-graphene battery with quarter-million cycle life

A conceptually new defect-free principle is proposed for designing graphene cathode of aluminum-ion battery: the fewer the defects, the better the performances. Developed through scalable approach, defect-free graphene aerogel cathode affords high capacity of 100 mAh g-1 under an ultrahigh rate of 500 C, exceeding defective graphene and previous reports. This defect-free principle can guide us to fabricate better graphene-based electrodes.

Tieqi Huang

Papers

Coaxial wet-spun yarn supercapacitors for high-energy density and safe wearable electronics

MXene/graphene hybrid fibers for high performance flexible supercapacitors

Ultrafast all-climate aluminum-graphene battery with quarter-million cycle life

A Defect‐Free Principle for Advanced Graphene Cathode of Aluminum‐Ion Battery

Direct 3D Printing of Ultralight Graphene Oxide Aerogel Microlattices