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

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

Volumetric performance, a much more reliable and precise parameter for evaluating the charge-storage capacity of supercapacitors compared with gravimetric performance, has aroused more and more interest in recent years owing to the rapid development of miniaturized, portable and wearable electronic devices as well as electric vehicles. Various carbon materials are widely used as electrode materials in supercapacitors. However, their intrinsically low specific capacitance and relatively low bulk density lead to a relatively low volumetric performance, significantly limiting their future application. This critical review points out the crucial importance of volumetric performance and reviews recent achievements of high volumetric performances obtained through the rational design and development of novel carbon-based materials. Particular emphasis is focused on discussing the factors influencing the volumetric performance of carbon materials from a structural design point of view. We then make an in-depth summary of various promising approaches used to make significant research breakthroughs in recent years. Current challenges, future research directions and opportunities in this fascinating field of supercapacitors with high gravimetric and volumetric performances are also discussed.

Carbon materials for high volumetric performance supercapacitors: design, progress, challenges and opportunities

The demand for flexible/wearable electronic devices that have aesthetic appeal and multi-functionality has stimulated the rapid development of flexible supercapacitors with enhanced electrochemical performance and mechanical flexibility. After a brief introduction to flexible supercapacitors, we summarize current progress made with graphene-based electrodes. Two recently proposed prototypes for flexible supercapacitors, known as micro-supercapacitors and fiber-type supercapacitors, are then discussed. We also present our perspective on the development of graphene-based electrodes for flexible supercapacitors.

Graphene-based materials for flexible supercapacitors

Advances in wireless technologies, low-power electronics, the internet of things, and in the domain of connected health are driving innovations in wearable medical devices at a tremendous pace. Wearable sensor systems composed of flexible and stretchable materials have the potential to better interface to the human skin, whereas silicon-based electronics are extremely efficient in sensor data processing and transmission. Therefore, flexible and stretchable sensors combined with low-power silicon-based electronics are a viable and efficient approach for medical monitoring. Flexible medical devices designed for monitoring human vital signs, such as body temperature, heart rate, respiration rate, blood pressure, pulse oxygenation, and blood glucose have applications in both fitness monitoring and medical diagnostics. As a review of the latest development in flexible and wearable human vitals sensors, the essential components required for vitals sensors are outlined and discussed here, including the reported sensor systems, sensing mechanisms, sensor fabrication, power, and data processing requirements.

Monitoring of Vital Signs with Flexible and Wearable Medical Devices

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

A layered architecture endows structural materials like nacre and biomimetic ceramics with enhanced mechanical performance because it introduces multiple strengthening and toughening mechanisms. Yet present studies predominantly involve enhancing the alignment in planar lamellar structures, and the effects of the stacking curvature have largely remained unexplored. Here we find that ordered curved stacking bands in lamellar structures act as a new structural mechanism to simultaneously improve strength and toughness. Aligned curved bands increase interlayer frictional resistance to show a strengthening effect and suppress the crack propagation to show an extrinsic toughening effect. In prototypical graphene oxide films, rational regulation of the intervals and orientations of curved bands bring a maximum 162% improvement in strength and 183% improvement in toughness simultaneously. Our results reveal the hidden effects of the stacking curvature on the mechanical behaviors of lamellar materials, opening an extra design dimension to fabricate stronger and tougher structural materials.

Yi Han

Papers

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

Aligning curved stacking bands to simultaneously strengthen and toughen lamellar materials.

Mode-Coupling Generation Using ITO Nanodisk Arrays with Au Substrate Enabling Narrow-Band Biosensing