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

Paper-based supercapacitors (SCs), a novel and interesting group of flexible energy storage devices, are attracting more and more attention from both industry and academia. Cellulose papers with a unique porous bulk structure and rough and absorptive surface properties enable the construction of paper-based SCs with a reasonably good performance at a low price. The inexpensive and environmentally friendly nature of paper as well as simple fabrication techniques make paper-based SCs promising candidates for the future ‘green’ and ‘once-use-and-throw-away’ electronics. This review introduces the design, fabrication and applications of paper-based SCs, giving a comprehensive coverage of this interesting field. Challenges and future perspectives are also discussed.

Flexible supercapacitors based on paper substrates: a new paradigm for low-cost energy storage.

ConspectusThe rational design and exploration of electrochromic devices will find a wide range of applications in smart windows for energy-efficient buildings, low-power displays, self-dimming rear mirrors for automobiles, electrochromic e-skins, and so on. Electrochromic devices generally consist of multilayer structures with transparent conductors, electrochromic films, ion conductors, and ion storage films. Synthetic strategies and new materials for electrochromic films and transparent conductors, comprehensive electrochemical kinetic analysis, and novel device design are areas of active study worldwide. These are believed to be the key factors that will help to significantly improve the electrochromic performance and extend their application areas.In this Account, we present our strategies to design and fabricate electrochromic devices with high performance and multifunctionality. We first describe the synthetic strategies, in which a porous tungsten oxide (WO3) film with nearly ideal optical modulati...

Next-Generation Multifunctional Electrochromic Devices

Stretchable and wearable WO3 electrochromic devices on silver nanowire (AgNW) elastic conductors are reported. The stretchable devices are mechanically robust and can be stretched, twisted, folded, and crumpled without performance failure. Fast coloration (1 s) and bleaching (4 s) time and good cyclic stability (81% retention after 100 cycles) were achieved at relaxed state. Proper functioning at stretched state (50% strain) was also demonstrated. The electrochromic devices were successfully implanted onto textile substrates for potential wearable applications. As most existing electrochromic devices are based on rigid technologies, the innovative devices in their soft form hold the promise for next-generation electronics such as stretchable, wearable, and implantable display applications.

Stretchable and Wearable Electrochromic Devices

Printed electrochromic flexible films were obtained by combining transparent silver grid electrodes formed by self-assembly and inkjet printed WO3 nanoparticles. Concentrated dispersions of WO3 nanoparticles were inkjet printed on transparent plastic silver grid electrodes with a high transparency of 83% in the spectral range of 400–800 nm, and a low sheet resistance in the range of 1–5 Ω sq−1. These electrodes were used for electrochromic applications for the first time. The resultant patterned nanostructured electrochromic films maintained their coloring and bleaching performance after bending of the flexible films.

Nanostructured electrochromic films by inkjet printing on large area and flexible transparent silver electrodes.

Micro-supercapacitors have attracted considerable attention due to their feasibility as power supplies for future integration into autonomous and portable devices. However, the conventional lab-on-chip fabrication method requires multiple patterning and metallization procedures, while the rigid substrate restricts versatility in applications such as flexible and wearable electronics. Here, we report the low cost, facile and scalable fabrication process of an all solid state flexible micro-supercapacitor on commercially available photo paper for the first time. Three dimensional interconnected coral-like polyaniline–manganese oxide composite material is electrochemically deposited on the interdigital finger electrodes. Electrochemical measurements reveal that the high aspect ratio finger electrode pattern and small gap interdigital finger electrode design is crucial to ensure superior performance. The optimized device shows an ultra high areal energy density of 6.3 μW h cm−2 at a power density of 35 μW cm−2 (94.73 mF cm−2 at 0.1 mA cm−2), while it maintains 4.8 μW h cm−2 at a power density of 3500 μW cm−2 (71.43 mF cm−2 at 10.0 mA cm−2). Meanwhile, it also has good flexibility. Such a flexible micro-supercapacitor is promising for future applications in lightweight, wearable or foldable electronics.

Wan Ling Foo

Papers

Nanostructured electrochromic films by inkjet printing on large area and flexible transparent silver electrodes.

Rational design of a high performance all solid state flexible micro-supercapacitor on paper