Electrochemical Supercapacitors: From Mechanism Understanding to Multifunctional Applications

The intercalation of ions into layered compounds has long been exploited in energy storage devices such as batteries and electrochemical capacitors. However, few host materials are known for ions much larger than lithium. We demonstrate the spontaneous intercalation of cations from aqueous salt solutions between two-dimensional (2D) Ti3C2 MXene layers. MXenes combine 2D conductive carbide layers with a hydrophilic, primarily hydroxyl-terminated surface. A variety of cations, including Na(+), K(+), NH4(+), Mg(2+), and Al(3+), can also be intercalated electrochemically, offering capacitance in excess of 300 farads per cubic centimeter (much higher than that of porous carbons). This study provides a basis for exploring a large family of 2D carbides and carbonitrides in electrochemical energy storage applications using single- and multivalent ions.

A comprehensive overview of the state-of-the-art progress toward mechanisms, new materials, and novel device designs for supercapacitors is provided. Further directions are also pointed out. 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, LaMnO 3 , and RbAg 4 I 5 /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.

In recent years, much effort have been dedicated to achieve thin, lightweight and even flexible energy-storage devices for wearable electronics. Here we demonstrate a novel kind of ultrathin all-solid-state supercapacitor configuration with an extremely simple process using two slightly separated polyaniline-based electrodes well solidified in the H(2)SO(4)-polyvinyl alcohol gel electrolyte. The thickness of the entire device is much comparable to that of a piece of commercial standard A4 print paper. Under its highly flexible (twisting) state, the integrate device shows a high specific capacitance of 350 F/g for the electrode materials, well cycle stability after 1000 cycles and a leakage current of as small as 17.2 μA. Furthermore, due to its polymer-based component structure, it has a specific capacitance of as high as 31.4 F/g for the entire device, which is more than 6 times that of current high-level commercial supercapacitor products. These highly flexible and all-solid-state paperlike polymer supercapacitors may bring new design opportunities of device configuration for energy-storage devices in the future wearable electronic area.