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, and RbAgI/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.

Flexible all‐solid‐state supercapacitors and in‐plane microsupercapacitors based on MXene and exfoliated graphene are fabricated with ultrahigh volumetric capacitances.

An aqueous rechargeable Zn//Co3 O4 battery is demonstrated with Zn@carbon fibers and Co3 O4 @Ni foam as the negative and positive electrodes, respectively, using an electrolyte of 1 m KOH and 10 × 10(-3) m Zn(Ac)2 . It can operate at a cell voltage as high as 1.78 V with an energy density of 241 W h kg(-1) and presents excellent cycling. The battery is also assembled into a flexible shape, which can be applied in flexible or wearable devices requiring high energy.

Two‐dimensional (2D) titanium carbide (Ti3C2) is emerging as an important member of the MXene family. However, fluoride‐based synthetic procedures remain an impediment to the practical applications of this promising class of materials. Here we demonstrate an efficient fluoride‐free etching method based on the anodic corrosion of titanium aluminium carbide (Ti3AlC2) in a binary aqueous electrolyte. The dissolution of aluminium followed by in situ intercalation of ammonium hydroxide results in the extraction of carbide flakes (Ti3C2Tx, T=O, OH) with sizes up to 18.6 μm and high yield (over 90 %) of mono‐ and bilayers. All‐solid‐state supercapacitor based on exfoliated sheets exhibits high areal and volumetric capacitances of 220 mF cm−2 and 439 F cm−3, respectively, at a scan rate of 10 mV s−1, superior to those of LiF/HCl‐etched MXenes. Our strategy paves a safe way to the scalable synthesis and application of MXene materials.