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.

An asymmetric supercapacitor (ASC) is a supercapacitor based on two different electrode materials. One electrode is based on redox (Faradic) reactions with or without non-faradic reactions, and the other one is mostly based on electric double-layer (non-Faradic or electrostatic) absorption/desportion. Aqueous electrolytes have higher ionic conductivity, larger capacitance and better safety than the organic electrolytes. Herein, some key electrode materials for aqueous ASCs are primarily reviewed, which provide a new direction for power sources to have higher energy density at high power densities, compared with traditional capacitors. Their negative electrode materials include carbonaceous materials (porous carbons, carbon nanotubes and graphene), oxides (V₂O₅ and MoO₃) and their composites, and their positive electrode materials include carbonaceous materials, oxides (RuO₂, MnO₂, MoO₃, V₂O₅, PbO₂, Co₃O₄), Ni(OH)₂, intercalation compounds (LiCoO₂, LiMn₂O₄, Li[NiCoMn]_1/3O₂, NaMnO₂ and KMnO₂). We describe the latest work on these electrode materials, and a particular focus is directed to the fabrication and electrochemical performance of various nanostructured electrode materials and some assembled ASCs. Finally, the future trends and prospects on advanced energy storage materials are suggested.

Aqueous rechargeable zinc‐metal‐based batteries are an attractive alternative to lithium‐ion batteries for grid‐scale energy‐storage systems because of their high specific capacity, low cost, eco‐friendliness, and nonflammability. However, uncontrollable zinc dendrite growth limits the cycle life by piercing the separator, resulting in low zinc utilization in both alkaline and mild/neutral electrolytes. Herein, a polyacrylonitrile coating layer on a zinc anode produced by a simple drop coating approach to address the dendrite issue is reported. The coating layer not only improves the hydrophilicity of the zinc anode but also regulates zinc‐ion transport, consequently facilitating the uniform deposition of zinc ions to avoid dendrite formation. A symmetrical cell with the polymer‐coating‐layer‐modified Zn anode displays dendrite‐free plating/stripping with a long cycle lifespan (>1100 h), much better than that of the bare Zn anode. The modified zinc anode coupled with a Mn‐doped V₂O₅ cathode forms a stable rechargeable full battery. This method is a facile and feasible way to solve the zinc dendrite problem for rechargeable aqueous zinc‐metal batteries, providing a solid basis for application of aqueous rechargeable Zn batteries.