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The world is recently witnessing an explosive development of novel electronic and optoelectronic devices that demand more-reliable power sources that combine higher energy density and longer-term durability. Supercapacitors have become one of the most promising energy-storage systems, as they present multifold advantages of high power density, fast charging-discharging, and long cyclic stability. However, the intrinsically low energy density inherent to traditional supercapacitors severely limits their widespread applications, triggering researchers to explore new types of supercapacitors with improved performance. Asymmetric supercapacitors (ASCs) assembled using two dissimilar electrode materials offer a distinct advantage of wide operational voltage window, and thereby significantly enhance the energy density. Recent progress made in the field of ASCs is critically reviewed, with the main focus on an extensive survey of the materials developed for ASC electrodes, as well as covering the progress made in the fabrication of ASC devices over the last few decades. Current challenges and a future outlook of the field of ASCs are also discussed.

Supercapacitors represent a major technology to store energy for many applications including electronics, automobiles, military, and space. Despite their high power density, the energy density in supercapacitors is presently inferior to that of the state-ofthe-art Li-ion batteries owing to the limited electrochemical performance exhibited by the conventional electrode materials. The advent of two-dimensional (2D) nanomaterials has spurred enormous research interest as supercapacitor electrode materials due to their fascinating electrochemical and mechanical properties. This Review discusses cutting-edge research on some of the key 2D supercapacitor electrode materials including transition metal dichalcogenides, transition metal oxides and hydroxides, MXenes, and phosphorene. Various synthetic approaches, novel electrode designs, and microstructure tuning of these 2D materials for achieving high energy and power densities are discussed.

Two-dimensional (2D) transition-metal dichalcogenides (TMDs) have emerged as promising capacitive materials for supercapacitor devices owing to their intrinsically layered structure and large surface areas. Hierarchically integrating 2D TMDs with other functional nanomaterials has recently been pursued to improve electrochemical performances; however, it often suffers from limited cyclic stabilities and capacitance losses due to the poor structural integrity at the interfaces of randomly assembled materials. Here, we report high-performance core/shell nanowire supercapacitors based on an array of one-dimensional (1D) nanowires seamlessly integrated with conformal 2D TMD layers. The 1D and 2D supercapacitor components possess "one-body" geometry with atomically sharp and structurally robust core/shell interfaces, as they were spontaneously converted from identical metal current collectors via sequential oxidation/sulfurization. These hybrid supercapacitors outperform previously developed any stand-alone 2D TMD-based supercapacitors; particularly, exhibiting an exceptional charge-discharge retention over 30,000 cycles owing to their structural robustness, suggesting great potential for unconventional energy storage technologies.

Two-dimensional MoS2 is a promising material for next-generation electronic and optoelectronic devices due to its unique electrical and optical properties including the band gap modulation with film thickness. Although MoS2 has shown excellent properties, wafer-scale production with layer control from single to few layers has yet to be demonstrated. The present study explored the large-scale and thickness-modulated growth of atomically thin MoS2 on Si/SiO2 substrates using a two-step sputtering-CVD method. Our process exhibited wafer-scale fabrication and successful thickness modulation of MoS2 layers from monolayer (0.72 nm) to multilayer (12.69 nm) with high uniformity. Electrical measurements on MoS2 field effect transistors (FETs) revealed a p-type semiconductor behavior with much higher field effect mobility and current on/off ratio as compared to previously reported CVD grown MoS2-FETs and amorphous silicon (a-Si) thin film transistors. Our results show that sputter-CVD is a viable method to synthesize large-area, high-quality, and layer-controlled MoS2 that can be adapted in conventional Si-based microfabrication technology and future flexible, high-temperature, and radiation hard electronics/optoelectronics.