International audienceSupercapacitors are electrochemical energy storage devices that operate on the simple mechanism of adsorption of ions from an electrolyte on a high-surface-area electrode. Over the past decade, the performance of supercapacitors has greatly improved, as electrode materials have been tuned at the nanoscale and electrolytes have gained an active role, enabling more efficient storage mechanisms. In porous carbon materials with subnanometre pores, the desolvation of the ions leads to surprisingly high capacitances. Oxide materials store charge by surface redox reactions, leading to the pseudocapacitive effect. Understanding the physical mechanisms underlying charge storage in these materials is important for further development of supercapacitors. Here we review recent progress, from both in situ experiments and advanced simulation techniques, in understanding the charge storage mechanism in carbon- and oxide-based supercapacitors. We also discuss the challenges that still need to be addressed for building better supercapacitors

Nanoscience and nanotechnology can provide tremendous benefits to electrochemical energy storage devices, such as batteries and supercapacitors, by combining new nanoscale properties to realize enhanced energy and power capabilities. A number of published reports on hybrid systems are systematically reviewed in this perspective. Several potential strategies to enhance the energy density above that of generation-I electric double layer capacitors (EDLC: activated carbon/activated carbon) are discussed and some fundamental issues and future directions are identified. We suggest a new hybrid supercapacitor system that is able to meet the energy and power demands for a variety of applications, ranging from microelectronic devices to electrical vehicles, which presents itself as a breakthrough improvement. Two practical hybrid supercapacitor systems, namely, a lithium-ion capacitor (LIC: graphite/activated carbon) and a nanohybrid capacitor (NHC: (nc-Li 4 Ti 5 O 12 /CNF composite)/activated carbon), are featured and compared. The proposed NHC can pave the way toward generation-II supercapacitor systems by taking advantage of a novel, high quality, high efficiency and inexpensive nanomaterial preparation procedure. With such a breakthrough in nanofabrication-nanohybridization technology, the NHC, which utilizes an ultrafast nano-crystalline Li 4 Ti 5 O 12 , is considered to be an alternative for conventional generation-I EDLCs.

To meet growing demands for electric automotive and regenerative energy storage applications, researchers all over the world have sought to increase the energy density of electrochemical capacitors. Hybridizing battery-capacitor electrodes can overcome the energy density limitation of the conventional electrochemical capacitors because they employ both the system of a battery-like (redox) and a capacitor-like (double-layer) electrode, producing a larger working voltage and capacitance. However, to balance such asymmetric systems, the rates for the redox portion must be substantially increased to the levels of double-layer process, which presents a significant challenge. An in situ material processing technology called "ultracentrifuging (UC) treatment" has been used to prepare a novel ultrafast Li4Ti5O12 (LTO) nanocrystal electrode for capacitive energy storage. This Account describes an extremely high-performance supercapacitor that utilizes highly optimized "nano-nano-LTO/carbon composites" prepared via the UC treatment. The UC-treated LTO nanocrystals are grown as either nanosheets or nanoparticles, and both have hyperlinks to two types of nanocarbons: carbon nanofibers and supergrowth (single-walled) carbon nanotubes. The spinel structured LTO has been prepared with two types of hyperdispersed carbons. The UC treatment at 75 000G stoichiometrically accelerates the in situ sol-gel reaction (hydrolysis followed by polycondensation) and further forms, anchors, and grafts the nanoscale LTO precursors onto the carbon matrices. The mechanochemical sol-gel reaction is followed by a short heat-treatment process in vacuo. This immediate treatment with heat is very important for achieving optimal crystallization, inhibiting oxidative decomposition of carbon matrices, and suppressing agglomeration. Such nanocrystal composites can store and deliver energy at the highest rate attained to this date. The charge-discharge profiles indicate a very high sustained capacity of 80 mAh g(-1) at an extremely high rate of 1200 C. Using this ultrafast material, we assembled a hybrid device called a "nanohybrid capacitor" that consists of a Faradaic Li-intercalating LTO electrode and a non-Faradaic AC electrode employing an anion (typically BF4(-)) adsorption-desorption process. The "nanohybrid capacitor" cell has demonstrated remarkable energy, power, and cycleability performance as an electrochemical capacitor electrode. It also exhibits the same ion adsorption-desorption process rates as those of standard activated carbon electrodes in electrochemical capacitors. The new-generation "nanohybrid capacitor" technology produced more than triple the energy density of a conventional electrochemical capacitor. Moreover, the synthetic simplicity of the high-performance nanostructures makes it possible to scale them up for large-volume material production and further applications in many other electrochemical energy storage devices.

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Supercapacitors, also known as electrochemical capacitors, have witnessed a fast evolution in the recent years, but challenges remain. This review covers the fundamentals and state-of-the-art developments of supercapacitors. Conventional and novel electrode materials, including high surface area porous carbons for electrical double layer capacitors (EDLCs) and transition metal oxides, carbides, nitrides and their various nanocomposites for pseudocapacitors -are described. Latest characterization techniques help to better understand the charge storage mechanisms in such supercapacitors and recognize their current limitations, while recently proposed synthesis approaches enable various breakthroughs in this field.