Safe and powerful energy storage devices are becoming increasingly important. Charging times of seconds to minutes, with power densities exceeding those of batteries, can in principle be provided by electrochemical capacitors--in particular, pseudocapacitors. Recent research has focused mainly on improving the gravimetric performance of the electrodes of such systems, but for portable electronics and vehicles volume is at a premium. The best volumetric capacitances of carbon-based electrodes are around 300 farads per cubic centimetre; hydrated ruthenium oxide can reach capacitances of 1,000 to 1,500 farads per cubic centimetre with great cyclability, but only in thin films. Recently, electrodes made of two-dimensional titanium carbide (Ti3C2, a member of the 'MXene' family), produced by etching aluminium from titanium aluminium carbide (Ti3AlC2, a 'MAX' phase) in concentrated hydrofluoric acid, have been shown to have volumetric capacitances of over 300 farads per cubic centimetre. Here we report a method of producing this material using a solution of lithium fluoride and hydrochloric acid. The resulting hydrophilic material swells in volume when hydrated, and can be shaped like clay and dried into a highly conductive solid or rolled into films tens of micrometres thick. Additive-free films of this titanium carbide 'clay' have volumetric capacitances of up to 900 farads per cubic centimetre, with excellent cyclability and rate performances. This capacitance is almost twice that of our previous report, and our synthetic method also offers a much faster route to film production as well as the avoidance of handling hazardous concentrated hydrofluoric acid.
Ultra-high-rate pseudocapacitive energy storage in twodimensional transition metal carbides. (2017) Nature Energy, 2 (8). 1-12.
Free-standing and flexible sandwich-like MXene/carbon nanotube (CNT) paper, composed of alternating MXene and CNT layers, is fabricated using a simple filtration method. These sandwich-like papers exhibit high volumetric capacitances, good rate performances, and excellent cycling stability when employed as electrodes in supercapacitors.
The scalable and sustainable manufacture of thick electrode films with high energy and power densities is critical for the large-scale storage of electrochemical energy for application in transportation and stationary electric grids. Two-dimensional nanomaterials have become the predominant choice of electrode material in the pursuit of high energy and power densities owing to their large surface-area-to-volume ratios and lack of solid-state diffusion. However, traditional electrode fabrication methods often lead to restacking of two-dimensional nanomaterials, which limits ion transport in thick films and results in systems in which the electrochemical performance is highly dependent on the thickness of the film. Strategies for facilitating ion transport-such as increasing the interlayer spacing by intercalation or introducing film porosity by designing nanoarchitectures-result in materials with low volumetric energy storage as well as complex and lengthy ion transport paths that impede performance at high charge-discharge rates. Vertical alignment of two-dimensional flakes enables directional ion transport that can lead to thickness-independent electrochemical performances in thick films. However, so far only limited success has been reported, and the mitigation of performance losses remains a major challenge when working with films of two-dimensional nanomaterials with thicknesses that are near to or exceed the industrial standard of 100 micrometres. Here we demonstrate electrochemical energy storage that is independent of film thickness for vertically aligned two-dimensional titanium carbide (TiCT ), a material from the MXene family (two-dimensional carbides and nitrides of transition metals (M), where X stands for carbon or nitrogen). The vertical alignment was achieved by mechanical shearing of a discotic lamellar liquid-crystal phase of TiCT . The resulting electrode films show excellent performance that is nearly independent of film thickness up to 200 micrometres, which makes them highly attractive for energy storage applications. Furthermore, the self-assembly approach presented here is scalable and can be extended to other systems that involve directional transport, such as catalysis and filtration.
We report on the synthesis of the first two-dimensional transition metal nitride, Ti4N3-based MXene. In contrast to the previously reported MXene synthesis methods - in which selective etching of a MAX phase precursor occurred in aqueous acidic solutions - here a molten fluoride salt is used to etch Al from a Ti4AlN3 powder precursor at 550 °C under an argon atmosphere. We further delaminated the resulting MXene to produce few-layered nanosheets and monolayers of Ti4N3Tx, where T is a surface termination (F, O, or OH). Density functional theory calculations of bare, non-terminated Ti4N3 and terminated Ti4N3Tx were performed to determine the most energetically stable form of this MXene. Bare and functionalized Ti4N3 are predicted to be metallic. Bare Ti4N3 is expected to show magnetism, which is significantly reduced in the presence of functional groups.
2D Nb2CTx MXene flakes are produced using an amine-assisted delamination process. Upon mixing with carbon nanotubes and filtration, freestanding, flexible paper is produced. The latter exhibits high capacity and excellent stability when used as the electrode for Li-ion batteries and capacitors.
CitationAll-MXene (2D titanium carbide) solid-state microsupercapacitors for on-chip energy storage 2016 Energy Environ. Sci. On-chip energy storage is a rapidly evolving research topic, opening doors for integration of batteries and supercapacitors at microscales on rigid and flexible platforms. Recently, a new class of two-dimensional (2D) transition metal carbides and nitrides (so-called MXenes) has shown great promise in electrochemical energy storage applications. Here, we report the farbication of all-MXene (Ti3C2Tx) solid-state interdigital microsupercapacitors by employing a solution spray-coating, followed by a photoresist-free direct laser cutting method. Our prototype devices consisted of two layes of Ti3C2Tx with two different flake sizes. The bottom layer was stacked large-size MXene flakes (lateral dimensions of 3-6 μm) serving mainly as current collectors. The top layer was made of small-size MXene flakes (~1 μm) with a large number of defects and edges as the electroactive layer responsible for energy storage. Compared to Ti3C2Tx micro-supercapacitors with platinum current collectors, the all-MXene devices exhibited much lower contact resistance, higher capacitances and better rate-capabilities. The areal and volumetric capacitances of ~27 mF cm -2 and ~357 F cm -3 , respectively, at a scan rate of 20 mV s -1 were achieved. The devices also demonstrated their excellent cyclic stability, with 100 % capacitance retention after 10,000 cycles at a scan rate of 50 mV s -1 . This study opens up a plethora of possible designs for high-performance on-chip devices employing different chemistries, flake sizes and morphologies of MXenes and their heterostructures. Eprint version Broader contextThe continuous development and further miniaturization of portable electronic devices and microelectromechanical systems has led to the increasing demands for micro or nanoscale power sources and energy storage units. Supercapacitors, also called electrochemical capacitors, are energy storage devices with long service life and high power densities that can be fully charged and discharged in seconds. Small-scale supercapacitors, or micro-supercapacitors (MSCs), can be integrated with self-powered microscale devices and provide the required power for a long duration of time without maintenance, serving as ideal stand-alone power sources. The intrinsic properties of electrode materials play a crucially important role in the performance of MSCs. Here, a novel MSC is fabricated by employing a new material, two-dimensional titanium carbide (MXene). The MXene MSCs offer long lifetime and higher areal and volumetric capacities compared to most of the previously reported devices. This work opens up a door for the design of on-chip devices with high energy storage capability by employing a large family (~ 20 members) of 2D MXenes and their heterostructures.
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