There is strong recent interest in ultrathin, flexible, safe energy storage devices to meet the various design and power needs of modern gadgets. To build such fully flexible and robust electrochemical devices, multiple components with specific electrochemical and interfacial properties need to be integrated into single units. Here we show that these basic components, the electrode, separator, and electrolyte, can all be integrated into single contiguous nanocomposite units that can serve as building blocks for a variety of thin mechanically flexible energy storage devices. Nanoporous cellulose paper embedded with aligned carbon nanotube electrode and electrolyte constitutes the basic unit. The units are used to build various flexible supercapacitor, battery, hybrid, and dual-storage battery-in-supercapacitor devices. The thin freestanding nanocomposite paper devices offer complete mechanical flexibility during operation. The supercapacitors operate with electrolytes including aqueous solvents, room temperature ionic liquids, and bioelectrolytes and over record temperature ranges. These easy-to-assemble integrated nanocomposite energy-storage systems could provide unprecedented design ingenuity for a variety of devices operating over a wide range of temperature and environmental conditions. batteries ͉ carbon nanotubes ͉ supercapacitor T here has been recent interest in flexible safe energy devices, based on supercapacitors and batteries, to meet the various requirements of modern gadgets (1-3). Electrochemical energy can be stored in two fundamentally different ways. In a battery, the charge storage is achieved by electron transfer that produces a redox reaction in the electroactive materials (3). In an electric double-layer capacitor, namely the supercapacitor, the chargestorage process is nonFaradic, that is, ideally no electron transfer takes place across the electrode interface, and the storage of electric charge and energy is electrostatic. Because the charging and discharging of such supercapacitors involve no chemical phase and composition changes, such capacitors have a high degree of cyclability. However, in certain supercapacitors based on pseudocapacitance, the essential process can be Faradic, similar to that in a battery. However, an essential fundamental difference from battery behavior arises because, in such systems, the chemical and associated electrode potentials are a continuous function of degree of charge, unlike the thermodynamic behavior of single-phase battery reactants (3). Now, with the demand for efficient power devices to meet the high-power and -energy applications, there seems to be the possibility of an ideal compromise, which combines some of the storage capabilities of batteries and some of the power-discharge characteristics of capacitors in devices capable of storing useful quantities of electricity that can be discharged very quickly. We address here this need to develop new integrated hybrid devices with adaptability in various thin-film as well as bulk applications by using...

There are several advantages of growing carbon nanotubes (CNTs) directly on bulk metals, for example in the formation of robust CNT-metal contacts during growth. Usually, aligned CNTs are grown either by using thin catalyst layers predeposited on substrates or through vapour-phase catalyst delivery. The latter method, although flexible, is unsuitable for growing CNTs directly on metallic substrates. Here we report on the growth of aligned multiwalled CNTs on a metallic alloy, Inconel 600 (Inconel), using vapour-phase catalyst delivery. The CNTs are well anchored to the substrate and show excellent electrical contact with it. These CNT-metal structures were then used to fabricate double-layer capacitors and field-emitter devices, which demonstrated improved performance over previously designed CNT structures. Inconel coatings can also be used to grow CNTs on other metallic substrates. This finding overcomes the substrate limitation for nanotube growth which should assist the development of future CNT-related technologies.

Structural components subject to cyclic stress can succumb to fatigue, causing them to fail at stress levels much lower than if they were under static mechanical loading. However, despite extensive research into the mechanical properties of carbon nanotube structures for more than a decade, data on the fatigue behaviour of such devices have never been reported. We show that under repeated high compressive strains, long, vertically aligned multiwalled nanotubes exhibit viscoelastic behaviour similar to that observed in soft-tissue membranes. Under compressive cyclic loading, the mechanical response of the nanotube arrays shows preconditioning, characteristic viscoelasticity-induced hysteresis, nonlinear elasticity and stress relaxation, and large deformations. Furthermore, no fatigue failure is observed at high strain amplitudes up to half a million cycles. This combination of soft-tissue-like behaviour and outstanding fatigue resistance suggests that properly engineered nanotube structures could mimic artificial tissues, and that their good electrical conductivity could lead to their use as compliant electrical contacts in a variety of applications.

Electrospinning is a versatile process used to prepare micro-and nano-sized fibers from various polymers dissolved in volatile solvents. In this report, cellulose and cellulose-heparin composite fibers are prepared from nonvolatile room temperature ionic liquid (RTIL) solvents by electrospinning. RTILs are extracted from the biopolymer fiber after the fiber formation using a cosolvent. Micron to nanometer sized, branched fibers were obtained from 10% (w/w) concentration of polysaccharide biopolymer in RTIL solution with an applied voltage of 15-20 kV. Cellulose-heparin composite fibers showed anticoagulant activity, demonstrating that the bioactivity of heparin remained unaffected even on exposure to a high voltage involved in electrospinning. IntroductionElectrospinning is a widely used simple technique to prepare micron-to nanometer-sized fibers of various polymers. 1 Electrospun fibers find applications in the making of fiber-reinforced composites, membranes, biosensors, electronic and optical devices, and as enzyme and catalytic supports. 2 The electrospinning technique is useful even in large-scale manufacturing environments such as textile industries. 3 A variety of novel tissue engineering scaffolds have been prepared by electrospinning various synthetic and natural biodegradable polymers. 4 However, the range of the polymers that can be electrospun is still limited by the availability of volatile solvents and their limited capability of dissolving polymers of different types. In this report, we conceive of making electrospun fibers from a relatively novel solvent system: room temperature ionic liquids (RTILs). RTILs have become more important in a wide array of chemical processes owing to their capability of dissolving both polar and nonpolar compounds. 5 Other desirable properties of RTILs include low or zero vapor pressure, low melting point, large liquidus range, high thermal stability, large electrochemical window, and recyclability. 6 Further, the properties of an RTIL can be modified by adjusting the structures of its anion or cation or both, and hence, RTILs are also called designer solvents. RTILs have proven to be a promising solvent system for the reactions involving biopolymers such as enzymes 7 and carbohydrates. [8][9][10] The successful application of RTILs in electrospinning could increase the number and types of materials from which the fibers can be made.Electrospinning can be considered as a derivative of the electrospray process, as both use high voltage to form a liquid jet. In the electrospinning process, a polymer solution is held by its surface tension at the end of a capillary. When a sufficiently large electric field is applied, the solution at the tip of the capillary elongates to form a cone because of coupled effects of the electrostatic repulsion within the charged droplet and attraction to a grounded electrode of opposite polarity. As the strength of the electric field is increased, the charge overcomes the surface tension, and a fine jet is ejected from the apex of the cone...

We present the fabrication and electrical characterization of a flexible hybrid composite structure using aligned multiwall carbon nanotube arrays in a poly(dimethylsiloxane) (PDMS) matrix. Using lithographically patterned nanotube arrays, one can make these structures at any length scale from submicrometer levels to bulk quantities. The PDMS matrix undergoes excellent conformal filling within the dense nanotube network, giving rise to extremely flexible conducting structures with unique electromechanical properties. We demonstrate its robustness against high stress conditions, under which the composite is found to retain its conducting nature. We also demonstrate that these structures can be utilized directly as flexible field-emission devices. Our devices show some of the best field-enhancement factors and turn-on electric fields reported so far.

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Triblock polymers, poly(ethylene oxide-b-propylene oxide-b-ethylene oxide) (PEO-b-PPO-b-PEO), are used as molecular templates in poly(methyl silsesquioxane) (MSQ) matrixes to fabricate nanoporous organosilicates for low dielectric constant applications. The results show that aggregation of block copolymers in the MSQ matrix can be prevented with the fast solvent evaporation which accompanies spin casting. Solid-state NMR shows that the triblock copolymer microphase-separates from the MSQ during a curing step, resulting in polymer domain size in the range of 3−15 nm, depending upon the polymer composition and loading percentage. When the films are heated to 500 °C, extremely small pores (2−6 nm) are generated, which are studied by small angle neutron scattering and positronium annihilation lifetime spectroscopy. These materials attain ultralow dielectric constants (k ≈ 1.5) with good electrical and mechanical properties.

Triblock polymers, poly(ethylene oxide-b-propylene oxide-b-ethylene oxide) (PEO-b-PPO-b-PEO), are used as molecular templates in poly(methyl silsesquioxane) (MSQ) matrixes to fabricate nanoporous organosilicates. The triblock copolymers microphase-separate into nanometer domains as the MSQ matrix becomes increasingly hydrophobic during a curing step. Extremely small pores (2−5 nm) are generated after thermally removing the template material. These materials attain ultralow dielectric constants (k ≈ 1.5) with electrical and mechanical integrity.