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1.
Adv Sci (Weinh) ; 6(12): 1802177, 2019 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-31380158

RESUMO

Noble-metal free, cost-effective, and highly stable catalysts with efficient activity for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) have attracted tremendous research interest in recent years. Here, a flexible, self-standing hybrid film comprising a N-doped single-wall carbon nanotube (SWCNT) network on which are anchored Ni nanoparticles encapsulated by a monolayer of N-doped carbon (NCNi) is reported. The films are prepared by floating catalyst chemical vapor deposition followed by NH3 treatment. The material obtained at optimum conditions shows excellent bifunctional electrocatalytic activity in alkaline media with low overpotentials of 190 and 270 mV for HER and OER, respectively, to reach a current density of 10 mA cm-2. A current density of 10 mA cm-2 at 1.57 V is achieved when this freestanding and binder-free rod-shaped NCNi/SWCNT assembly is used as cathode and anode in 1 m KOH solution for overall water splitting, presenting one of the best values reported to date.

2.
Nat Mater ; 18(1): 62-68, 2019 01.
Artigo em Inglês | MEDLINE | ID: mdl-30455446

RESUMO

Inorganic chalcogenides are traditional high-performance thermoelectric materials. However, they suffer from intrinsic brittleness and it is very difficult to obtain materials with both high thermoelectric ability and good flexibility. Here, we report a flexible thermoelectric material comprising highly ordered Bi2Te3 nanocrystals anchored on a single-walled carbon nanotube (SWCNT) network, where a crystallographic relationship exists between the Bi2Te3 <[Formula: see text]> orientation and SWCNT bundle axis. This material has a power factor of ~1,600 µW m-1 K-2 at room temperature, decreasing to 1,100 µW m-1 K-2 at 473 K. With a low in-plane lattice thermal conductivity of 0.26 ± 0.03 W m-1 K-1, a maximum thermoelectric figure of merit (ZT) of 0.89 at room temperature is achieved, originating from a strong phonon scattering effect. The origin of the excellent flexibility and thermoelectric performance of the Bi2Te3-SWCNT material is attributed, by experimental and computational evidence, to its crystal orientation, interface and nanopore structure. Our results provide insight into the design and fabrication of high-performance flexible thermoelectric materials.

3.
Adv Sci (Weinh) ; 5(5): 1700965, 2018 May.
Artigo em Inglês | MEDLINE | ID: mdl-29876218

RESUMO

This study reports a simple and effective technique for the high-throughput fabrication of flexible all-carbon nanotube (CNT) electronics using a photosensitive dry film instead of traditional liquid photoresists. A 10 in. sized photosensitive dry film is laminated onto a flexible substrate by a roll-to-roll technology, and a 5 µm pattern resolution of the resulting CNT films is achieved for the construction of flexible and transparent all-CNT thin-film transistors (TFTs) and integrated circuits. The fabricated TFTs exhibit a desirable electrical performance including an on-off current ratio of more than 105, a carrier mobility of 33 cm2 V-1 s-1, and a small hysteresis. The standard deviations of on-current and mobility are, respectively, 5% and 2% of the average value, demonstrating the excellent reproducibility and uniformity of the devices, which allows constructing a large noise margin inverter circuit with a voltage gain of 30. This study indicates that a photosensitive dry film is very promising for the low-cost, fast, reliable, and scalable fabrication of flexible and transparent CNT-based integrated circuits, and opens up opportunities for future high-throughput CNT-based printed electronics.

4.
Adv Mater ; 30(32): e1802057, 2018 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-29952030

RESUMO

Single-wall carbon nanotubes (SWCNTs), especially in the form of large-area and high-quality thin films, are a promising material for use in flexible and transparent electronics. Here, a continuous synthesis, deposition, and transfer technique is reported for the fabrication of meter-scale SWCNT thin films, which have an excellent optoelectrical performance including a low sheet resistance of 65 Ω/◽ with a transmittance of 90% at a wavelength of 550 nm. Using these SWCNT thin films, high-performance all-CNT thin-film transistors and integrated circuits are demonstrated, including 101-stage ring oscillators. The results pave the way for the future development of large-scale, flexible, and transparent electronics based on CNT thin films.

5.
Sci Adv ; 4(5): eaap9264, 2018 05.
Artigo em Inglês | MEDLINE | ID: mdl-29736413

RESUMO

Single-wall carbon nanotubes (SWCNTs) are ideal for fabricating transparent conductive films because of their small diameter, good optical and electrical properties, and excellent flexibility. However, a high intertube Schottky junction resistance, together with the existence of aggregated bundles of SWCNTs, leads to a degraded optoelectronic performance of the films. We report a network of isolated SWCNTs prepared by an injection floating catalyst chemical vapor deposition method, in which crossed SWCNTs are welded together by graphitic carbon. Pristine SWCNT films show a record low sheet resistance of 41 ohm □-1 at 90% transmittance for 550-nm light. After HNO3 treatment, the sheet resistance further decreases to 25 ohm □-1. Organic light-emitting diodes using this SWCNT film as anodes demonstrate a low turn-on voltage of 2.5 V, a high current efficiency of 75 cd A-1, and excellent flexibility. Investigation of isolated SWCNT-based field-effect transistors shows that the carbon-welded joints convert the Schottky contacts between metallic and semiconducting SWCNTs into near-ohmic ones, which significantly improves the conductivity of the transparent SWCNT network. Our work provides a new avenue of assembling individual SWCNTs into macroscopic thin films, which demonstrate great potential for use as transparent electrodes in various flexible electronics.

6.
Small ; 13(45)2017 12.
Artigo em Inglês | MEDLINE | ID: mdl-28961364

RESUMO

Oxygen reduction reaction (ORR) is a key step that determines the performance of a variety of energy storage and conversion devices, such as fuel cells and metal-air batteries. Heteroatom-doped carbon nanotubes (CNTs) and graphenes have attracted increasing interest and hold great promise as efficient ORR catalysts to replace noble-metal-based catalysts, owing to their unique structure characteristics, excellent physicochemical properties, low cost, and rich resources. In this review, recent progress on the design, fabrication, and performance of heteroatom-doped CNT- and graphene-based catalysts is summarized, aiming to provide insights into the working mechanism of these heteroatom-doped nanocarbons in ORR. The advantages, challenges that remain, and possible solutions of these nanocarbon-based electrocatalysts are discussed. Finally, future developing trends of the CNT- and graphene-based ORR catalysts are proposed.

7.
Nanoscale ; 9(24): 8213-8219, 2017 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-28580987

RESUMO

A vertically aligned carbon nanotube (VACNT) array is a promising candidate for a high-performance thermal interface material in high-power microprocessors due to its excellent thermal transport property. However, its rough and entangled free tips always cause poor interfacial contact, which results in serious contact resistance dominating the total thermal resistance. Here, we employed a thin carbon cover to restrain the disorderly growth of the free tips of a VACNT array. As a result, all the free tips are seamlessly connected by this thin carbon cover and the top surface of the array is smoothed. This unique structure guarantees the participation of all the carbon nanotubes in the array in the heat transport. Consequently the VACNT array grown on a Cu substrate shows a record low thermal resistance of 0.8 mm2 K W-1 including the two-sided contact resistances, which is 4 times lower than the best result previously reported. Remarkably, the VACNT array can be easily peeled away from the Cu substrate and act as a thermal pad with excellent flexibility, adhesive ability and heat transport capability. As a result the CNT array with a thin carbon cover shows great potential for use as a high-performance flexible thermal interface material.

8.
Adv Mater ; 29(32)2017 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-28635068

RESUMO

A major obstacle for the use of single-wall carbon nanotubes (SWCNTs) in electronic devices is their mixture of different types of electrical conductivity that strongly depends on their helical structure. The existence of metal impurities as a residue of a metallic growth catalyst may also lower the performance of SWCNT-based devices. Here, it is shown that by using silicon oxide (SiOx ) nanoparticles as a catalyst, metal-free semiconducting and metallic SWCNTs can be selectively synthesized by the chemical vapor deposition of ethanol. It is found that control over the nanoparticle size and the content of oxygen in the SiOx catalyst plays a key role in the selective growth of SWCNTs. Furthermore, by using the as-grown semiconducting and metallic SWCNTs as the channel material and source/drain electrodes, respectively, all-SWCNT thin-film transistors are fabricated to demonstrate the remarkable potential of these SWCNTs for electronic devices.

9.
Adv Sci (Weinh) ; 3(10): 1600113, 2016 10.
Artigo em Inglês | MEDLINE | ID: mdl-27840800

RESUMO

Carbon nanotubes (CNTs) filled with iron sulfide nanoparticles (NPs) are prepared by inserting sulfur and ferrocene into the hollow core of CNTs followed by heat treatment. It is found that pyrrhotite-11T iron sulfide (Fe-S) NPs with an average size of ≈15 nm are encapsulated in the tubular cavity of the CNTs (Fe-S@CNTs), and each particle is a single crystal. When used as the anode material of lithium-ion batteries, the Fe-S@CNT material exhibits excellent electrochemical lithium storage performance in terms of high reversible capacity, good cyclic stability, and desirable rate capability. In situ transmission electron microscopy studies show that the CNTs not only play an essential role in accommodating the volume expansion of the Fe-S NPs but also provide a fast transport path for Li ions. The results demonstrate that CNTs act as a unique nanocontainer and reactor that permit the loading and formation of electrochemically active materials with desirable electrochemical lithium storage performance. CNTs with their superior structural stability and Li-ion transfer kinetics are responsible for the improved rate capability and cycling performance of Fe-S NPs in CNTs.

10.
ACS Nano ; 10(9): 8676-82, 2016 09 27.
Artigo em Inglês | MEDLINE | ID: mdl-27537348

RESUMO

Lithium-sulfur (Li-S) batteries are attracting increasing interest due to their high theoretical specific energy density, low cost, and eco-friendliness. However, most reports of the high gravimetric specific capacity and long cyclic life are not practically reliable because of their low areal specific capacity derived from the low areal sulfur loading and low sulfur content. Here, we fabricated a highly porous graphene with high pore volume of 3.51 cm(3) g(-1) as the sulfur host, enabling a high sulfur content of 80 wt %, and based on this, we further proposed an all-graphene structure for the sulfur cathode with highly conductive graphene as the current collector and partially oxygenated graphene as a polysulfide-adsorption layer. This cathode structural design enables a 5 mg cm(-2) sulfur-loaded cathode showing both high initial gravimetric specific capacity (1500 mAh g(-1)) and areal specific capacity (7.5 mAh cm(-2)), together with excellent cycling stability for 400 cycles, indicating great promise for more reliable lithium-sulfur batteries.

12.
Nat Commun ; 7: 11160, 2016 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-27025784

RESUMO

The growth of high-quality semiconducting single-wall carbon nanotubes with a narrow band-gap distribution is crucial for the fabrication of high-performance electronic devices. However, the single-wall carbon nanotubes grown from traditional metal catalysts usually have diversified structures and properties. Here we design and prepare an acorn-like, partially carbon-coated cobalt nanoparticle catalyst with a uniform size and structure by the thermal reduction of a [Co(CN)6](3-) precursor adsorbed on a self-assembled block copolymer nanodomain. The inner cobalt nanoparticle functions as active catalytic phase for carbon nanotube growth, whereas the outer carbon layer prevents the aggregation of cobalt nanoparticles and ensures a perpendicular growth mode. The grown single-wall carbon nanotubes have a very narrow diameter distribution centred at 1.7 nm and a high semiconducting content of >95%. These semiconducting single-wall carbon nanotubes have a very small band-gap difference of ∼0.08 eV and show excellent thin-film transistor performance.

13.
Nanoscale ; 7(45): 19201-6, 2015 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-26526104

RESUMO

A nitrogen-doped mesoporous carbon containing a network of carbon nanotubes (CNTs) was produced for use as a catalyst for the oxygen reduction reaction (ORR). SiO2 nanoparticles were decorated with clusters of Fe atoms to act as catalyst seeds for CNT growth, after which the material was impregnated with aniline. After polymerization of the aniline, the material was pyrolysed and the SiO2 was removed by acid treatment. The resulting carbon-based hybrid also contained some Fe from the CNT growth catalyst and was doped with N from the aniline. The Fe-N species act as active catalytic sites and the CNT network enables efficient electron transport in the material. Mesopores left by the removal of the SiO2 template provide short transport pathways and easy access to ions. As a result, the catalyst showed not only excellent ORR activity, with 59 mV more positive onset potential and 30 mV more positive half-wave potential than a Pt/C catalyst, but also much longer durability and stronger tolerance to methanol crossover than a Pt/C catalyst.

14.
Nano Lett ; 15(8): 4922-7, 2015 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-26114583

RESUMO

The hollow core of a carbon nanotube (CNT) provides a unique opportunity to explore the physics, chemistry, biology, and metallurgy of different materials confined in such nanospace. Here, we investigate the nonequilibrium metallurgical processes taking place inside CNTs by in situ transmission electron microscopy using CNTs as nanoscale resistively heated crucibles having encapsulated metal nanowires/crystals in their channels. Because of nanometer size of the system and intimate contact between the CNTs and confined metals, an efficient heat transfer and high cooling rates (∼10(13) K/s) were achieved as a result of a flash bias pulse followed by system natural quenching, leading to the formation of disordered amorphous-like structures in iron, cobalt, and gold. An intermediate state between crystalline and amorphous phases was discovered, revealing a memory effect of local short-to-medium range order during these phase transitions. Furthermore, subsequent directional crystallization of an amorphous iron nanowire formed by this method was realized under controlled Joule heating. High-density crystalline defects were generated during crystallization due to a confinement effect from the CNT and severe plastic deformation involved.

15.
ACS Nano ; 9(5): 5063-71, 2015 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-25869474

RESUMO

Silicon has the highest theoretical lithium storage capacity of all materials at 4200 mAh/g; therefore, it is considered to be a promising candidate as the anode of high-energy-density lithium-ion batteries (LIBs). However, serious volume changes caused by lithium insertion/deinsertion lead to a rapid decay of the performance of the Si anode. Here, a Si nanoparticle (NP)-filled carbon nanotube (CNT) material was prepared by chemical vapor deposition, and a nanobattery was constructed inside a transmission electron microscope (TEM) using the Si NP-filled CNT as working electrode to directly investigate the structural change of the Si NPs and the confinement effect of the CNT during the lithiation and delithiation processes. It is found that the volume expansion (∼180%) of the lithiated Si NPs is restricted by the wall of the CNTs and that the CNT can accommodate this volume expansion without breaking its tubular structure. The Si NP-filled CNTs showed a high reversible lithium storage capacity and desirable high rate capability, because the pulverization and exfoliation of the Si NPs confined in CNTs were efficiently prevented. Our results demonstrate that filling CNTs with high-capacity active materials is a feasible way to make high-performance LIB electrode materials, taking advantage of the unique confinement effect and good electrical conductivity of the CNTs.

16.
Nanoscale ; 6(20): 12065-70, 2014 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-25189467

RESUMO

Nitrogen-doped (N-doped) single-wall carbon nanotubes (SWCNTs) were synthesized by chemical vapor deposition using SiOx nanoparticles as a catalyst and ethylenediamine as the source of both carbon and nitrogen. The N-doped SWCNTs have a mean diameter of 1.1 nm and a narrow diameter range, with 92% of them having diameters from 0.7 to 1.4 nm. Multi-wavelength laser Raman spectra and temperature-dependent electrical resistance indicate that the SWCNT sample is enriched with metallic nanotubes. These N-doped SWCNTs showed excellent electrocatalytic activity for the oxygen reduction reaction and highly selective and sensitive sensing ability for dopamine detection.


Assuntos
Metais/química , Nanotubos de Carbono/química , Nitrogênio/química , Dióxido de Silício/química , Carbono/química , Catálise , Dopamina/química , Eletroquímica , Eletrodos , Etilenodiaminas/química , Teste de Materiais , Nanotecnologia , Oxigênio/química , Análise Espectral Raman , Temperatura
17.
ACS Nano ; 8(7): 7156-62, 2014 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-24959864

RESUMO

We report the bulk synthesis of a sample with a high concentration of metallic single-wall carbon nanotubes (m-SWCNTs) using a modified floating catalyst chemical vapor deposition method with methane as the carbon precursor. By tuning experimental parameters, such as species and flux of carrier gases, catalyst concentration, growth temperature, etc., small-diameter semiconducting SWCNTs (s-SWCNTs) and large-diameter m-SWCNTs were obtained. Using identical growth conditions, at a temperature of 1000 °C, it was found that the addition of hydrogen as an etchant gas resulted in the preferential removal of the smaller diameter s-SWCNTs. As a result, a sample enriched with large-diameter metallic SWCNTs was obtained. The self-assembled fishnet-like m-SWCNT network showed excellent optical transparency and electrical conductivity.

18.
J Phys Chem Lett ; 5(8): 1427-32, 2014 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-26269989

RESUMO

The effect of sulfur on the catalytic nucleation and growth of single-wall carbon nanotubes (SWCNTs) from an iron catalyst was investigated in situ by transmission electron microscopy (TEM). The catalyst precursor of ferrocene and growth promoter of sulfur were selectively loaded inside of the hollow core of multiwall CNTs with open ends, which served as a nanoreactor powered by applying a voltage inside of the chamber of a TEM. It was found that a SWCNT nucleated and grew perpendicularly from a region of the catalyst nanoparticle surface, instead of the normal tangential growth that occurs with no sulfur addition. Our in situ TEM observation combined with CVD growth studies suggests that sulfur functions to promote the nucleation and growth of SWCNTs by forming inhomogeneous local active sites and modifying the interface bonding between catalysts and precipitated graphitic layers, so that carbon caps can be lifted off from the catalyst particle.

19.
ACS Nano ; 8(1): 292-301, 2014 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-24354297

RESUMO

We report a simple, versatile in situ transmission electron microscopy (TEM) approach for investigating the nucleation and growth mechanism of carbon nanotubes (CNTs), by which the composition, phase transition, and physical state of various catalysts can be clearly resolved. In our approach, catalyst nanoparticles (NPs) are placed in a multiwall CNT "tubular furnace" with two open ends, and a high temperature is obtained by Joule heating in the specimen chamber of a TEM. The carbon is supplied by electron irradiation-induced injection of carbon atoms. Comparative studies on the catalytic behavior of traditional iron oxide and recently discovered gold catalysts were performed. It was found that the growth of CNTs from iron oxide involves the reduction of Fe2O3 to Fe3C, nucleation and growth of CNTs from partially liquefied Fe3C, and finally the formation of elemental Fe when the growth stops. In contrast, while changes in shape, size, and orientation were also observed for the fluctuating Au NPs, no chemical reactions or phase transitions occurred during the nucleation of CNTs. These two distinct nucleation and growth processes and mechanisms would be valuable for the structure-controlled growth of CNTs by catalyst design and engineering.

20.
ACS Nano ; 7(8): 6831-9, 2013 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-23883135

RESUMO

We developed a simple and scalable selective synthesis method of high-quality, highly concentrated semiconducting single-wall carbon nanotubes (s-SWCNTs) by in situ hydrogen etching. Samples containing ~93% s-SWCNTs were obtained in bulk. These s-SWCNTs with good structural integrity showed a high oxidation resistance temperature of ~800 °C. Thin-film transistors based on the s-SWCNTs demonstrated a high carrier mobility of 21.1 cm(2) V(-1) s(-1) at an on/off ratio of 1.1 × 10(4) and a high on/off ratio of 4.0 × 10(5) with a carrier mobility of 7.0 cm(2) V(-1) s(-1). A biosensor fabricated using the s-SWCNTs had a very low dopamine detection limit of 10(-18) mol/L at room temperature.


Assuntos
Técnicas Biossensoriais , Dopamina/análise , Nanotubos de Carbono/química , Dopamina/química , Hidrogênio/química , Teste de Materiais , Microscopia Eletrônica de Transmissão , Nanotecnologia/métodos , Oxigênio/química , Tamanho da Partícula , Semicondutores , Análise Espectral Raman , Propriedades de Superfície , Temperatura , Fatores de Tempo , Transistores Eletrônicos
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