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Showing papers on "Carbon nanotube published in 2014"


Journal ArticleDOI
TL;DR: N nanoscale nickel oxide/nickel heterostructures formed on carbon nanotube sidewalls as highly effective electrocatalysts for hydrogen evolution reaction with activity similar to platinum are reported.
Abstract: There is ongoing research into new electrocatalysts for hydrogen production from water splitting. Here, the authors report the electrocatalytic performance of nickel/nickel oxide heterostructures on carbon nanotubes, and are able to assemble a water electrolyzer operated by a single-cell 1.5 V battery.

1,345 citations


Journal ArticleDOI
TL;DR: A hierarchically structured carbon microfibre made of an interconnected network of aligned single-walled carbon nanotubes with interposed nitrogen-doped reduced graphene oxide sheets is synthesized and subsequently used to make a supercapacitor with high volumetric energy density.
Abstract: Hierarchical hybrid carbon fibres consisting of a network of nitrogen-doped reduced graphene oxide and single-walled carbon nanotubes are synthesized and subsequently used to make a supercapacitor with high volumetric energy density.

1,276 citations


Journal ArticleDOI
TL;DR: This paper identifies thermal stability as a fundamental weak point of perovskite solar cells, and demonstrates an elegant approach to mitigating thermal degradation by replacing the organic hole transport material with polymer-functionalized single-walled carbon nanotubes (SWNTs) embedded in an insulating polymer matrix.
Abstract: Organic–inorganic perovskite solar cells have recently emerged at the forefront of photovoltaics research. Power conversion efficiencies have experienced an unprecedented increase to reported values exceeding 19% within just four years. With the focus mainly on efficiency, the aspect of stability has so far not been thoroughly addressed. In this paper, we identify thermal stability as a fundamental weak point of perovskite solar cells, and demonstrate an elegant approach to mitigating thermal degradation by replacing the organic hole transport material with polymer-functionalized single-walled carbon nanotubes (SWNTs) embedded in an insulating polymer matrix. With this composite structure, we achieve JV scanned power-conversion efficiencies of up to 15.3% with an average efficiency of 10 ± 2%. Moreover, we observe strong retardation in thermal degradation as compared to cells employing state-of-the-art organic hole-transporting materials. In addition, the resistance to water ingress is remarkably enhanced...

1,052 citations


Journal ArticleDOI
TL;DR: A nanohybrid that consists of carbon nanotubes decorated with CoP nanocrystals (CoP/CNT) was prepared by the low-temperature phosphidation of a Co3O4/C NT precursor and only requires overpotentials of 70 and 122 mV to attain current densities of 2 and 10 mA cm(-2), respectively.
Abstract: The development of effective and inexpensive hydrogen evolution reaction (HER) electrocatalysts for future renewable energy systems is highly desired. The strongly acidic conditions in proton exchange membranes create a need for acid-stable HER catalysts. A nanohybrid that consists of carbon nanotubes decorated with CoP nanocrystals (CoP/CNT) was prepared by the low-temperature phosphidation of a Co3O4/CNT precursor. As a novel non-noble-metal HER catalyst operating in acidic electrolytes, the nanohybrid exhibits an onset overpotential of as low as 40 mV, a Tafel slope of 54 mV dec−1, an exchange current density of 0.13 mA cm−2, and a Faradaic efficiency of nearly 100 %. This catalyst maintains its catalytic activity for at least 18 hours and only requires overpotentials of 70 and 122 mV to attain current densities of 2 and 10 mA cm−2, respectively.

1,007 citations


Journal ArticleDOI
TL;DR: The synthesis of cobalt-embedded nitrogen-rich carbon nanotubes (NRCNTs) that can efficiently electrocatalyze the hydrogen evolution reaction (HER) with activities close to that of Pt and function well under acidic, neutral or basic media alike, allowing them to be coupled with the best available oxygen-evolving catalysts.
Abstract: Despite being technically possible, splitting water to generate hydrogen is still practically unfeasible due mainly to the lack of sustainable and efficient catalysts for the half reactions involved. Herein we report the synthesis of cobalt-embedded nitrogen-rich carbon nanotubes (NRCNTs) that 1) can efficiently electrocatalyze the hydrogen evolution reaction (HER) with activities close to that of Pt and 2) function well under acidic, neutral or basic media alike, allowing them to be coupled with the best available oxygen-evolving catalysts-which also play crucial roles in the overall water-splitting reaction. The materials are synthesized by a simple, easily scalable synthetic route involving thermal treatment of Co(2+) -embedded graphitic carbon nitride derived from inexpensive starting materials (dicyandiamide and CoCl2 ). The materials' efficient catalytic activity is mainly attributed to their nitrogen dopants and concomitant structural defects.

945 citations


Journal ArticleDOI
TL;DR: Graphene plasmons are rapidly emerging as a viable tool for fast electrical manipulation of light as mentioned in this paper, and the prospects for applications to electro-optical modulation, optical sensing, quantum plasmonics, light harvesting, spectral photometry, and tunable lighting at the nanoscale are further stimulated by the relatively low level of losses and high degree of spatial confinement that characterize these excitations compared with conventional plasmic materials.
Abstract: Graphene plasmons are rapidly emerging as a viable tool for fast electrical manipulation of light. The prospects for applications to electro-optical modulation, optical sensing, quantum plasmonics, light harvesting, spectral photometry, and tunable lighting at the nanoscale are further stimulated by the relatively low level of losses and high degree of spatial confinement that characterize these excitations compared with conventional plasmonic materials. We start with a general description of the plasmons in extended graphene, followed by analytical methods that lead to reasonably accurate estimates of both the plasmon energies and the strengths of coupling to external light in graphene nanostructures, including graphene ribbons. We discuss several possible strategies to extend these plasmons towards the visible and near infrared, including a reduction in the size of the graphene structures and an increase in the level of doping. Specifically, we discuss plasmons in narrow ribbons and molecular-size graphene structures. We further formulate prescriptions based on geometry to increase the level of electrostatic doping without causing electrical breakdown. Results are also presented for plasmons in highly-doped single-wall carbon nanotubes, which exhibit similar characteristics as narrow ribbons and show a relatively small dependence on the chirality of the tubes. We further discuss perfect light absorption by a single-atom carbon layer, which we illustrate by investigating arrays of ribbons using fully analytical expressions. Finally, we explore the possibility of exploiting optically pumped transient plasmons in graphene, whereby the optically heated graphene valence band can sustain collective plasmon oscillations similar to those of highly doped graphene, and well-defined during the picosecond time window over which the electron is at an elevated temperature.

900 citations


Journal ArticleDOI
TL;DR: In this paper, a review focuses on recent progress in the experimental and computational studies of the roles of heteroatoms in heterogeneous nanocarbons for electrocatalytic oxygen reduction reaction (ORR).
Abstract: Heterogeneous nanocarbon materials are being increasingly investigated and deployed in numerous new technologies and devices for sustainable energy conversion and storage. Nanocarbons often consist of fullerene, graphene and carbon nanotubes. Their derivatives include quantum dots, nanofibres, nanoribbons, nanospheres/capsules and other nanostructured morphologies. The heterogeneous forms of these nanocarbons stem from the implantation of alien atoms into the aromatic carbon lattice or the covalent grafting of functional groups onto the carbon basal plane or edge sites. Heterogeneous nanocarbons have shown remarkable advantages in solar cells, water splitting, supercapacitors, lithium ion batteries and catalysis. This review focuses on recent progress in the experimental and computational studies of the roles of heteroatoms in heterogeneous nanocarbons for electrocatalytic oxygen reduction reaction (ORR). Critical perspectives are devoted to the ambiguous phenomena in this emerging research area. The long standing debate about the active sites is discussed with an emphasis on more rational development of advanced nanocarbon-based electrocatalysts for ORR.

869 citations


Journal ArticleDOI
TL;DR: The strength and flexibility of carbon nanotubes make them of potential use in controlling other nanoscale structures, which suggests they will have a significant role in nanotechnology engineering.
Abstract: Current discoveries of different forms of carbon nanostructures have motivated research on their applications in various fields. They hold promise for applications in medicine, gene, and drug delivery areas. Many different production methods for carbon nanotubes (CNTs) have been introduced; functionalization, filling, doping, and chemical modification have been achieved, and characterization, separation, and manipulation of individual CNTs are now possible. Parameters such as structure, surface area, surface charge, size distribution, surface chemistry, and agglomeration state as well as purity of the samples have considerable impact on the reactivity of carbon nanotubes. Otherwise, the strength and flexibility of carbon nanotubes make them of potential use in controlling other nanoscale structures, which suggests they will have a significant role in nanotechnology engineering.

833 citations


Journal ArticleDOI
TL;DR: In this paper, a strategy to encapsulate 3D transition metals Fe, Co and the FeCo alloy into nitrogen-doped carbon nanotubes (CNTs) and investigated their hydrogen evolution reaction (HER) activity in acidic electrolytes.
Abstract: Employing a low-cost and highly efficient electrocatalyst to replace Pt-based catalysts for hydrogen evolution reaction (HER) has attracted increasing interest in renewable energy research. Earth-abundant transition metals such as Fe, Co and Ni have been investigated as promising alternatives in alkaline electrolytes. However, these non-precious-metal catalysts are not stable in acids, excluding their application in the acidic solid polymer electrolyte (SPE). Herein, we report a strategy to encapsulate 3d transition metals Fe, Co and the FeCo alloy into nitrogen-doped carbon nanotubes (CNTs) and investigated their HER activity in acidic electrolytes. The optimized catalysts exhibited long-term durability and high activity with only an ∼70 mV onset overpotential vs. RHE which is quite close to that of the commercial 40% Pt/C catalyst, demonstrating the potential for the replacement of Pt-based catalysts. Density functional theory (DFT) calculations indicated that the introduction of metal and nitrogen dopants can synergistically optimize the electronic structure of the CNTs and the adsorption free energy of H atoms on CNTs, and therefore promote the HER with a Volmer–Heyrovsky mechanism.

783 citations


Journal ArticleDOI
TL;DR: A new class of highly efficient oxygen evolution catalysts has been synthesized through the self-assembly of graphitic carbon nitride nanosheets and carbon nanotubes, driven by π-π stacking and electrostatic interactions, and exhibit higher catalytic oxygen evolution activity and stronger durability than Ir-based noble-metal catalysts.
Abstract: A new class of highly efficient oxygen evolution catalysts has been synthesized through the self-assembly of graphitic carbon nitride nanosheets and carbon nanotubes, driven by π-π stacking and electrostatic interactions. Remarkably, the catalysts exhibit higher catalytic oxygen evolution activity and stronger durability than Ir-based noble-metal catalysts and display the best performance among the reported nonmetal catalysts. This good result is attributed to the high nitrogen content and the efficient mass and charge transfer in the porous three-dimensional nanostructure.

760 citations


Journal ArticleDOI
Hao Sun1, Renchao Che1, Xiao You1, Yishu Jiang1, Zhibin Yang1, Jue Deng1, Longbin Qiu1, Huisheng Peng1 
TL;DR: The incorporation of a second phase such as a metal and a conducting polymer greatly enhances the microwave-absorption capability and a remarkable reflection loss is achieved.
Abstract: Aligned carbon-nanotube (CNT) sheets are used as building blocks to prepare light-weight, frequency-tunable and high-performance microwave absorbers, and the absorption frequency can be accurately controlled by stacking them with different intersectional angles. A remarkable reflection loss of -47.66 dB is achieved by stacking four aligned CNT sheets with an intersectional angle of 90° between two neighboring ones. The incorporation of a second phase such as a metal and a conducting polymer greatly enhances the microwave-absorption capability.

Journal ArticleDOI
01 Sep 2014-Small
TL;DR: This is a review on recent developments in the field of conductive nanomaterials and their application in printed electronics, with particular emphasis on inkjet printing of ink formulations based on metal nanoparticles, carbon nanotubes, and graphene sheets.
Abstract: This is a review on recent developments in the field of conductive nanomaterials and their application in printed electronics, with particular emphasis on inkjet printing of ink formulations based on metal nanoparticles, carbon nanotubes, and graphene sheets. The review describes the basic properties of conductive nanomaterials suitable for printed electronics (metal nanoparticles, carbon nanotubes, and graphene), their stabilization in dispersions, formulations of conductive inks, and obtaining conductive patterns by using various sintering methods. Applications of conductive nanomaterials for electronic devices (transparent electrodes, metallization of solar cells, RFID antennas, TFTs, and light emitting devices) are also briefly reviewed.

Journal ArticleDOI
26 Jun 2014-Nature
TL;DR: It is shown that SWNTs of a single chirality, (12, 6), can be produced directly with an abundance higher than 92 per cent when using tungsten-based bimetallic alloy nanocrystals as catalysts, unlike other catalysts used so far, which have such high melting points that they maintain their crystalline structure during the chemical vapour deposition process.
Abstract: Single-walled carbon nanotubes of a single chirality can be produced with an abundance of more than 92 per cent when using tungsten-based bimetallic alloy nanocrystals as catalysts. Single-walled carbon nanotubes (SWNTs) have many outstanding material properties that depend sensitively on their exact structure. This structure–function relationship can be fully exploited only with access to structurally pure SWNTs, but producing just one tube type remains a considerable challenge. Here Feng Yang et al. describe a strategy to realize chirality-specific growth of a single SWNT type using solid tungsten–cobalt alloy nanoparticles as catalysts. The tungsten component ensures high-temperature stability for the catalyst structure and cobalt is an effective catalyst. Optimization of the strategy should boost selectivity further, to deliver structurally pure SWNT samples that may enable wider use and development of these unique materials for practical applications. Carbon nanotubes have many material properties that make them attractive for applications1,2. In the context of nanoelectronics3, interest has focused on single-walled carbon nanotubes4 (SWNTs) because slight changes in tube diameter and wrapping angle, defined by the chirality indices (n, m), will shift their electrical conductivity from one characteristic of a metallic state to one characteristic of a semiconducting state, and will also change the bandgap. However, this structure–function relationship can be fully exploited only with structurally pure SWNTs. Solution-based separation methods5 yield tubes within a narrow structure range, but the ultimate goal of producing just one type of SWNT by controlling its structure during growth has proved to be a considerable challenge over the last two decades6,7,8,9. Such efforts aim to optimize the composition6,10,11,12,13,14,15,16,17 or shape18,19,20,21 of the catalyst particles that are used in the chemical vapour deposition synthesis process to decompose the carbon feedstock and influence SWNT nucleation and growth22,23,24,25. This approach resulted in the highest reported proportion, 55 per cent, of single-chirality SWNTs in an as-grown sample11. Here we show that SWNTs of a single chirality, (12, 6), can be produced directly with an abundance higher than 92 per cent when using tungsten-based bimetallic alloy nanocrystals as catalysts. These, unlike other catalysts used so far, have such high melting points that they maintain their crystalline structure during the chemical vapour deposition process. This feature seems crucial because experiment and simulation both suggest that the highly selective growth of (12, 6) SWNTs is the result of a good structural match between the carbon atom arrangement around the nanotube circumference and the arrangement of the catalytically active atoms in one of the planes of the nanocrystal catalyst. We anticipate that using high-melting-point alloy nanocrystals with optimized structures as catalysts paves the way for total chirality control in SWNT growth and will thus promote the development of SWNT applications.

Journal ArticleDOI
16 Jan 2014-Nature
TL;DR: It is shown that strong, rapid adhesion between two hydrogels can be achieved at room temperature by spreading a droplet of a nanoparticle solution on one gel’s surface and then bringing the other gel into contact with it.
Abstract: Adhesives are made of polymers because, unlike other materials, polymers ensure good contact between surfaces by covering asperities, and retard the fracture of adhesive joints by dissipating energy under stress. But using polymers to 'glue' together polymer gels is difficult, requiring chemical reactions, heating, pH changes, ultraviolet irradiation or an electric field. Here we show that strong, rapid adhesion between two hydrogels can be achieved at room temperature by spreading a droplet of a nanoparticle solution on one gel's surface and then bringing the other gel into contact with it. The method relies on the nanoparticles' ability to adsorb onto polymer gels and to act as connectors between polymer chains, and on the ability of polymer chains to reorganize and dissipate energy under stress when adsorbed onto nanoparticles. We demonstrate this approach by pressing together pieces of hydrogels, for approximately 30 seconds, that have the same or different chemical properties or rigidities, using various solutions of silica nanoparticles, to achieve a strong bond. Furthermore, we show that carbon nanotubes and cellulose nanocrystals that do not bond hydrogels together become adhesive when their surface chemistry is modified. To illustrate the promise of the method for biological tissues, we also glued together two cut pieces of calf's liver using a solution of silica nanoparticles. As a rapid, simple and efficient way to assemble gels or tissues, this method is desirable for many emerging technological and medical applications such as microfluidics, actuation, tissue engineering and surgery.

Journal ArticleDOI
TL;DR: In this paper, the periodic table is used to explore how the choice of anode material affects rate performance, cycle stability, Li-ion insertion/extraction potentials, voltage hysteresis, volumetric and specific capacities, and other critical parameters.
Abstract: Growing market demand for portable energy storage has triggered significant research on high-capacity lithium-ion (Li-ion) battery anodes. Various elements have been utilized in innovative structures to enable these anodes, which can potentially increase the energy density and decrease the cost of Li-ion batteries. In this review, electrode and material parameters are considered in anode fabrication. The periodic table is then used to explore how the choice of anode material affects rate performance, cycle stability, Li-ion insertion/extraction potentials, voltage hysteresis, volumetric and specific capacities, and other critical parameters. Silicon (Si), germanium (Ge), and tin (Sn) anodes receive more attention in literature and in this review, but other elements, such as antimony (Sb), lead (Pb), magnesium (Mg), aluminum (Al), gallium (Ga), phosphorus (P), arsenic (As), bismuth (Bi), and zinc (Zn) are also discussed. Among conversion anodes focus is placed on oxides, nitrides, phosphides, and hydrides. Nanostructured carbon (C) receives separate consideration. Issues in high- capacity research, such as volume change, insufficient coulombic efficiency, and solid electrolyte interphase (SEI) layer stability are elucidated. Finally, advanced carbon composites utilizing carbon nanotubes (CNT), graphene, and size preserving external shells are discussed, including high mass loading (thick) electrodes and electrodes capable of providing load-bearing properties.

Journal ArticleDOI
TL;DR: In this paper, a hierarchical nanostructure composed of NiMn-layered double hydroxide microcrystals grafted on carbon nanotube (CNT) backbone is constructed by an in situ growth route, which exhibits superior supercapacitive performance.
Abstract: A hierarchical nanostructure composed of NiMn-layered double hydroxide (NiMn-LDH) microcrystals grafted on carbon nanotube (CNT) backbone is constructed by an in situ growth route, which exhibits superior supercapacitive performance. The resulting composite material (NiMn-LDH/CNT) displays a three-dimensional architecture with tunable Ni/Mn ratio, well-defined core-shell configuration, and enlarged surface area. An electrochemical investigation shows that the Ni3Mn1-LDH/CNT electrode is rather active, which delivers a maximum specific capacitance of 2960 F g–1 (at 1.5 A g–1), excellent rate capability (79.5% retention at 30 A g–1), and cyclic stability. Moreover, an all-solid-state asymmetric supercapacitor (SC) with good flexibility is fabricated by using the NiMn-LDH/CNT film and reduced graphene oxide (RGO)/CNT film as the positive and negative electrode, respectively, exhibiting a wide cell voltage of 1.7 V and largely enhanced energy density up to 88.3 Wh kg–1 (based on the total weight of the device). By virtue of the high-capacity of pseudocapacitive hydroxides and desirable conductivity of carbon-based materials, the monolithic design demonstrated in this work provides a promising approach for the development of flexible energy storage systems.

Journal ArticleDOI
TL;DR: In this article, the synthesis methods employed for the doping of different types of carbon materials with various elements and the characterization techniques used to investigate their physicochemical properties such as degree of graphitization, dopant content and surface area are reviewed.
Abstract: Carbon materials such as graphite, graphene, carbon nanotubes and ordered mesoporous carbon have attracted a lot of attention for their use in fuel cells, due to beneficial properties like high conductivity, high mechanical and chemical stability and, for the latter, high surface area. Doping these materials with nitrogen or, less commonly, other elements alters their (electronic) properties, making them particularly suitable for application as electrocatalysts for the oxygen reduction reaction (ORR) in a fuel cell. This paper reviews the synthesis methods employed for the doping of these different types of carbon materials with various elements and the characterization techniques used to investigate their physicochemical properties such as degree of graphitization, dopant content, dopant configuration and surface area. Furthermore, their application as electrocatalysts for the oxygen reduction in a fuel cell is reviewed. Finally, the possible mechanisms for the ORR on N-doped carbon materials are critically discussed and compared to the mechanisms of commercial Pt/C electrocatalysts.

Journal ArticleDOI
01 Jun 2014-Small
TL;DR: A new N-doped graphene/single-walled carbon nanotube (SWCNT) hybrid (NGSH) material is reported as an efficient noble-metal-free bifunctional electrocatalyst for both ORR and OER, opening up new avenues for energy conversion technologies based on earth-abundant, scalable, noble- metal-free catalysts.
Abstract: There is a growing interest in oxygen electrode catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), as they play a key role in a wide range of renewable energy technologies such as fuel cells, metal-air batteries, and water splitting. Nevertheless, the development of highly-active bifunctional catalysts at low cost for both ORR and OER still remains a huge challenge. Herein, we report a new N-doped graphene/single-walled carbon nanotube (SWCNT) hybrid (NGSH) material as an efficient noble-metal-free bifunctional electrocatalyst for both ORR and OER. NGSHs were fabricated by in situ doping during chemical vapor deposition growth on layered double hydroxide derived bifunctional catalysts. Our one-step approach not only provides simultaneous growth of graphene and SWCNTs, leading to the formation of three dimensional interconnected network, but also brings the intrinsic dispersion of graphene and carbon nanotubes and the dispersion of N-containing functional groups within a highly conductive scaffold. Thus, the NGSHs possess a large specific surface area of 812.9 m(2) g(-1) and high electrical conductivity of 53.8 S cm(-1) . Despite of relatively low nitrogen content (0.53 at%), the NGSHs demonstrate a high ORR activity, much superior to two constituent components and even comparable to the commercial 20 wt% Pt/C catalysts with much better durability and resistance to crossover effect. The same hybrid material also presents high catalytic activity towards OER, rendering them high-performance cheap catalysts for both ORR and OER. Our result opens up new avenues for energy conversion technologies based on earth-abundant, scalable, noble-metal-free catalysts.

Journal ArticleDOI
20 Feb 2014-Nature
TL;DR: It is shown that 40-nanometre-wide graphene nanoribbons epitaxially grown on silicon carbide are single-channel room-temperature ballistic conductors on a length scale greater than ten micrometres, which is similar to the performance of metallic carbon nanotubes.
Abstract: Graphene nanoribbons will be essential components in future graphene nanoelectronics. However, in typical nanoribbons produced from lithographically patterned exfoliated graphene, the charge carriers travel only about ten nanometres between scattering events, resulting in minimum sheet resistances of about one kilohm per square. Here we show that 40-nanometre-wide graphene nanoribbons epitaxially grown on silicon carbide are single-channel room-temperature ballistic conductors on a length scale greater than ten micrometres, which is similar to the performance of metallic carbon nanotubes. This is equivalent to sheet resistances below 1 ohm per square, surpassing theoretical predictions for perfect graphene by at least an order of magnitude. In neutral graphene ribbons, we show that transport is dominated by two modes. One is ballistic and temperature independent; the other is thermally activated. Transport is protected from back-scattering, possibly reflecting ground-state properties of neutral graphene. At room temperature, the resistance of both modes is found to increase abruptly at a particular length--the ballistic mode at 16 micrometres and the other at 160 nanometres. Our epitaxial graphene nanoribbons will be important not only in fundamental science, but also--because they can be readily produced in thousands--in advanced nanoelectronics, which can make use of their room-temperature ballistic transport properties.

Journal ArticleDOI
TL;DR: Nitrogen-doped aligned CNT/graphene sandwiches are rationally designed and in-situ fabricated by a facile catalytic growth on bifunctional natural catalysts that exhibit high-rate performances as scaffolds for lithium-sulfur batteries, with a high initial capacity.
Abstract: Nitrogen-doped aligned CNT/graphene sandwiches are rationally designed and in-situ fabricated by a facile catalytic growth on bifunctional natural catalysts that exhibit high-rate performances as scaffolds for lithium-sulfur batteries, with a high initial capacity of 1152 mA h g(-1) at 1.0 C. A remarkable capacity of 770 mA h g(-1) can be achieved at 5.0 C. Such a design strategy for materials opens up new perspectives to novel advanced functional composites, especially interface-modified hierarchical nanocarbons for broad applications.

Journal ArticleDOI
TL;DR: In this paper, a 3D graphene foam (GF)/carbon nanotube (CNT) hybrid film with high flexibility and robustness was used as the ideal support for deposition of large amounts of electrochemically active materials per unit area.
Abstract: In this work, we report the fabrication of a new 3D graphene foam (GF)/carbon nanotube (CNT) hybrid film with high flexibility and robustness as the ideal support for deposition of large amounts of electrochemically active materials per unit area. To demonstrate the concept, we have deposited MnO2 and polypyrrole (Ppy) on the GF/CNT films and successfully fabricated lightweight and flexible asymmetric supercapacitors (ASCs). These ASCs assembled from GF/CNT/MnO2 and GF/CNT/Ppy hybrid films with high loading of electroactive materials in an aqueous electrolyte are able to function with an output voltage of 1.6 V, and deliver high energy/power density (22.8 W h kg−1 at 860 W kg−1 and 2.7 kW kg−1 at 6.2 W h kg−1). The rate performance can be further improved with less loading of electroactive materials (10.3 kW kg−1 at 10.9 W h kg−1). The ASCs demonstrate remarkable cycling stability (capacitance retention of 90.2–83.5% after 10 000 cycles), which is among the best reported for ASCs with both electrodes made of non-carbon electroactive materials. Also the ASCs are able to perfectly retain their electrochemical performance at different bending angles. These ASCs demonstrate great potential as power sources for flexible and lightweight electronic devices.

Journal ArticleDOI
TL;DR: This tutorial review focuses on the synthetic techniques for preparation of porous carbon spheres and carbon monoliths, including hydrothermal carbonization, emulsion Templating, ice templating and new developments in making porous carbons from sustainable biomass and metal-organic framework templates.
Abstract: The development of the next generation of advanced lithium-ion batteries (LIBs) requires new & advanced materials and novel fabrication techniques in order to push the boundaries of performance and open up new and exciting markets. Structured carbon materials, with controlled pore features on the micron and nanometer scales, are explored as advanced alternatives to conventional graphite as the active material of the LIB anode. Mesoporous carbon materials, carbon nanotube-based materials, and graphene-based materials have been extensively investigated and reviewed. Morphology control (e.g., colloids, thin films, nanofibrous mats, monoliths) and hierarchical pores (particularly the presence of large pores) exhibit an increasing influence on LIB performance. This tutorial review focuses on the synthetic techniques for preparation of porous carbon spheres and carbon monoliths, including hydrothermal carbonization, emulsion templating, ice templating and new developments in making porous carbons from sustainable biomass and metal-organic framework templating. We begin with a brief introduction to LIBs, defining key parameters and terminology used to assess the performance of anode materials, and then address synthetic techniques for the fabrication of carbon spheres & monoliths and the relevant composites, followed, respectively, by a review of their performance as LIB anode materials. The review is completed with a prospective view on the possible direction of future research in this field.

Journal ArticleDOI
05 May 2014-ACS Nano
TL;DR: Among the prepared catalysts, Mo2C/CNT-graphene shows the highest activity for hydrogen evolution reaction with a small onset overpotential and Tafel slope of 58 mV/dec as well as an excellent stability in acid media.
Abstract: Highly active and stable electrocatalysts for hydrogen evolution have been developed on the basis of molybdenum compounds (Mo2C, Mo2N, and MoS2) on carbon nanotube (CNT)-graphene hybrid support via a modified urea-glass route. By a simple modification of synthetic variables, the final phases are easily controlled from carbide, nitride to sulfide with homogeneous dispersion of nanocrystals on the CNT-graphene support. Among the prepared catalysts, Mo2C/CNT-graphene shows the highest activity for hydrogen evolution reaction with a small onset overpotential of 62 mV and Tafel slope of 58 mV/dec as well as an excellent stability in acid media. Such enhanced catalytic activity may originate from its low hydrogen binding energy and high conductivity. Moreover, the CNT-graphene hybrid support plays crucial roles to enhance the activity of molybdenum compounds by alleviating aggregation of the nanocrystals, providing a large area to contact with electrolyte, and facilitating the electron transfer.

Journal ArticleDOI
TL;DR: In this article, a rational hybridization of the sp2 nanocarbon and nanostructured porous carbon into hierarchical all-carbon nanoarchitectures is demonstrated, with full inherited advantages of the component materials.
Abstract: The sp2-hybridized nanocarbon (e.g., carbon nanotubes (CNTs) and graphene) exhibits extraordinary mechanical strength and electrical conductivity but limited external accessible surface area and a small amount of pores, while nanostructured porous carbon affords a huge surface area and abundant pore structures but very poor electrical conductance. Herein the rational hybridization of the sp2 nanocarbon and nanostructured porous carbon into hierarchical all-carbon nanoarchitectures is demonstrated, with full inherited advantages of the component materials. The sp2 graphene/CNT interlinked networks give the composites good electrical conductivity and a robust framework, while the meso-/microporous carbon and the interlamellar compartment between the opposite graphene accommodate sulfur and polysulfides. The strong confinement induced by micro-/mesopores of all-carbon nanoarchitectures renders the transformation of S8 crystal into amorphous cyclo-S8 molecular clusters, restraining the shuttle phenomenon for high capacity retention of a lithium-sulfur cell. Therefore, the composite cathode with an ultrahigh specific capacity of 1121 mAh g−1 at 0.5 C, a favorable high-rate capability of 809 mAh g−1 at 10 C, a very low capacity decay of 0.12% per cycle, and an impressive cycling stability of 877 mAh g−1 after 150 cycles at 1 C. As sulfur loading increases from 50 wt% to 77 wt%, high capacities of 970, 914, and 613 mAh g−1 are still available at current densities of 0.5, 1, and 5 C, respectively. Based on the total mass of packaged devices, gravimetric energy density of GSH@APC-S//Li cell is expected to be 400 Wh kg−1 at a power density of 10 000 W kg−1, matching the level of engine driven systems.

Journal ArticleDOI
TL;DR: In this article, the importance of proper structural and compositional engineering that leads to improved physical/chemical properties of iron oxides for efficient electrochemical energy storage is stressed and novel approaches to the construction of iron-oxide-based nanostructures are highlighted.
Abstract: Iron oxides, such as Fe2O3 and Fe3O4, have recently received increased attention as very promising anode materials for rechargeable lithium-ion batteries (LIBs) because of their high theoretical capacity, non-toxicity, low cost, and improved safety. Nanostructure engineering has been demonstrated as an effective approach to improve the electrochemical performance of electrode materials. Here, recent research progress in the rational design and synthesis of diverse iron oxide-based nanomaterials and their lithium storage performance for LIBs, including 1D nanowires/rods, 2D nanosheets/flakes, 3D porous/hierarchical architectures, various hollow structures, and hybrid nanostructures of iron oxides and carbon (including amorphous carbon, carbon nanotubes, and graphene). By focusing on synthesis strategies for various iron-oxide-based nanostructures and the impacts of nanostructuring on their electrochemical performance, novel approaches to the construction of iron-oxide-based nanostructures are highlighted and the importance of proper structural and compositional engineering that leads to improved physical/chemical properties of iron oxides for efficient electrochemical energy storage is stressed. Iron-oxide-based nanomaterials stand a good chance as negative electrodes for next generation LIBs.

Journal ArticleDOI
TL;DR: An overview of the practical benefits from chemical modification/doping, including the controllability of electronic energy level, charge carrier density, surface energy and surface reactivity for diverse advanced applications is presented, namely flexible electronics/optoelectronics, energy conversion/storage, nanocomposites, and environmental remediation.
Abstract: Outstanding pristine properties of carbon nanotubes and graphene have limited the scope for real-life applications without precise controllability of the material structures and properties. This invited article to celebrate the 25th anniversary of Advanced Materials reviews the current research status in the chemical modification/doping of carbon nanotubes and graphene and their relevant applications with optimized structures and properties. A broad aspect of specific correlations between chemical modification/doping schemes of the graphitic carbons with their novel tunable material properties is summarized. An overview of the practical benefits from chemical modification/doping, including the controllability of electronic energy level, charge carrier density, surface energy and surface reactivity for diverse advanced applications is presented, namely flexible electronics/optoelectronics, energy conversion/storage, nanocomposites, and environmental remediation, with a particular emphasis on their optimized interfacial structures and properties. Future research direction is also proposed to surpass existing technological bottlenecks and realize idealized graphitic carbon applications.

Journal ArticleDOI
07 Aug 2014-Nature
TL;DR: This work converts molecular precursors into ultrashort singly capped ‘armchair’ nanotube seeds using surface-catalysed cyclodehydrogenation on a platinum surface, and elongates these during a subsequent growth phase to produce single-chirality and essentially defect-free SWCNTs with lengths up to a few hundred nanometres.
Abstract: Present preparation methods fail to meet fully the demand for structurally pure single-walled carbon nanotubes; surface-catalysed cyclodehydrogenation reactions are now shown to convert precursor molecules deposited on a platinum(111) surface into ultrashort nanotube seeds that can then be grown further into defect-free and structurally pure single-walled carbon nanotubes of single chirality. The electronic properties of single-walled carbon nanotubes (SWCNTs) are extraordinarily sensitive to their precise structure. To exploit their technological potential fully, samples containing only one SWCNT type are needed. Juan Ramon Sanchez-Valencia et al. have combined synthetic chemistry with materials engineering to develop a strategy that, with further optimization, could provide a route to nanotube-based materials for use in light detectors, photovoltaics, field-effect transistors and sensors. They use a surface-catalysed cyclodehydrogenation reaction to fold rationally designed precursor molecules deposited on a Pt(111) surface to produce 'end caps' that act as seeds for the growth of defect-free and structurally pure SWCNTs. The technique requires only modest temperatures and is fully compatible with today's complementary metal oxide semiconductor technologies. Cover: Konstantin Amsharov. Over the past two decades, single-walled carbon nanotubes (SWCNTs) have received much attention because their extraordinary properties are promising for numerous applications1,2. Many of these properties depend sensitively on SWCNT structure, which is characterized by the chiral index (n,m) that denotes the length and orientation of the circumferential vector in the hexagonal carbon lattice. Electronic properties are particularly strongly affected, with subtle structural changes switching tubes from metallic to semiconducting with various bandgaps. Monodisperse ‘single-chirality’ (that is, with a single (n,m) index) SWCNTs are thus needed to fully exploit their technological potential1,2. Controlled synthesis through catalyst engineering3,4,5,6, end-cap engineering7 or cloning strategies8,9, and also tube sorting based on chromatography10,11, density-gradient centrifugation, electrophoresis and other techniques12, have delivered SWCNT samples with narrow distributions of tube diameter and a large fraction of a predetermined tube type. But an effective pathway to truly monodisperse SWCNTs remains elusive. The use of template molecules to unambiguously dictate the diameter and chirality of the resulting nanotube8,13,14,15,16 holds great promise in this regard, but has hitherto had only limited practical success7,17,18. Here we show that this bottom-up strategy can produce targeted nanotubes: we convert molecular precursors into ultrashort singly capped (6,6) ‘armchair’ nanotube seeds using surface-catalysed cyclodehydrogenation on a platinum (111) surface, and then elongate these during a subsequent growth phase to produce single-chirality and essentially defect-free SWCNTs with lengths up to a few hundred nanometres. We expect that our on-surface synthesis approach will provide a route to nanotube-based materials with highly optimized properties for applications such as light detectors, photovoltaics, field-effect transistors and sensors2.

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TL;DR: An Fe-N-decorated hybrid material of carbon nanotubes grown in situ from porous carbon microblocks is designed and constructed, giving this low-priced material an outstanding catalytic performance for ORR closely comparable with Pt/C of the same quantity.
Abstract: An Fe-N-decorated hybrid material of carbon nanotubes (CNTs) grown in situ from porous carbon microblocks is designed and constructed. This material successfully combines the desirable merits for oxygen reduction reaction (ORR), such as highly active Fe-N species, good conductivity, large pore size, and sufficient surface area. These structural advantages give this low-priced material an outstanding catalytic performance for ORR closely comparable with Pt/C of the same quantity.

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TL;DR: In this article, an overview of the electrochemical studies on activated carbon, carbide derived carbon, zeolite-templated carbon, carbon aerogel, carbon nanotube, onion-like carbon, and graphene is provided.
Abstract: Electric double layer capacitors, also called supercapacitors, ultracapacitors, and electrochemical capacitors, are gaining increasing popularity in high power energy storage applications. Novel carbon materials with high surface area, high electrical conductivity, as well as a range of shapes, sizes and pore size distributions are being constantly developed and tested as potential supercapacitor electrodes. This article provides an overview of the electrochemical studies on activated carbon, carbide derived carbon, zeolite-templated carbon, carbon aerogel, carbon nanotube, onion-like carbon, and graphene. We discuss the key performance advantages and limitations of various nanostructured carbon materials and provide an overview of the current understanding of the structure–property relationships related to the transport and adsorption of electrolyte ions on their surfaces, specific and volumetric capacitance, self-discharge, cycle life, electrolyte stability, and others. We discuss the impact of microstructural defects, pore size distribution, pore tortuosity, chemistry and functional groups on the carbon surface, nanoscale curvature, and carbon-electrolyte interfacial energy. Finally, we review state-of-the art commercial large scale applications of supercapacitors, including their use in smart grids and distributed energy storage, hybrid electric and electric vehicles, energy efficient industrial equipment, ships, wind power stations, uninterruptible power supplies, power backup, and consumer devices. © 2013 John Wiley & Sons, Ltd.

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TL;DR: This paper will be helpful to better understand the current status of polymer/CNT fibers, especially high-performance fibers, and to find the most suitable processing techniques and conditions.
Abstract: Carbon nanotubes (CNTs) are regarded as ideal filler materials for polymeric fiber reinforcement due to their exceptional mechanical properties and 1D cylindrical geometry (nanometer-size diameter and very high aspect ratio). The reported processing conditions and property improvements of CNT reinforced polymeric fiber are summarized in this review. Because of CNT polymer interaction, polymer chains in CNTs’ vicinity (interphase) have been observed to have more compact packing, higher orientation, and better mechanical properties than bulk polymer. Evidences of the existence of interphase polymers in composite fibers, characterizations of their structures, and fiber properties are summarized and discussed. Implications of interphase phenomena on a broader field of fiber and polymer processing to make much stronger materials are now in the early stages of exploration. Beside improvements in tensile properties, the presence of CNTs in polymeric fibers strongly affects other properties, such as thermal stabi...