Single-walled carbon nanotubes can be classified as either metallic or semiconducting, depending on their conductivity, which is determined by their chirality. Existing synthesis methods cannot controllably grow nanotubes with a specific type of conductivity. By varying the noble gas ambient during thermal annealing of the catalyst, and in combination with oxidative and reductive species, we altered the fraction of tubes with metallic conductivity from one-third of the population to a maximum of 91%. In situ transmission electron microscopy studies reveal that this variation leads to differences in both morphology and coarsening behavior of the nanoparticles that we used to nucleate nanotubes. These catalyst rearrangements demonstrate that there are correlations between catalyst morphology and resulting nanotube electronic structure and indicate that chiral-selective growth may be possible.
The advance of nanomaterials has opened new opportunities to develop ever more sensitive sensors owing to their high surface-to-volume ratio. However, it is challenging to achieve intrinsic sensitivities of nanomaterials for ultra-low level detections due to their vulnerability against contaminations. Here we show that despite considerable achievements in the last decade, continuous in situ cleaning of carbon nanotubes with ultraviolet light during gas sensing can still dramatically enhance their performance. For instance in nitric oxide detection, while sensitivity in air is improved two orders of magnitude, under controlled environment it reaches a detection limit of 590 parts-per-quadrillion (ppq) at room temperature. Furthermore, aiming for practical applications we illustrate how to address gas selectivity by introducing a gate bias. The concept of continuous in situ cleaning not only reveals the tremendous sensing potential of pristine carbon nanotubes but also more importantly it can be applied to other nanostructures.
Formation of ripples on a supported graphene sheet involves interfacial interaction with the substrate. In this work, graphene was grown on a copper foil by chemical vapor deposition from methane. On thermal quenching from elevated temperatures, we observed the formation of ripples in grown graphene, developing a peculiar topographic pattern in the form of wavy grooves and single/double rolls, roughly honeycomb cells, or their combinations. Studies on pure copper foil under corresponding conditions but without the presence of hydrocarbon revealed the appearance of peculiar patterns on the foil surface, such as dendritic structures that are distinctive not of equilibrium solidified phases but arise from planar and/or convective instabilities driven by solutal and thermal capillary forces. We propose a new origin for the formation of ripples in the course of graphene growth at elevated temperatures, where the topographic pattern formation is governed by dynamic instabilities on the interface of a carbon-catalyst binary system. These non-equilibrium processes can be described based on Mullins-Sekerka and Benard-Marangoni instabilities in diluted binary alloys, which offer control over the ripple texturing through synthesis parameters such as temperature, imposed temperature gradient, quenching rate, diffusion coefficients of carbon in the metal catalyst, and the miscibility gap of the metal catalyst-carbon system.
A simple, highly scalable method of obtaining densely-packed, three-dimensional structures of interconnected, bilayer, hollow carbon nanocages, is reported. High-quality nanocages with well controlled wall thickness are synthesized via catalytic templating on densely-packed, mono-sized nickel nanoparticles, nucleating in situ during short, mid-temperature annealing of an inexpensive precursor
Graphite’s capacity of intercalating lithium in rechargeable batteries is limited (theoretically, 372 mAh g−1) due to low diffusion within commensurately-stacked graphene layers. Graphene foam with highly enriched incommensurately-stacked layers was grown and applied as an active electrode in rechargeable batteries. A 93% incommensurate graphene foam demonstrated a reversible specific capacity of 1,540 mAh g−1 with a 75% coulombic efficiency, and an 86% incommensurate sample achieves above 99% coulombic efficiency exhibiting 930 mAh g−1 specific capacity. The structural and binding analysis of graphene show that lithium atoms highly intercalate within weakly interacting incommensurately-stacked graphene network, followed by a further flexible rearrangement of layers for a long-term stable cycling. We consider lithium intercalation model for multilayer graphene where capacity varies with N number of layers resulting LiN+1C2N stoichiometry. The effective capacity of commonly used carbon-based rechargeable batteries can be significantly improved using incommensurate graphene as an anode material.
Understanding the performance volatility of carbon nanotube-based devices will expedite their applications. We performed in situ electrical and Raman scattering studies on an individual semiconducting single-walled carbon nanotube in the field-effect transistor geometry under different ambient and temperatures. The Raman G+ mode frequency responds in synchronization with changes in the charge density induced by an external gate voltage. Ambient caused a blueshift in the G+ mode and a reversible transformation of the device performance from n-type in vacuum to p-type in air, owing to the charge transfer-induced phonon renormalization by oxygen.
A simple method for the fabrication of highly photoactive nanocrystalline two-layer TiO(2) electrodes for solar cell applications is presented. Diluted titanium acetylacetonate has been used as a precursor for covering SnO(2):F (FTO) films with dense packed TiO(2) nanocrystallites. The nanoporous thick TiO(2) film follows the dense packed thin TiO(2) film as a second layer. For the latter, amorphous TiO(2) nanoparticles have been successfully synthesized by a sol-gel technique in an acidic environment with pH<1 and hydrothermal growth at a temperature of 200 °C. The acidic nanoparticle gel was neutralized by basic ammonia and a TiO(2) gel of pH 5 was obtained; this pH value is higher than the recently reported value of 3.1 (Park et al 2005 Adv. Mater. 17 2349-53). Highly interconnected, nanoporous, transparent and active TiO(2) films have been fabricated from the pH 5 gel. SEM, AFM and XRD analyses have been carried out for investigation of the crystal structure and the size of nanoparticles as well as the surface morphology of the films. Investigation of the photocurrent-voltage characteristics has shown improvement in cell performance along with the modification of the surface morphology, depending on pH of the TiO(2) gel. Increasing the pH of the gel from 2.1 to 5 enhanced the overall conversion efficiency of the dye-sensitized solar cells by approximately 30%. An energy conversion efficiency of 8.83% has been achieved for the cell (AM1.5, 100 mWcm(-2) simulated sunlight) compared to 6.61% efficiency in the absence of ammonia in the TiO(2) gel.
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