Daniel D. Tune

Double‐Walled Carbon Nanotube Processing

Single-walled carbon nanotubes (SWCNTs) have been the focus of intense research, and the body of literature continues to grow exponentially, despite more than two decades having passed since the first reports. As well as extensive studies of the fundamental properties, this has seen SWCNTs used in a plethora of applications as far ranging as microelectronics, energy storage, solar cells, and sensors, to cancer treatment, drug delivery, and neuronal interfaces. On the other hand, the properties and applications of double-walled carbon nanotubes (DWCNTs) have remained relatively under-explored. This is despite DWCNTs not only sharing many of the same unique characteristics of their single-walled counterparts, but also possessing an additional suite of potentially advantageous properties arising due to the presence of the second wall and the often complex inter-wall interactions that arise. For example, it is envisaged that the outer wall can be selectively functionalized whilst still leaving the inner wall in its pristine state and available for signal transduction. A similar situation arises in DWCNT field effect transistors (FETs), where the outer wall can provide a convenient degree of chemical shielding of the inner wall from the external environment, allowing the excellent transconductance properties of the pristine nanotubes to be more fully exploited. Additionally, DWCNTs should also offer unique opportunities to further the fundamental understanding of the inter-wall interactions within and between carbon nanotubes. However, the realization of these goals has so far been limited by the same challenge experienced by the SWCNT field until recent years, namely, the inherent heterogeneity of raw, as-produced DWCNT material. As such, there is now an emerging field of research regarding DWCNT processing that focuses on the preparation of material of defined length, diameter and electronic type, and which is rapidly building upon the experience gained by the broader SWCNT community. This review describes the background of the field, summarizing some relevant theory and the available synthesis and purification routes; then provides a thorough synopsis of the current state-of-the-art in DWCNT sorting methodologies, outlines contemporary challenges in the field, and discusses the outlook for various potential applications of the resulting material.

The potential sunlight harvesting efficiency of carbon nanotube solar cells

Elsewhere, laboratory-scale solar cells have been demonstrated which show clear evidence of the successful exploitation of semiconducting single walled carbon nanotubes (SWNTs) as primary absorbers of sunlight energy. The unique properties of SWNTs may allow for high efficiency solar cell devices however little progress has been made to quantify this. Herein we provide an in-depth analysis of the potential of SWNTs to harvest sunlight, using the best currently available data to simulate the absorption properties of different semiconducting SWNT species and thus calculating a species-dependent potential sunlight harvesting efficiency. The same model is then used to simulate relevant tandem cell scenarios, predicting a conservative estimate of the sunlight harvesting potential of ∼28% for a multijunction device absorbing in the visible and ∼19% for a similar device absorbing primarily in the infrared, whilst minimising absorption in the visible.

A TiO2 Nanofiber-Carbon Nanotube-Composite Photoanode for Improved Efficiency in Dye-Sensitized Solar Cells.

A light-scattering layer fabricated from electrospun titanium dioxide nanofibers (TiO2 -NFs) and single-walled carbon nanotubes (SWCNTs) formed a fiber-based photoanode. The nanocomposite scattering layer had a lawn-like structure and integration of carbon nanotubes into the NF photoanodes increased the power conversion efficiency from 2.9 % to 4.8 % under 1 Sun illumination. Under reduced light intensity (0.25 Sun), TiO2 -NF and TiO2 -NF/SWCNT-based DSSCs reached PCE values of up to 3.7 % and 6.6 %, respectively.

Single‐Walled Carbon Nanotube/Polyaniline/n‐Silicon Solar Cells: Fabrication, Characterization, and Performance Measurements

Carbon nanotube-silicon solar cells are a recently investigated photovoltaic architecture with demonstrated high efficiencies. Silicon solar-cell devices fabricated with a thin film of conductive polymer (polyaniline) have been reported, but these devices can suffer from poor performance due to the limited lateral current-carrying capacity of thin polymer films. Herein, hybrid solar-cell devices of a thin film of polyaniline deposited on silicon and covered by a single-walled carbon nanotube film are fabricated and characterized. These hybrid devices combine the conformal coverage given by the polymer and the excellent electrical properties of single-walled carbon nanotube films and significantly outperform either of their component counterparts. Treatment of the silicon base and carbon nanotubes with hydrofluoric acid and a strong oxidizer (thionyl chloride) leads to a significant improvement in performance.

Effect of Nanotube Film Thickness on the Performance of Nanotube-Silicon Hybrid Solar Cells

The results of measurements on solar cells made from randomly aligned thin films of single walled carbon nanotubes (SWCNTs) on n-type monocrystalline silicon are presented. The films are made by vacuum filtration from aqueous TritonX-100 suspensions of large diameter arc-discharge SWCNTs. The dependence of the solar cell performance on the thickness of the SWCNT film is shown in detail, as is the variation in performance due to doping of the SWCNT film with SOCl2.

Investigating the Effect of Carbon Nanotube Diameter and Wall Number in Carbon Nanotube/Silicon Heterojunction Solar Cells

Suspensions of single-walled, double-walled and multi-walled carbon nanotubes (CNTs) were generated in the same solvent at similar concentrations. Films were fabricated from these suspensions and used in carbon nanotube/silicon heterojunction solar cells and their properties were compared with reference to the number of walls in the nanotube samples. It was found that single-walled nanotubes generally produced more favorable results; however, the double and multi-walled nanotube films used in this study yielded cells with higher open circuit voltages. It was also determined that post fabrication treatments applied to the nanotube films have a lesser effect on multi-walled nanotubes than on the other two types.

Heterojunction Solar Cells Based on Silicon and Composite Films of Graphene Oxide and Carbon Nanotubes

Graphene oxide (GO) sheets have been used as the surfactant to disperse single-walled carbon nanotubes (CNT) in water to prepare GO/CNT electrodes that are applied to silicon to form a heterojunction that can be used in solar cells. GO/CNT films with different ratios of the two components and with various thicknesses have been used as semitransparent electrodes, and the influence of both factors on the performance of the solar cell has been studied. The degradation rate of the GO/CNT-silicon devices under ambient conditions has also been explored. The influence of the film thickness on the device performance is related to the interplay of two competing factors, namely, sheet resistance and transmittance. CNTs help to improve the conductivity of the GO/CNT film, and GO is able to protect the silicon from oxidation in the atmosphere.

Aligned Carbon Nanotube Thin Films from Liquid Crystal Polyelectrolyte Inks

Single walled carbon nanotube thin films are fabricated by solution shearing from high concentration sodium nanotubide polyelectrolyte inks. The solutions are produced by simple stirring of the nanotubes with elemental sodium in dimethylacetamide, and the nanotubes are thus not subject to any sonication-induced damage. At such elevated concentrations (∼4 mg mL(-1)), the solutions exist in the liquid crystal phase and during deposition this order is transferred to the films, which are well aligned in the direction of shear with a 2D nematic order parameter of ∼0.7 determined by polarized absorption measurements. Compared to similarly formed films made from superacids, the polyelectrolyte films contain smaller bundles and a much narrower distribution of bundle diameters. After p-doping with an organic oxidizer, the films exhibit a very high DC electrical to optical conductivity ratio of σ(DC)/σ(OP) ∼ 35, corresponding to a calculated DC conductivity of over 7000 S cm(-1). When very thin (T550 ∼ 96%), smooth (RMS roughness, R(q) ∼ 2.2 nm), and highly aligned films made via this new route are used as the front electrodes of carbon nanotube-silicon solar cells, the power conversion efficiency is almost an order of magnitude greater than that obtained when using the much rougher (R(q) ∼ 20-30 nm) and less conductive (peak σ(DC)/σ(OP) ∼ 2.5) films formed by common vacuum filtration of the same starting material, and having the same transmittance.

Sorting of Double-Walled Carbon Nanotubes According to Their Outer Wall Electronic Type via a Gel Permeation Method

In this work, we demonstrate the application of the gel permeation technique to the sorting of double-walled carbon nanotubes (DWCNTs) according to their outer wall electronic type. Our method uses Sephacryl S-200 gel and yields sorted fractions of DWCNTs with impurities removed and highly enriched in nanotubes with either metallic (M) or semiconducting (S) outer walls. The prepared fractions are fully characterized using optical absorption spectroscopy, transmission electron microscopy, and atomic force microscopy, and the entire procedure is monitored in real time using process Raman analysis. The sorted DWCNTs are then integrated into single nanotube field effect transistors, allowing detailed electronic measurement of the transconductance properties of the four unique inner@outer wall combinations of S@S, S@M, M@S, and M@M.

Heterojunction Solar Cells Based on Silicon and Composite Films of Polyaniline and Carbon Nanotubes

Composite films of polyaniline (PANI) and single-walled carbon nanotubes have been produced by a simple vacuum filtration process from aqueous solution, and the films have been applied on n-type silicon to form heterojunction solar cells. The performance of devices with the composite electrodes of different constituent ratios and of various film thicknesses has been investigated. It was found that the incorporation of the conducting polymer reduces the sheet resistance of the films, while the overall thickness influences both the conductivity and the amount of light transmitted through to the underlying silicon. By optimizing the composition and thickness of the films, a power conversion efficiency of 7.4% was obtained, which is a 60% increase over that obtained from devices without the polymer. Analysis of the DC electrical to optical conductivity ratios of the various films and comparison of this with the solar cell performance data shows that the improved output is not due solely to better electrical and optical properties but depends strongly on the exact nature of the junction as well, which changes with PANI content.