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We report the fundamental dependence of thermal diffusivity and electrical conductance on the diameter and defect level for vertically aligned single-walled carbon nanotube (SWCNT) forests. By synthesizing a series of SWCNT forests with continuous control of the diameter and defect level over a wide range while holding all other structures fixed, we found an inverse and mutually exclusive relationship between the thermal diffusivity and the electrical conductance. This relationship was explained by the differences in the fundamental mechanisms governing each property and the optimum required structures. We concluded that high thermal diffusivity and electrical conductance would be extremely difficult to simultaneously achieve by a single SWCNT forest structure within current chemical vapor deposition synthetic technology, and the "ideal" SWCNT forest structure would differ depending on application.

We report a new direction for highly efficient carbon nanotube (CNT) synthesis where, in place of conventional highly reactive carbon feedstocks at low concentrations, highly stable carbon feedstocks at high concentrations were shown to produce superior yields. We found that a saturated hydrocarbon that is considered to possess a low reactivity, delivered at high concentrations, could achieve an extremely high growth yield (2.5 times that when using ethylene). This result stems from the unique behavior where the CNT yield linearly increased with carbon concentration, in contrast to more reactive carbon feedstocks, where the yield peaks. We propose that the mechanisms for the growth kinetics for high- and low-reactivity carbon feedstocks are fundamentally different, where the latter benefits from a longer catalyst lifetime because of a relatively low production rate of carbon impurities.

Alignment represents an important structural parameter of carbon nanotubes (CNTs) owing to their exceptionally high aspect ratio, one-dimensional property. In this paper, we demonstrate a general approach to control the alignment of few-walled CNT forests from nearly random to nearly ideally aligned by tailoring the density of active catalysts at the catalyst formation stage, which can be experimentally achieved by controlling the CNT forest mass density. Experimentally, we found that the catalyst density and the degree of alignment were inseparably linked because of a crowding effect from neighboring CNTs, that is, the increasing confinement of CNTs with increased density. Therefore, the CNT density governed the degree of alignment, which increased monotonically with the density. This relationship, in turn, allowed the precise control of the alignment through control of the mass density. To understand this behavior further, we developed a simple, first-order model based on the flexural modulus of the CNTs that could quantitatively describe the relationship between the degree of alignment (HOF) and carbon nanotube spacing (crowding effect) of any type of CNTs.

A novel system for fractionating single wall carbon nanotubes (SWCNTs) by length via a three-step cross-flow filtration has been developed in which three membrane filters of different pore sizes, 1.0, 0.45, and 0.2 microm, were used. SWCNTs dispersed in water with the help of sodium carboxymethylcellulose (CMC) detergents were successfully sorted into four samples, and the atomic force microscopy (AFM) observation of those samples confirmed that their length distribution peaks are within the expected ranges from pore sizes of used filters. However, the result of the similar filtration process using a different detergent, sodium dodecylbenzenesulfonate (SDBS), showed no pronounced correlation between the length distribution of SWCNTs and the pore size. The observed difference in the sorting phenomena caused by the detergent type suggests that the permeation property depends on the complex structure resulting from the dispersed SWCNTs and detergent molecules.

A gas shower system was introduced to improve the growth of single-walled carbon nanotube (SWNT) forests by controlling the gas flow direction. Delivery of gases from the top of the forest enabled direct and precise supply of ethylene and water vapor to the Fe catalysts. As such, this approach solved one of the limiting factors of water-assisted chemical vapor deposition method (CVD), that is, delivery of the very small optimum water level to the catalysts. Consequently, this approach improved SWNT forests growth stability, uniformity, reproducibility, carbon efficiency (32%), and catalyst lifetime. With this improved growth, we could synthesize a 1 cm tall forest with 1 x 1 cm size. Also we employed this approach to grow an A4 size SWNT forest to highlight the scalability of water-assisted CVD.