Department of Advanced Materials Science and Engineering, Kangwon National University, Chuncheon, Gangwon-do, Republic of Korea.
Nanotechnology. 2012 Mar 16;23(10):105607. doi: 10.1088/0957-4484/23/10/105607. Epub 2012 Feb 24.
The electronic, physical and optical properties of single-walled carbon nanotubes (SWNTs) are governed by their diameter and chirality, and thus much research has been focused on controlling the diameter and chirality of SWNTs. To date, control of the catalyst particle size has been thought to be one of the most promising approaches to control the diameter or chirality of SWNTs owing to the correlation between catalyst particle size and tube diameter.In this study, we demonstrate the size engineering of catalytic nanoparticles for the controlled growth of diameter-specified and horizontally aligned SWNTs on quartz substrates. Uniformly sized iron nanoparticles derived from ferritin molecules were used as a catalyst, and their size was intentionally decreased via thermal heat treatment at 900 °C under atmospheric Ar ambient. ST-cut quartz wafers were used as growth substrates in order to elucidate the effect of the size of the nanoparticles on the tube diameter and the effect of catalyst size on the degree of parallel alignment on the quartz substrates. SWNTs grown by chemical vapor deposition using methane as feedstock exhibited a high degree of horizontal alignment when the particle density was low enough to produce individual SWNTs without bundling. Annealing for 60 min at 900 °C produced a reduction of nanoparticle diameter from 2.6 to 1.8 nm and a decrease in the mean tube diameter from 1.2 to 0.8 nm, respectively. Raman spectroscopy results corroborated the observation that prolonged heat treatment of nanoparticles yields thinner tubes with narrower size distributions. The results of this work suggest that straightforward thermal annealing can be a facile way to obtain uniform-sized SWNTs as well as catalytic nanoparticles.
单壁碳纳米管 (SWNTs) 的电子、物理和光学性质由其直径和手性决定,因此,大量研究集中在控制 SWNTs 的直径和手性上。迄今为止,由于催化剂颗粒尺寸与管直径之间存在相关性,控制催化剂颗粒尺寸被认为是控制 SWNTs 直径或手性的最有前途的方法之一。在本研究中,我们展示了催化纳米粒子的尺寸工程,用于在石英衬底上控制生长具有指定直径和水平排列的 SWNTs。使用来自铁蛋白分子的均匀尺寸的铁纳米粒子作为催化剂,并在大气 Ar 环境下于 900°C 进行热热处理以有意减小其尺寸。使用 ST 切割石英晶片作为生长衬底,以阐明纳米粒子的尺寸对管直径的影响以及催化剂尺寸对石英衬底上平行排列程度的影响。使用甲烷作为原料通过化学气相沉积生长的 SWNTs 表现出高度的水平排列,当粒子密度足够低以产生没有缠结的单个 SWNTs 时。在 900°C 下退火 60 分钟会导致纳米粒子直径从 2.6nm 减小到 1.8nm,平均管直径从 1.2nm 减小到 0.8nm。拉曼光谱结果证实了这样的观察结果,即纳米粒子的长时间热处理会产生更细的管,且尺寸分布更窄。这项工作的结果表明,简单的热退火可以是获得均匀尺寸的 SWNTs 以及催化纳米粒子的一种简便方法。