Surface chemistry of metal catalyst under carbon nanotube growth conditions.

摘要

The catalyst nanoparticle is critical to the yield, type, and diameter in the growth and nucleation of carbon nanotubes. The objective of this study is focused on determining what changes take place with the catalyst chemistry under growth conditions typically seen in chemical vapor deposition, CVD, experiments. It is well known that catalyst poisoning can occur and in turn effects the catalytic activity of the nanoparticle. A complete description of this mechanism is as of yet undetermined. In order to elucidate this process iron films were deposited onto Si substrates that contained a support layer of Al2O3 or SiO2. These samples were investigated with various surface chemistry techniques such as X-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES), and electron energy loss spectroscopy (EELS). In addition, structural characteristics were investigated with scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The surface techniques were used in-situ in order to observe chemistries that might not be observable outside a CVD reactor. Two sets of experiments were performed on the silica and alumina supports. The first consisted of carbon nanotube growth at near atmospheric pressure, while the second was performed under vacuum. The oxide support was shown to have an affect on the type of nanotubes grown under identical conditions. The silica support films produced more MWNT, while the alumina support films produced more SWNT. This difference was due to the amount of ripening that takes place on the oxide supports. Also in-situ XPS revealed differences in the chemistry of iron catalyst during growth and these differences were attributed to substrate interactions between alumina and iron. Finally, in-situ XPS analysis showed no evidence of carbides or oxides acting as a catalyst during the nucleation process.