Flame synthesis of carbon nanotubes and metallic nanomaterials
Name
54910394-MIT.pdf
Description
Full printable version
Size
137.85 MB
Format
Adobe PDF
Checksum (MD5)
5753979aca2480d9545628a4745d1056
Author(s)
Height, Murray John, 1975-
Advisor(s)
Jack B. Howard and Jefferson W. Tester.
Date Issued
2003
Publisher
Massachusetts Institute of Technology
Abstract
Carbon nanotubes are a remarkable material with many appealing properties. Despite the appeal of this material, there are few synthesis techniques capable of producing nanotubes in large quantities at low-cost. The broad objective of this study was to examine the potential of a premixed flame for the synthesis of carbon nanotubes with the view that flame synthesis may prove a means of continuous production at low-cost. The specific approach focused on the formation of metallic nanoparticles in flames; identification of nanotube formation zones, time scales, and transition conditions; characterization of material properties; and the development of a formation mechanism and associated flame-model. Carbon nanotube formation requires a source of carbon, a source of heat and the presence of metal particles. A fuel-rich flame is a high-temperature, carbon-rich environment and addition of metal is likely to give conditions suitable for nanotube growth. This study considered a premixed acetylene/oxygen/15 mol% argon flame doped with iron pentacarbonyl (Fe(CO)₅) vapor (typically 6100 ppm), operated at 50 Torr pressure and 30 cm/s cold gas feed velocity. The flame was investigated with regard to the growth of metal particles and subsequent formation and growth of carbon nanotubes. Thermophoretic samples were extracted from the flame at various heights above burner (HAB) and analyzed using transmission electron microscopy (TEM). HAB is representative of residence time in the flame. Size distribution and number density data were extracted from TEM images using a quantitative image analysis technique. The mean particle size for a precursor concentration of 6100 ppm was observed to increase from around 2 to 4 nm between 20 and 75 mm HAB.
(cont.) The particle number density results showed a decreasing number density with increasing HAB, giving a complementary picture of the particle dynamics in the flame. Single-walled carbon nanotubes (SWNT) were also observed to form in the premixed flame. Thermophoretic sampling and TEM analysis gave insight into nanotube formation dynamics. Nanotube structures were observed to form as early as 30 mm HAB (20 ms) with growth proceeding rapidly within the next 10 to 20 mm HAB. The growth-rate for the nanotubes in this interval is estimated to be between 10 and 100 ptm per second. The upper region of the flame (50 to 70 mm HAB; 35 to 53 ms) is dominated by tangled web structures formed via the coalescence of individual nanotubes formed earlier in the flame. The nanotube structures are exclusively single-walled with no multi-walled nanotubes observed in any of the flame samples. The effect of carbon availability on nanotube formation was tested by collecting samples over a range of fuel equivalence ratios at fixed HAB. The morphology of the collected material revealed a nanotube formation 'window' of 1.5 < < 1.9, with lower dominated by discrete particles and higher favoring soot-like structures. These results were also verified using Raman spectroscopy. A clear trend of improved nanotube quality (number and length of nanotubes) is observed at lower . More filaments were observed with increasing concentration, however the length (and quality) of the nanotubes appeared higher at lower concentrations ...
Description
Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemical Engineering, 2003.
Includes bibliographical references.
Subjects
Chemical Engineering.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
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