Document Type
Dissertation
Date of Award
Summer 8-31-2007
Degree Name
Doctor of Philosophy in Chemical Engineering - (Ph.D.)
Department
Chemical Engineering
First Advisor
Zafar Iqbal
Second Advisor
Joseph W. Bozzelli
Third Advisor
Laurent Simon
Fourth Advisor
Reginald Farrow
Fifth Advisor
Frank J. Owens
Sixth Advisor
Jing Wu
Abstract
The first phase of the work presented in this dissertation is the development of a scaleable process for the cost-effective synthesis of single walled carbon nanotubes (SWNTs) by thermally-induced catalytic chemical vapor deposition (CVD). With the goal of understanding the growth mechanism and optimize the synthesis process, the effect of CVD and catalyst parameters on nanotube formation was investigated in detail. It was found that nucleation and growth of SWNTs occurred within a few seconds of the introduction of the carbon source, carbon monoxide, at temperatures above 675°C over a Co-Mo/MgO catalyst/support system, resulting in the formation of high quality thinly bundled SWNTs with a narrow individual nanotube diameter distribution. A simple kinetic model is proposed to explain the observed growth and exit gas (CO2) concentration data. A scaled up run using fluidized bed reactor is performed to demonstrate large SWNTs production.
In the second phase of the research performed some of the CVD parameters optimized for the synthesis of pure nanotubes were used to infiltrate SWNTs as well as multiwalled carbon nanotubes (MWNTs) into catalyst precursor filled iron and aluminum matrices, respectively, to directly fabricate metal-nanotube composites. Two carbon sources, carbon monoxide and acetylene were used for the synthesis of SWNTs and MWNTs, respectively. The yield strength of iron-carbon nanotube composites showed substantial enhancement of up to 45% and 36 % with 1 wt % of infiltrated SWNTs and MWNTs, respectively, relative to that of similarly treated pure iron samples of the same piece density without carbon nanotubes. Vickers hardness measurements showed an increase of 74% and 96% for iron composites filled with SWNTs and MWNTs, respectively. The use of a mixed feed of CO and acetylene resulted in carbide-free fabrication of the nanocomposites. A reaction mechanism supporting the observed carbide-free growth is also presented.
In the third phase of the research performed, a SWNT fabrication protocol using CVD growth or electrophoretic deposition was employed for integrating nanotubes as biosensor and chemical gas sensor probes. For biosensor probes, vertically aligned SWNTs were grown or deposited on metal interconnects (Cr/Co), at precise locations, which were patterned on quartz substrates using photo- and e-beam Iithogrpahy to make electrical connections to each SWNT/bundle individually. Gas sensor probes were fabricated using individually suspended SWNTs contacted by Cr/Au pads as source and drain field effect transistor components for the monitoring of NO2 vapors. The adsorption of an electron donating gas such as NO2 on the SWNT sidewalls shifts the Fermi level of the p-type semiconducting nanotubes, consequently changing their electrical conductivity. Experimental results showed that sensor response to NO2 (at 10-300 ppm levels) was of the order of a few seconds at 100 ppm, and was reversible and reproducible. Recovery of the sensor response was achieved by heating the sensors at 120 °C for a period of 10-12 hours indicating physisorption of the NO2 molecules on the nanotube sidewalls.
Recommended Citation
Goyal, Amit, "New approaches to scaled-up carbon nanotube synthesis and nanotube-based metal composites and sensors" (2007). Dissertations. 829.
https://digitalcommons.njit.edu/dissertations/829
