Density functional theory has been used to investigate cathode materials for rechargeable batteries, carbon nanotube interactions with catalyst particles and transition metal catalyzed hydrogen release in magnesium hydride nanoclusters. An effort has been made to the understand structural and electrochemical properties of lithium iron silicate (Li2FeSiO4) and its manganese-doped analogue. Starting from the X-ray measurements, the crystal structure of Li2FeSiO4 was refined, and several metastable phases of partially delithiated Li2FeSiO4 were identified. There are signs that manganese doping leads to structural instability and that lithium extraction beyond 50% capacity only occurs at impractically high potentials in the new material. The chemical interaction energies of single-walled carbon nanotubes and nanoclusters were calculated. It is found that the interaction needs to be strong enough to compete with the energy gained by detaching the nanotubes and forming closed ends with carbon caps. This represents a new criterion for determining catalyst metal suitability. The stability of isolated carbon nanotube fragments were also studied, and it is argued that chirality selection during growth is best achieved by exploiting the much wider energy span of open-ended carbon nanotube fragments. Magnesium hydride nanoclusters were doped with transition metals Ti, V, Fe, and Ni. The resulting changes in hydrogen desorption energies from the surface were calculated, and the associated changes in the cluster structures reveal that the transition metals not only lower the desorption energy of hydrogen, but also seem to work as proposed in the gateway hypothesis of transition metal catalysis.

The recent breakthroughs in genomics and molecular diagnostics will not be reflected in health-care systems unless the biogenetic or other nucleic acid-based tests are transferred from the laboratory to clinical market. Developments in microfabrication techniques brought lab-on-a-chip (LOC) into being the best candidate for conducting sample preparation for such clinical devices, or point-of-care testing set-ups. Sample preparation procedure consists of several stages including cell transportation, separation, cell lysis and nucleic acid purification and detection. LOC, as a subset of Microelectromechanical systems (MEMS), refers to a tiny, compact, portable, automated and easy-to-use microchip capable of performing the sample-preparation stages together. Complexity in micro-fabrications and inconsistency of the stages oppose integration of them into one chip. Among the variety of mechanisms utilized in LOC for cell lysis, electrical methods have the highest potential to be integrated with other microchip-based mechanisms. There are, however, major limitations in electrical cell lysis methods: the difficulty and high-cost fabrication of microfluidic chips and the high voltage requirements for cell lysis. Addressing these limitations, the focus of this thesis is on realization of cell lysis microchips suitable for LOC applications. We have developed a new methodology of fabricating microfluidic chips with electrical functionality. Traditional lithography of microchannel with electrode, needed for making electro-microfluidic chips, is considerably complicated. We have combined several easy-to-implement techniques to realize electro-microchannel with laser-ablated polyimide. The current techniques for etching polyimide are by excimer lasers in bulky set-ups and with involvement of toxic gas. We present a method of ablating microfluidic channels in polyimide using a 30W CO2 laser. Although this technique has poorer resolution, this approach is more cost effective, safer and easier to handle. We have verified the performance of the fabricated electro-microfluidic chips on electroporation of mammalian cells. Electrical cell lysis mechanisms need an operational voltage that is relatively high compared to other cell manipulation techniques, especially for lysing bacteria. Microelectro-devices have dealt with this limitation mostly by reducing the inter-distance of electrodes. The technique has been realized in tiny flow-through microchips with built-in electrodes in a distance of a few micrometers which is in the scale of cell size. In addition to the low throughput of such devices, high probability of blocking cells in such tiny channels is a serious challenge. We have developed a cell lysis device featured with aligned carbon nanotube (CNT) to reduce the high voltage requirement and to improve the throughput. The vertically aligned CNT on an electrode inside a MEMS device provides highly strengthened electric field near the tip. The concept of strengthened electric field by means of CNT has been applied in field electron emission but not in cell lysis. The results show that the incorporation of CNT in lysing bacteria reduces the required operational voltage and improves throughput. This achievement is a significant progress toward integration of cell lysis in a low-voltage, high-throughput LOC. We further developed the proposed fabrication methodology of micro-electro-fluidic chips, described earlier, to perform electroporation of single mammalian cell. We have advanced the method of embedding CNT in microchannel so that on-chip fluorescent microscopy is also feasible. The results verify the enhancement of electroporation by incorporating CNT into electrical cell lysis. In addition, a novel methodology of making CNT-embedded microfluidic devices has been presented. The embedding methodology is an opening toward fabrication of a CNT-featured LOC for other applications.

This report discuss the developement of a MATLAB-based tool for the analysis ofsurface area coverage of carbon nanotube networks from atomic force microscopyimages. The tool was compared with a manual method and the conclusion was that ithas, at least, the same accuracy as the manual mehtod, and it needs much less time forthe analysis. The tool couldn’t analyze images of carbon nanotube networks if theimages were to noisy or the networks to dense. The tool can help in the research ofthin-film transistors with carbon nanotube networks as the semiconducting channelmaterial.

In this work, carbon nanotubes were deposited onto the insulative glass fibre surface to form a semiconductive network. Utilizing the unique properties of CNTs network, a multifunctional composite interphase could be achieved. The interfacial adhesion strength was improved by CNTs distributed in the interphase. The semiconductive interphase have been used as a chemical/phaysical sensor, strain sensor and microswitch.

<p>The primary goals of this study were to demonstrate and fully characterize a microscale ionization source (i.e. micro-ion source) and to determine the validity of impact ionization theory for microscale devices and pressures up to 100 mTorr. The field emission properties of carbon nanotubes (CNTs) along with Micro-Electro-Mechanical Systems (MEMS) design processes were used to achieve these goals. Microwave Plasma-enhanced CVD was used to grow vertically aligned Multi-Walled Carbon Nanotubes (MWNTs) on the microscale devices. A 4-dimensional parametric study focusing on CNT growth parameters confirmed that Fe catalyst thickness had a strong effect on MWNT diameter. The MWNT growth rate was seen to be a strong function of the methane-to-ammonia gas ratio during MWNT growth. A high methane-to-ammonia gas ratio was selected for MWNT growth on the MEMS devices in order to minimize growth time and ensure that the thermal budget of those devices was met. </p><p>A CNT-enabled microtriode device was fabricated and characterized. A new aspect of this device was the inclusion of a 10 micron-thick silicon dioxide electrical isolation layer. This thick oxide layer enabled anode current saturation and performance improvements such as an increase in dc amplification factor from 27 to 600. The same 3-panel device was also used as an ionization source. Ion currents were measured in the 3-panel micro-ion source for helium, argon, nitrogen and xenon in the 0.1 to 100 mTorr pressure range. A linear increase in ion current was observed for an increase in pressure. However, simulations indicated that the 3-panel design could be modified to improve performance as well as better understand device behavior. Thus, simulations and literature reports on electron impact ionization sources were used to design a new 4-panel micro-ion source. The 4-panel micro-ion source showed an approximate 10-fold performance improvement compared to the 3-panel ion source device. The improvement was attributed to the increased electron current and improved ion collection efficiency of the 4-panel device. Further, the same device was also operated in a 3-panel mode and showed superior performance compared to the original 3-panel device, mainly because of increased ion collection efficiency. </p><p>The effect of voltages applied to the different electrodes in the 4-panel micro-ion source on ion source performance was studied to better understand device behavior. The validity of the ion current equation (which was developed for macroscale ion sources operating at low pressures) in the 4-panel micro-ion source was studied. Experimental ion currents were measured for helium, argon and xenon in the 3 to 100 mTorr pressure range. For comparison, theoretical ion currents were calculated using the ion current equation for the 4-panel micro-ion source utilizing values calculated from SIMION simulations and measured electron currents. The measured ion current values in the 3 to 20 mTorr pressure range followed the calculated ion currents quite closely. A significant deviation was observed in the 20-100 mTorr pressure range. The experimental ion current values were used to develop a corrected empirical model for the 4-panel micro-ion source in this high pressure range (i.e., 3 to 100 mTorr). The role of secondary electrons and electron path lengths at higher pressures is discussed.</p> / Dissertation

<p>Carbon nanomaterials have a wide range of promising and exciting applications. One of the most heavily investigated carbon nanomaterial in recent history has been the carbon nanotube. The intense interest in carbon nanotubes can be attributed to the many exceptional characteristics which give them great potential to revolutionize modern mechanical, optical and electronic technologies. However, controlling these characteristics in a scalable fashion has been extremely difficult. Although some progress has been made in controlling the quality, diameter distribution and other characteristics of carbon nanotube samples, several issues still remain. The two major challenges which have stood in the way of their mainstream application are controlling their orientation and their electronic characteristics. Developing and understanding a Chemical Vapor Deposition based carbon nanotube synthesis method has been the major focus of the research presented here. Although several methods were investigated, including the so-called "fast-heating, slow-cooling" and large feeding gas flowrate methods, it was ultimately found that high-quality, perfectly aligned carbon nanotubes from a variety of metal catalysts could be grown on quartz substrates. Furthermore, it was found that using MeOH could selectively etch small-diameter metallic carbon nanotubes, which ultimately led to the productions of perfectly aligned single-walled carbon nanotube samples consisting almost entirely of semiconducting carbon nanotubes. Thiophene was utilized to investigate and support the hypothesized role of MeOH in producing these selectively gown semiconducting carbon nanotube samples. Additionally, this sulfur-containing compound was used for the first time to demonstrate a two-fold density enhancement in surface grown carbon nanotube samples. This method for selectively producing perfectly aligned semiconducting carbon nanotubes represents a major step towards the integration of carbon nanotubes into mainstream applications.</p><p>Although extremely useful in a variety of technologies, carbon nanotubes have proven impractical for use in H₂ storage applications. As such, microporous carbons have been heavily investigated for such ends. Microporous carbons have distinguished themselves as excellent candidates for H₂ storage media. They are lightweight and have a net-capacity of almost 100%, meaning that nearly all of the H₂ stored in these materials is easily recoverable for use in devices. However, developing a microporous carbon with the appropriately small pore diameters (~1nm), large pore volumes (>1cm<super>3</super>) and large surface areas (&#8805;3000m<super>2</super>/g) has proven exceedingly difficult. Furthermore, maintaining the ideal graphitic pore structure has also been an unresolved issue in many production means. Several microporous carbon synthesis methods were investigated herein, including inorganic and organically templated production schemes. Ultimately, thermally treating poly (etherether ketone) in CO₂ and steam environments was found to produce large surface area porous carbons (&#8805;3000m<super>2</super>/g) with the appropriately small pore diameters (<3nm) and large pore volumes (>1cm<super>3</super>) necessary for optimized storage of H2. Furthermore, the surface chemistry of these pores was found to be graphitic. As a result of these ideal conditions, these porous carbons were found to store ~5.8wt.% H₂ at 77K and 40bar. This represents one of the most promising materials presently under investigation by the United States Department of Energy H₂ Sorption Center of Excellence. </p><p>The success of both of these materials demonstrates the diversity and promise of carbon nanomaterials. It is hoped that these materials will be further developed and will continue to revolutionize a variety of vital technologies.</p> / Dissertation

Disinfectants, such as chlorine, are widely used in water treatment plants to ensure the safety and quality of drinking water. However, these disinfectants easily react with some natural or man-made organic compounds in raw water and form disinfection by-products (DBPs). For example, halogenated acetic acid (HAAs) and trihalomethanes (THMs) are two main components of DBPs. These DBPs contained in drinking water will increase the risk of cancer in human body. Therefore, researches on halogenated acetic acid¡¦s potential of causing cancer have increased currently. Organic acids are usually the reactants which proceed in chlorination reaction into products of disinfection by-products in water treatment plant. The purpose of this study is to investigate adsorption characteristics in solution by using tests of kinetics and equilibrium adsorptions and kinetic model evaluations of selected fulvic acids (FA) extracted from raw water. Therefore, we use commercial single-walled carbon nanotube (SWCNT) for the adsorbents, and calculate thermodynamic parameters (£GG, £GS and £GH) in order to further understand the adsorption mechanism of CNTs. The maximum adsorbed amounts of FA onto SWCNTs was calculated by the Langmuir model at 25¢J, reaching 61.88mg / g which were much higher than that onto commercially available granular activated carbon (10.69 mg/g). The adsorption capacity of FA onto CNTs increased with decreasing outer diameter of CNTs (dp), molecular weight of FA, trmperature and pH value in all texts. In the condition of constant temperature 25¢J, we analyzed HAAFP after the test of equilibrium adsorption and that the removal efficiency of HAAFP could reach 40.76%. The best selection in kinetic models evaluation, fitting models such as Modified Freundlich equation, Pseudo-1st-order equation and Pesudo-2nd-oder equation, is Modified Freundlch equation model. In addition, intraparticle diffusion equation model was fitted well and showed adsorption process was controlled by pore diffusion. We calculated the activation energy of carbon nanotube adsorption of FA and found that film diffusion was the main factor for controlling reaction rate. According to results of thermodynamic parameters indicated that the adsorption was spontaneously and an exothermic reaction. It is obvious that the adsorption capacity as well as the reaction rate of CNTs are superior to that of granular activated carbon in raw water. These results suggest that CNTs possess highly potential applications in environmental protection. In the future, if we can combine nanotube technology with disinfection technology and apply such technique on the end of processing unit for design of either the domestic treatment facilities or small simple water treatment in drinking water. Thus it will enhance the new treatment technology of drinking water and the safety of the public health. Another possibility will be to promote the opportunity of marketing development in drinking water.

Polymer light emitting diodes (PLED) were using a heterocyclic aromatic rigid-rod polymer poly-p-phenylene-benzobisoxazole (PBO) as an opto-electronically active layer; and poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonic acid) (PEDOT:PSS) as a hole transporting layer. Aluminum (Al) and indium tin oxide (ITO) were served as device cathode and anode, respectively. [6,6]-phenyl C61-butyric acid methyl ester (PC61BM) or derivatized multi-wall carbon nano-tube (MWCNT-C18), with great electron transporting ability, was doped into PBO to enhance the performance of PLED devices as well as the thin-film electrical conductivity. The optical length was changed by using different spin coating speeds and durations. From the research, the £fmax of electroluminescence (EL) was blue-shifted as PEDOT:PSS spin coating speed increased for a thinner layer. Once using a higher spin coating speed repeatedly to coat PEDOT:PSS, the £fmax of electroluminescence was red-shifted. If the PEDOT:PSS film thicknesses were similar, the EL spectra were almost the same, independent of device processing scheme. The injection current and EL intensity were enhanced by doping PC61BM or MWCNT- C18. The electric conductivity parallel to film surface (£m¡ü) was increased as the doping concentration increased. Because of the extremely different aspect ratio, the MWCNT-C18 had a lower percolation threshold concentration. Therefore, at a low MWCNT-C18 doping concentration, the injection current and the EL intensity were enhanced compared with those of PC61BM.

We comprehensively investigated the concentration effect of dispersed single-walled carbon nanotubes (SWCNTs) in polymer films for being a saturable absorber (SA) to stabilize the mode locking performance of the Erbium-doped fiber laser (EDFL) pulse through the diagnosis of its nonlinear properties of SA. The measured modulation depth was 1 to 4.5% as the thickness increased from 18 to 265 £gm. We obtained the stable pulse of the mode-locked EDFL (MLEDFL) when the full-width half-maximum (FWHM) decreased from 3.43 to 2.02 ps as the concentrations of SWCNTs SA increased from 0.125 to 0.5 wt%. At constant concentration of 0.125 wt%, the similar pulse shortening effect of the MLEDFL was also observed when the FWHM decreased from 3.43 to 1.85 ps was the thickness of SWCNTs SA increased from 8 to 100 £gm. In EDFL system, we vary group-velocity dispersion (GVD) with different cavity length to achieve optical pulse compression. We got the shortest pulsewidth was 713 fs, and the time-bandwidth product (TBP) was 0.345. An in-depth study on the stable mode-locked pulse formation employing SWCNTs SA, it is possible to fabricate the SWCNT films for use in high performance MLEDFL and utilization of many other low-cost nanodevices.

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