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Metal-Organic Frameworks and Graphene-Based Support Materials for Heterogeneous CatalysisLin, Andrew 01 January 2018 (has links)
Nanoparticles are involved in a broad range of applications, including heterogeneous catalysis. Nanoparticles tend to quickly lose their well-defined shapes and facets due to aggregation under duress such as heat.
A series of highly studied materials are explored as support materials for nanoparticle supports. These supports include metal-organic frameworks (MOF), graphene oxide (GO), and a MOF-PRGO (partially reduced graphene oxide) hybrid. The inclusion of a support with the palladium increased lifespan of the catalyst by separation of nanoparticles. The choice of support material not only allowed for supporting of palladium nanoparticles, but allowed for rational catalyst synthesis in order to design catalysts with improved catalytic activity.
CO oxidation, vanillin hydrogenation, and Suzuki cross coupling were studied. For the CO oxidation reaction, a cerium-based MOF, Ce-MOF, is shown to increase activity of palladium nanoparticles by capturing reactant gases and acting as an oxygen reservoir that cycles between (III) and (IV) states while transferring oxygen to palladium nanoparticles at the Pd/Ce-MOF interface. A hybrid Ce-MOF-PRGO was synthesized to increase the surface area and acidity of Ce-MOF materials and was shown to be active for vanillin hydrogenation. Smaller rod-like Ce-MOF crystals were observed, indicating intercalation of crystals on GO. Zirconium-based MOF UiO-66-NH2 was acidified via incorporation of tungstophosphoric acid (HPW), which increased the selectivity of products by adjusting the mechanistic pathway. GO was partially functionalized with aromatic amines to improve the coupling of bromobenzene and phenylboronic acid. Small amounts of aromatic amines increased the Pd(0) content and decreased nanoparticle size.
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Single-Step Biofriendly Synthesis of Surface Modifiable, Near-Spherical Gold Nanoparticles for Applications in Biological Detection and CatalysisBadwaik, Vivek D. 01 August 2011 (has links)
There is an increased interest in understanding the toxicity and rational design of gold nanoparticles (GNPs) for biomedical applications in recent years. Such efforts warrant reliable, viable, and biofriendly synthetic methodology for GNPs with homogeneous sizes and shapes, particularly sizes above 30 nm, which is currently challenging. In the present study, an environmentally benign, biofriendly, singlestep/ single-phase synthetic method using dextrose as a reducing and capping agent in a buffered aqueous solution at moderate temperature is introduced. The resulting GNPs are near-spherical, stable, catalytically active, place exchangeable, and water-soluble within the size range of 10-120 nm. The added advantage of the biologically friendly reaction medium employed in this new synthetic approach provides a method for the direct embedment/integration of GNPs into biological systems such as the E. coli bacterium without additional capping ligand or surface modification processes.
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Mercury Transportation in Soil Using Gypsum from Flue Gas Desulphurization Unit in Coal-Fired Power PlantWang, Kelin 01 July 2012 (has links)
This work investigates mercury flux in soil amended by gypsum from flue gas desulphurization (FGD) units of coal-fired power plants. There are two phases of this research, including field and greenhouse studies. Previous studies indicate that FGD gypsum could increase corn yield, but may lead to more mercury uptake by corn.
Recent studies have been carried out in greenhouses to investigate mercury transport in FGD gypsum treated soil. Major aspects include uptake of mercury by plants and emission of mercury into the atmosphere based on application rates of FGD gypsum. Additional aspects include rainfall, temperature, soil, and plants types. Higher FGD gypsum application rates generally led to higher mercury concentration in the soil, as well as, increased mercury emission into the atmosphere, and increased mercury levels in plants, especially roots and leaves. Soil properties and plant species also played important roles in mercury transport. In addition, it was also found that increased water and higher temperatures may contribute to mercury emission in the atmosphere.
Some plants, such as tall fescue, were able to prevent mercury from atmospheric emission and infiltration within the soil. Mercury concentration in the stem of plants was found to be increased and then plateaued upon increasing FGD gypsum application. However, mercury in roots and leaves was generally increased upon increasing FGD gypsum application rates. Some mercury was likely absorbed by leaves of plants from mercury in the surrounding atmosphere.
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Corrosion properties of aluminium alloys and surface treated alloys in tap waterGustafsson, Sofia January 2011 (has links)
The aim of this thesis is to obtain a basic knowledge of the factors that affect corrosion of aluminium in tap water for different kinds of applications like water pipes for tap water, solar systems, HVAC&R-applications (like fan coil units on chillers) and heat sinks for electronic or industrial applications. Open systems are used in some applications and closed systems in others. There is a clear difference in the corrosion behaviour of these two systems. The main reasons for this difference are that the content of oxygen differs between the two systems and also that inhibitors can be used in closed systems to hinder corrosion. In this thesis focus will be on corrosion in open systems. The corrosion properties in tap water for different alloys of aluminium and different surface treatments have been examined. The influences on corrosion of the oxygen content in water and the iron content in aluminium alloys have been investigated. The corrosion properties of an aluminium alloy in deionised water have also been examined.
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Kinetic Studies of the Sulfoxidation of Aryl Methyl Sulfides by Trans-Dioxoruthenium(VI) Porphyrin ComplexesAbebrese, Chris 01 December 2009 (has links)
The development of an efficient, catalytically active, biomimetic model for cytochrome P-450 enzymes has been an area of intense research activity. Ruthenium porphyrin complexes have been the center of this research and have successfully been utilized, as catalysts, in major oxidation reactions such as the hydroxylation of alkanes, the epoxidation of alkenes and aromatic rings, and the N-oxidation of amines, among others. In this project, the kinetics of two-electron sulfoxidation of para-substituted phenyl methyl sulfides to the corresponding sulfoxides with well-characterized trans-dioxoruthenium(VI) porphyrin complexes were studied by rapid stopped-flow spectroscopy. The substituent effect in sulfides and in dioxoruthenium(VI) complexes were also kinetically investigated. The low-reactive trans-dioxoruthenium(VI) porphyrin complexes (3a-b) were synthesized from the oxidation of their carbonylruthenium(II) porphyrin precursors with m-chloroperoxybenzoic acid (m-CPBA) and characterized spectroscopically by 1H-NMR, IR, and UV-vis. The low-reactivity of these complexes makes them suitable for kinetic studies. The sulfoxidation with the trans-dioxoruthenium(VI) species followed a pseudo-first order kinetic decay from RuVI to RuIV species with no accumulation of intermediates. The reactivity order in the series of dioxoruthenium(VI) complexes follows 3b > 3a >3c, which is consistent with expectations based on the electrophilic nature of high-valent metal-oxo species. Steric effect of the substituents on the complexes also affected the reactivity order. The kinetic results revealed that the sulfoxidation reaction with these well-characterized dioxoruthenium(VI) complexes is 3 – 4 orders of magnitude faster than the epoxidation reaction with the same complexes under similar conditions.
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Catalyst loaded porous membranes for environmental applications : Smart MembranesRen, Bin January 2007 (has links)
<p>This project involves the fabrication and testing of microporous, polymer membranes designed to remove minute amounts of toxic air pollutants such as formaldehyde from air streams. The hypothesis to be tested is that active, the silver contained within the porous polymer membranes results in high formaldehyde retention.</p><p>Monolayers consist of different sizes of sPS particles are assembled first on the silicon wafers by spin coating method and convective assembly method, respectively. Then each kind of monolayer with one dimension of sPS particles is deposited with a nanometer scaled silver thin film with a bench top metal evaporator. The porous membranes are produced by assembly of close-packed colloidal crystals of silver capped polystyrene template particles and subsequent infiltration with polyurethane prepolymer. The prepolymer is cured by UV exposure. The sPS particles are removed from the particle polymer membrane by treatment with organic solvents resulting in the formation of inverse opal structures. Silver does not dissolve in the organic solvents and cannot leave the pores due to the small size of connecting holes in an inverse opal. All the monolayers, cylindrical colloidal crystals and microcapillaries after infiltration of polyurethane had been characterized by optical microscope, and the porous membranes had been characterized by SEM.</p><p>The application of porous membranes with silver caps is to absorb formaldehyde in the air, while in fact the silver caps are oxidized and become Ag2O, which will initiate a gas-phase/solid reaction with formaldehyde. In the future, TiO2 will be applied together with Ag2O, since TiO2 is another good absorbent for formaldehyde</p>
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Polymer Nanocomposite Analysis and Optimization for Renewable Energy and MaterialsHenry, Nathan Walter 01 December 2011 (has links)
Polymer nanocomposites are an important research interest in the area of engineering and functional materials, including the search for more environmentally materials for renewable energy and materials. The ability to analyze and optimize morphology is crucial to realizing their potential, since the distribution of materials in the composite strongly influences its properties. This dissertation presents research into three different polymer nanocomposite systems with three different applications that underscore the need to understand and control the composite morphology to succeed.
The first project details work on development of a copolymer compatibilizer to enhance the dispersion of the plant-derived biopolymer lignin in composite blends with polystyrene. The copolymer was designed with hydroxyl functionality that can form hydrogen bonds with lignin, and the effect of modulating the density of these groups was investigated, both on bulk dispersion and interfacial mixing.
The second project presented concerns resolving the interfacial morphology of composite bulk heterojunction organic photovoltaic devices based on a polythiophene-based photoactive polymer and a modified carbon fullerene, which are archetypical of the highest performing cells yet produced. Neutron reflectivity was extensively employed to probe the interfacial width and degree of intermixing between the components to elucidate the morphological impact on device performance.
The final project involves modifying nanoscale cellulose crystallites, dubbed nanowhiskers, by replacing a portion of the hydroxyl groups with acetate groups to improve their dispersion in polymethyl methacrylate. Neutron reflectivity was again employed to probe the interface between the two materials to observe and quantify intermixing.
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Photocuring of multifunctional monomers initiated by camphorquinone/amine systems for application in dental restorative resins /Nie, Jun, January 1900 (has links)
Diss. (sammanfattning) Stockholm : Karol. inst. / Härtill 5 uppsatser.
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Μελέτη των τριαδικών συστημάτων Zn(II)/RCO2-/N-Δότες: συμβολή σε θέματα βιοανόργανης χημείας και χημείας μοριακών υλικώνΛαλιώτη, Νικολία 15 March 2010 (has links)
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Μοντελοποίηση βιολογικών δράσεων Zn(II) και Cd(II)Κατσουλάκου, Ευγενία Κ. 04 August 2010 (has links)
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