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An analysis of dendritic cooperativity in protein hydrolysis: Author: O'Dell, Jacob Webb; Date: 2005-08-15; Program: Chemistry; Abstract: Catalysts are compounds that increase the rate of a chemical reaction by lowering the activation energy while not being permanently altered. Adding a catalyst to a reaction, while increasing the rate, complicates purification because the catalyst must be separated from the product(s) of the reaction. If the catalyst is a drastically different size than the product then seperation can be achieved as easily as filtering over a membrane. Dendrimers are becoming popular scaffolding for tethering catalysts. Attaching a catalyst to a dendrimer makes a bigger catalytic unit that is easily separated f...; Download File | View full details

Chemical interaction of nitric oxide and human hemoglobin: Author: Luchsinger, Benjamin Peter; Date: 2004-05-15; Program: Chemistry; Abstract: In the past decade an entirely new areas of biomedical science have emerged with the recognition of the critical roles played by nitric oxide (NO) in biology. The discoveries of the role of NO in the cardiovascular systems, where it participates in regulating the tone of blood vessels and the flow of blood, raised an intriguing biochemical problem about the chemical interaction of NO and hemoglobin in blood. Historically, investigation of the interaction of NO and hemoglobin have suggested the formation of heme-Fe(II)NO hemoglobin and nitrate. Neither of these products is considered to exhibit...; Download File | View full details

Development of palladium L-edge X-Ray absorption spectroscopy and its application on chloro palladium complexes: Author: Boysen, Ryan Bradley; Date: 2006-05-15; Program: Chemistry; Abstract: X-ray Absorption Spectroscopy (XAS) is a synchrotron-based experimental technique that can provide information about geometric and electronic structures of transition metal complexes with unoccupied d orbitals. Combination of metal L-edge and ligand K-edge XAS has the potential to define the experimental ground state electronic structure. We developed a quantitative treatment for Pd L-edge spectroscopy based on the already established Cl K-edge XAS for a series of chloro palladium complexes, which are precatalysts in numerous organic transformations. We found that Pd-Cl bonds are highly covale...; Download File | View full details

General Chemistry laboratory for engineers: a research-based approach: Author: Sorey, Timothy Lowell; Date: 2005-12-15; Program: Chemistry; Abstract: Changes made in requirements to the Accreditation Board for Engineering and Technology in 2000 have made it possible for several engineering curricula to take one semester of a two part general Chemistry series. At Montana State University - Bozeman engineering majors constitute just over 37% of the total 850 students per year in the first term general Chemistry population. The single-semester engineering curricula enroll 88% of the engineering students. These students receive an incomplete survey of general Chemistry, missing important topics such as equilibrium and kinetics, acids and bases,...; Download File | View full details

Spin-Label Electron Paramagnetic Resonance Characterization of Heterogeneously Functionalized Dendrimers: Author: Walter, Eric Dale; Date: 2004-05-15; Program: Chemistry; Abstract: Dendrimers are roughly spherical macromolecular polymers that can provide a molecular framework for the attachment of various functionalities. The range of application can be vastly expanded when attached with a heterogeneous mix of functionalities tailored to meet a specific need. The effective application requires the acquisition of several new techniques. First, chemical control of the average ratio of functional groups and analytical methods to determine the ratio. Secondly, a determination of the distribution of ratios. And finally, a method whereby the spatial distribution is determined....; Download File | View full details

Studies on selectivity in the Pauson-Khand reaction and synthesis of an intermediate of isocarbacyclin: Author: Meyer, Todd Roland; Date: 2005-08-15; Program: Chemistry; Abstract: The Pauson-Khand reaction is a highly convergent process that is an efficient way to make substituted cyclopentenones. Some substrates undergo cyclization with high diastereoselectivity while others do not. It was thought that an efficient construction of the bicyclo[3.3.0]octenone core of isocarbacylin could be achieved using the thermal catalytic Pauson-Khand reaction developed in the Livinghouse laboratories in combination with known trends in the diastereoselective features of this reaction. Efforts toward this end are described using two different routes, involving cyclization of a dienyn...; Download File | View full details

Studies of nucleophile ring opening of oxabicyclic systems in highly polar media: application to a total synthesis of antitumor agent, (-)-epothilone: Author: Diep, Nhut Kiet; Date: 2006-08-15; Program: Chemistry; Abstract: Polyketides constitute an important family of natural products, having a broad spectrum of biological activity such as antitumor, antibiotic, antifungal, or immunomodulatory action.¹ Many of these compounds possess polypropionates (units with alternating hydroxyl and methyl groups), reflecting their common biosynthesis that is found within nature. Their structural complexity and importance of these compounds as therapeutical agents have made them attractive targets for synthetic organic chemists.¹ Excellent chiral propionate reagents have been developed over the years, ...; Download File | View full details

Protein Cage Architectures as a Nano-Platform for Material Synthesis and Metal Binding: Author: Allen, Mark Andrew; Date: 2006-08-15; Program: Chemistry; Abstract: Supramolecular proteins that assemble into cage like architectures have been used for nano-material synthesis and as a scaffold for metal binding. Material synthesis can be performed by exploiting the cage-like properties of these nano-containers and relying on the electrostatically distinct interior environment that drive mineral encapsulation. Ferritin and ferritin like proteins can be used as size constrained reaction vessels that encapsulate materials that have sizes that are determined by the internal dimensions of the protein cage. These range from 5 nm for the ferritin like protein from...; Download File | View full details

The synthesis of glycodendrimers and their applications in carbohydrate-protein interactions and catalysis: Author: Morgan, Joel Ryan; Date: 2006-08-15; Program: Chemistry; Abstract: Glycodendrimers were synthesized for studies in carbohydrate-protein interactions, and from these studies we gained insight into the mechanism of some carbohydrate-protein interactions. First, the synthesis of tris-mannose cluster functionalized glycodendrimers of different sizes using a "click Chemistry" approach is described. The macromolecules were characterized using 1H and 13C NMR and MALDITOF MS. Next, a heterogeneous dendrimer functionalization strategy to control the presentation of the carbohydrate clusters around the dendrimer periphery is reported. Nacetyl galactosamine an...; Download File | View full details

Enhancing the antibiotic susceptibility of Pseudomonas aeruginosa biofilms by quorum sensing inhibition: Author: Huff, Caol Philipp; Date: 2006-12-15; Program: Chemistry; Abstract: Biofilm forming bacteria are industrially and medically relevant organisms that are exceptionally resistant to garden variety antimicrobial treatments. This resistance is due in part to a biofilm forming bacteria's ability to sense and communicate with neighboring bacteria. As a result of this intercellular communication, bacteria are able to cooperate as a complex community. This communication system is used to modulate important facets of biofilm behavior and thus is an attractive target for biofilm control and potential antimicrobial agents. Inhibition of the molecular signaling system used...; Download File | View full details

A study of polymeric platinum (II) compounds and nanoscale materials: Author: Anderson, Bernard Marshall; Date: 2004-05-15; Program: Chemistry; Abstract: The photophysical and structural properties of the tetra-u- pyrophosphitodiplatinate (2-) anion have been well studied in the past. One such analogue of this compound is a phosphorescent red compound of unknown structure. A new synthesis route has been was found for both the tetra-u- pyrophosphitodiplatinate (2-) and the red anionic compounds. By synthesizing the pyrophosphorus ligand outright and reacting that with tetrachloroplatinate (2-) either the tetra-u-pyrophosphitodiplatinate (2-) or the red anionic compounds can be synthesized depending on the amount of the phosphorus acid that is pr...; Download File | View full details

Mannose/TEMPO functionalized PAMAM dendrimers: their relative locations and components of affinity toward concanavalin A: Author: Samuelson, Lynn Elizabeth; Date: 2004-05-15; Program: Chemistry; Abstract: Surface functionalized dendrimers are being used for several applications including the study of protein-carbohydrate interactions. Mannose-functionalized dendrimers with varying concentrations of saccharides on the dendrimer surface were synthesized. Spin labels (2,2,6,6-tetramethylpiperidine N-oxide) were incorporated onto the dendrimer's surface as well. Linebroadening effects in the EPR spectra of these compounds allowed us to determine the distance between spin labels (and thus between carbohydrates). The mannose-spin labeled functionalized dendrimers were further studied to determine eff...; Download File | View full details

Molecular Beam Studies of Hyperthermal Atomic Oxygen and Argon Interactions with Polymer Surfaces and Gas-Phase Molecules: Author: Brunsvold, Amy Leigh; Date: 2007-05-15; Program: Chemistry; Abstract: O atoms and N2 molecules in the outer atmosphere of the Earth collide with spacecraft surfaces and various gases that are released from space vehicles. The high relative velocity of the collisions promotes high reaction probability and large energy transfers, leading to materials degradation and chemiluminescent reactions, which may interfere with the mission of the vehicle. The work presented in this thesis uses sophisticated molecular beam and surface science techniques to study materials degradation and individual reactive and inelastic collisions in an effort to understand the complex chem...; Download File | View full details

Palladium (II)-catalyzed stereoselective formation of alpha-O-Glycosides: Author: Schuff, Brandon Patrick; Date: 2007-05-15; Program: Chemistry; Abstract: The development of new methods for stereoselective formation of alpha- or beta-O-glycosides has been extensively investigated due to the critical roles carbohydrates play in a variety of biological systems. To date, many efforts have focused on developing new methods and reagents for the generation of isolated glycosyl donors which subsequently undergo glycosidic bond formation with nucleophilic glycosyl acceptors. Despite their potential applications to complex carbohydrate synthesis, each of these methods relies on the nature of the substrates to stereoselectively control the formation of gl...; Download File | View full details

Design and synthesis of dendrimers for studying two-photon absorption characteristics: Author: Sims, Michael Keith; Date: 2007-05-15; Program: Chemistry; Abstract: While entering a technologically advanced world, where inventions of weapons occur rapidly, there is a constant need for research leading up to and preventing these weapons from being harmful. The use of lasers as an eye-damaging agent is one such weapon that requires the construction of good optical limiting materials that combat the harmful effects of these lasers. Optical power limiting materials should have the capability to respond quickly as well as span a large frequency range. Over the last two years, research has been conducted on the synthesis and absorption characteristics of new de...; Download File | View full details

Application of proton transfer reaction mass spectrometry to measure hydrocarbon emissions in engine exhaust: Author: Rogers, Todd Michael; Date: 2007-08-15; Program: Chemistry; Abstract: Megacities around the world face air quality problems due to exhaust emissions from large vehicle fleets. Chemical reactions involving volatile organic compounds (VOC) from automobile exhaust are known to produce ground level ozone which poses a threat to human health and plant life. Additionally, some of these organic compounds are known carcinogens. While the dangers of VOC are well known, their production from in use vehicles and aircraft are relatively poorly understood. This dissertation will describe how a Proton Transfer Reaction Mass Spectrometer (PTR-MS) was altered to make the first ...; Download File | View full details

Biomimetic synthesis of catalytic materials: Author: Varpness, Zachary Bradley; Date: 2007-08-15; Program: Chemistry; Abstract: Supramolecular proteins assemblies have been used as platforms for the synthesis of catalytic nanomaterials. These supramolecular structures are assembled from a limited number of subunits that provide a unique structurally defined platform for the synthesis of catalytic nanomaterials. Small heat shock protein (Hsp) and ferritin (Fn) are 12 nm protein cage-like assemblies of 24 subunits that have been used as platforms for the synthesis of noble metal nanoparticles through the in vitro reduction of corresponding ions. Protein encapsulated metal nanoparticles were used as catalysts for photoche...; Download File | View full details

Spin-Label Electron Paramagnetic Resonance Investigation of PAMAM Dendrimer End-Group Structure and Dynamics: Author: Sebby, Karl Bernell; Date: 2007-12-15; Program: Chemistry; Abstract: PAMAM dendrimers are nanoparticles containing a series of branching units emanating from an ethylene diamine initiator core. Control of the number of branching units during synthesis results in monodisperse macromolecules with a specified, but variable, number of terminal branches, to which various functionalities can be attached. The ability to attach large numbers of functional groups, in controlled ratios, to the dendrimer end-groups makes dendrimers attractive templates for a variety of applications. For example, partially glycosylated dendrimers are being explored as multivalent ligands f...; Download File | View full details

Design and synthesis of fluorescent dyes for use in proteomic research: Author: Spicka, Kevin James; Date: 2008-08-15; Program: Chemistry; Abstract: Proteomics is a rapidly developing field requiring powerful new technology in order to be able to detect proteins at increasingly lower concentrations. To aid in the detection of proteins at lower concentrations, DIGE dyes, a family of spectrally resolved fluorescent dyes, are currently available to proteomic researchers for 2D gel analysis. However, the demands of protein detection dictate that dyes that are even more sensitive and versatile be created. The syntheses of highly sensitive, water soluble BODIPY fluorophore dyes are described. These dyes are proposed to have the necessary sensiti...; Download File | View full details

The use of In(OTf)3 as a Lewis Acid in carbohydrate Chemistry, and exploration in silicon tethered reactions: Author: Bizier, Nicholas Paul; Date: 2008-12-15; Program: Chemistry; Abstract: The feasibility of using Indium (III) triflate as a Lewis Acid for a number of different carbohydrate reactions was explored. First, the use of In(OTf)3 as a catalyst in the acylation of a number of carbohydrates was explored. The utility and compatibility of the In(OTf)3 reaction conditions with a number of protecting groups on the sugars were examined by 1H NMR analysis. In the second part of the carbohydrate methodology, the feasibility of using In(OTf)3 to promote glycosylation reactions using a number of glycosyl donors was evaluated. These studies were conducted using 1H NMR, 13CNMR, and...; Download File | View full details

Exogenous ligand effects on S-nitrosohemoglobin formation in reactions of methemoglobin with nitric oxide: Author: Mellmann, Lisa Jean; Date: 2009-05-15; Program: Chemistry; Abstract: Blood's function of carrying oxygen to tissues is regulated by physiological oxygen gradients that are coupled to vasoconstriction and vasodilation by nitric oxide bioactivity. However, the mechanism by which local oxygen tension utilizes nitric oxide signaling in order to regulate blood flow remains a major unanswered question in biology. Hemoglobin in red blood cells appears to be an ideal sensor, but lack of knowledge about hemoglobin's Chemistry with nitric oxide creates a problem for understanding how hemoglobin induces vasodilation. A central focus of this work was to illuminate complexi...; Download File | View full details

Quantitative prediction of dye fluorescence quantum yields in proteins: Author: Hutcheson, Ryan Mitchell; Date: 2009-05-15; Program: Chemistry; Abstract: The application of a method previously developed by Callis et al. to predict the quantum yields of Trp fluorescence has been successfully applied to the fluorescence of fluorescein and flavins in proteins. The calculated lifetime range of 2 ps - 4 ns is in agreement with experiment. The fluctuations in the electron transfer rate are shown to be dictated by the fluctuations in the density of states. This is evident by the comparison of the fractional deviation of the interaction, density of states and the rate. Here the fluctuations in the density of states is an order of magnitude larger than ...; Download File | View full details

Using PAMAM dendrimer frameworks to investigate multivalent binding in protein-carbohydrate interactions: Author: Wolfenden, Mark Leroy; Date: 2009-12-15; Program: Chemistry; Abstract: Polyvalent interactions in biological systems have been of great interest recently; how nature creates high affinity polyvalent binding with low monomeric affinity, is yet to be clearly understood. We have created a bivalent lectincarbohydrate binding system using dendrimers as the carbohydrate mounted scaffold and Concanavalin A (Con A) as the mannose/glucose binding lectin to investigate this mode of interaction. The relative affinities of the utilized carbohydrates toward Con A are: mannose binds 4 times stronger than glucose, and galactose shows no affinity. With these relative affinities ...; Download File | View full details

Exploring the potential of protein cages as MRI contrast agents with an emphasis on protein cage characterization by mass spectrometry techniques: Author: Liepold, Lars Otto; Date: 2009-12-15; Program: Chemistry; Abstract: Described here is the development of a protein cages as efficient and potentially relevant MRI contrast agents. Three approaches are outlined to fuse high affinity Gd³⁺ chelating moieties to the surfaces of protein cages. In the first approach, a metal binding peptide has been genetically engineered into the subunit of Cowpea chlorotic mottle virus (CCMV) and to the small heat shock protein cage from Methanococcus jannaschii (HSP). The genetic fusion resulted in a 200x binding enhancement of Gd³⁺ to CCMV in comparison with wild type CCMV and me...; Download File | View full details

The synthesis of fluorescent and phosphorescent dyes for biochemical application: Author: Sanger, Elizabeth Ann; Date: 2010-05-15; Program: Chemistry; Abstract: Current dyes for proteomics that are applicable to multiplexing experiments suffer from lack of sensitivity and poor water solubility. A series of tetramethyl rhodamine derivatives were developed to study the effects of substitution patterns on the photophysical properties of the fluorophores. After identifying the superior fluorophore a zwitterionic side chain with properties beneficial for two dimensional applications was coupled to the fluorophore and the photophysical properties were studied. Iridium(III) cationic fluorophores are interesting synthetic targets due to their ultraviolet abso...; Download File | View full details

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