Dissertations / Theses: 'Organic Chemistry'

1

Stenta, Marco <1979&gt. "Computational models in organic and bio-organic chemistry." Doctoral thesis, Alma Mater Studiorum - Università di Bologna, 2008. http://amsdottorato.unibo.it/1069/1/Tesi_Stenta_Marco.pdf.

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Stenta, Marco <1979&gt. "Computational models in organic and bio-organic chemistry." Doctoral thesis, Alma Mater Studiorum - Università di Bologna, 2008. http://amsdottorato.unibo.it/1069/.

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3

Fisher, Grant Andrew. "Model construction in organic chemistry." Thesis, University of Leeds, 2003. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.401068.

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4

Yang, Hongfang. "Benzotriazole intermediates in organic chemistry." [Gainesville, Fla.] : University of Florida, 2004. http://purl.fcla.edu/fcla/etd/UFE0005743.

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5

Kulkarni, S. Y. "Analytical methods in organic chemistry." Thesis(Ph.D.), CSIR-National Chemical Laboratory, Pune, 1985. http://dspace.ncl.res.in:8080/xmlui/handle/20.500.12252/3241.

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6

Goei, Elisabeth Rukmini. "Using Green Chemistry Experiments to Engage Sophomore Organic Chemistry." Miami University / OhioLINK, 2010. http://rave.ohiolink.edu/etdc/view?acc_num=miami1280437800.

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7

Alcock, S. "Tobacco chemistry." Thesis, University of Nottingham, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.356015.

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8

Leste-Lasserre, Pierre. "Sulfur allotrope chemistry." Thesis, McGill University, 2001. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=38218.

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The synthesis of the sulfur homocycles S6, S9, S10, S12 and S20, which belong to the group of sulfur allotropes, has been achieved based on existing procedures. Polymeric sulfur Smu was also prepared.
The parameters of a small scale model reaction between 2,3-diphenyl-1,3-butadiene and S10 were optimized. Products were identified and 1H-NMR yields were calculated by comparison with an internal standard. The experimental parameters of this model served as a base for further reactions of S 10 with a variety of simple or conjugated olefins. The products of these reactions were fully isolated and characterized using standard spectroscopic techniques. The structures of a new bis-sulfurated compound having a norbornane framework and of the product obtained from the dimerization of norborn-5-ene-2,3-dithiol were also confirmed by single crystal X-ray crystallography.
The sulfur homocycles S9, S12 and S20 were also found to react with norbornene and two different 1,3-dienes. Products were identified and 1H-NMR yields for these small scale reactions were calculated by internal standard comparison. Differences and similarities with the products obtained with S10 are discussed. Sulfuration efficiencies of the different allotropes towards selected substrates are also compared.
A mechanistic study was carried out. The implication of sulfur radicals in the thermal decomposition of S10 has been suggested. Reaction mechanisms accounting for the formation of the different products observed are proposed.

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9

Santangelo, Ellen M. "Stereoselective syntheses of semichemicals : Applications in ecological chemistry." Doctoral thesis, KTH, Chemistry, 2004. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-74.

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This thesis describes the syntheses of semiochemicals and their applications in the development of control methods for pest insects. The compounds synthesized are divided into three groups: 1) Lepidoptera pheromones; 2) methyl substituted chiral pheromones and 3) aphid pheromones.

Different purification techniques have been explored in order to provide > 99% pure semiochemicals for field tests. Examples of the techniques are uses of urea inclusion complexes, argentum chromatography, low temperature crystallization and what we call the Baeckström isolation technique.

Iridoids have been produced in a synthetic strategy including an intramolecular enal-enamine [4+2] cycloaddition, a dynamic acetylation and an enantioselective transesterification mediated by a lipase from Pseudomonas cepacia. The use of chiral auxiliaries to perform the intramolecular [4+2] cycloaddition has also been investigated. A useful asymmetric route to iridoids has been developed.

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10

Liu, Zhijian. "Novel aryne chemistry in organic synthesis." [Ames, Iowa : Iowa State University], 2006.

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11

Feeder, Neil. "The crystal chemistry of organic peracids." Thesis, University of Cambridge, 1992. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.260610.

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12

Greenacre, Caroline M. "Tropospheric chemistry of halogenated organic compounds." Thesis, University of Oxford, 2004. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.404120.

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Breed, Peter G. "Organic chemistry on highly functionalised supports." Thesis, University of Oxford, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.312151.

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14

Kinnison, David J. A. "Tropospheric chemistry of halogenated organic compounds." Thesis, University of Oxford, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.240663.

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15

Dudd, Lucinda M. "Organic chemistry in high-temperature water." Thesis, Nottingham Trent University, 2004. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.403413.

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16

Sehgal, Sunil Kumar. "Computer assisted design of organic chemistry." Thesis, University of Leeds, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.277647.

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17

McLean, William Neil. "Metal catalysed reactions in organic chemistry." Thesis, University of Liverpool, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.257123.

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18

Zappi, Guillermo Daniel. "Indirect electrochemical oxidations in organic chemistry." Thesis, University of Southampton, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.252698.

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19

Potts, Graham David. "The crystal chemistry of organic pigments." Thesis, University of Cambridge, 1993. https://www.repository.cam.ac.uk/handle/1810/272647.

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20

Selander, Nicklas. "Development of Multi-Component Reactions using Catalytically Generated Allyl Metal Reagents." Licentiate thesis, Stockholm University, Department of Organic Chemistry, 2008. http://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-8077.

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This licentiate thesis is based on the development of catalytic reactions for the synthesis and application of organometallic reagents. By use of palladium pincer-complex catalysts, we have developed an efficient procedure for the synthesis of allylboronates starting from allylic alcohols. These reactions were further extended by including various one-pot multi-component reactions, using the in situ generated allylboronates. Furthermore, novel unsymmetrical palladium pincer-complexes were synthesized and studied in auto-tandem catalysis.

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21

Tilliet, Mélanie. "Synthesis and study of new oxazoline-based ligands." Doctoral thesis, KTH, Organisk kemi, 2008. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-4858.

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This thesis deals with the study of oxazoline-based ligands in metal-catalyzed asymmetric reactions. The first part describes the synthesis of six new bifunctinal pyridine-bis(oxazoline) ligands and their applications in asymmetric metal-catalysis. These ligands, in addition to a Lewis acid coordination site, are equipped with a Lewis basic part in the 4-position of the oxazoline rings. Dual activation by means of this system was probed in cyanide addition to aldehydes. The second part is concerned with the synthesis of two pyridine-bis(oxazoline) ligands bearing bulky triazole groups in the 4-position of the oxazoline rings and a macrocyclic ligand consisting of a pyridine-bis(oxazoline) moiety and a diaza-18-crown-6 ether. The synthesis of these compounds benefits from the use of “click chemistry”. The ligands thus obtained were tested in different asymmetric catalytic reactions. Complexation studies with different bifunctional molecules that could bind into the cavity of the macrocycle were carried out using NMR spectroscopy. A third chapter is devoted to the synthesis of a supported pyridine-bis(oxazoline) catalyst and its use in catalysis. The pyridine-bis(oxazoline) ligand was efficiently connected to a polystyrene resin via a robust triazole linker. This resin could be employed in different metal-catalyzed asymmetric reactions and good results were obtained in terms of yield and enantioselectivity. Moreover, this polymer-bound ligand could be easily and efficiently recycled. Finally, the last part deals with the use of a hydroxy-containing phosphinooxazoline ligand in the hydrosilylation of imines and in the asymmetric intermolecular Heck reaction. A cationic iridium complex of this ligand was studied by NMR spectroscopy.
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22

Seward, Christopher M. P. "Stereoselective glycosylation chemistry." Thesis, University of Oxford, 2002. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.270281.

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23

Thornton, Steven Rupert. "Novel nitrone chemistry." Thesis, University of Nottingham, 1993. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.335298.

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24

Rodriguez-Cruz, N. M. "Chemistry of coal." Thesis, University of Newcastle Upon Tyne, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.372569.

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25

Bancroft, Matthew N. "Molybdenum-sulfur chemistry." Thesis, University of Sheffield, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.301264.

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26

Al, Djaidi Djamal Sholeh Chemistry Faculty of Science UNSW. "Studies in multicyclic chemistry." Awarded by:University of New South Wales. School of Chemistry, 2006. http://handle.unsw.edu.au/1959.4/27310.

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* A series of investigations has been carried out on multicyclic organic systems. The Ritter Reaction was used to obtain bridged imines containing an azacyclohexene functionality. The crystal structure of the benzene inclusion compound of one of these was determined, and also that of another spontaneously oxidised example. The reactivity of these bridged imines was then investigated using mercaptoacetic acid, and also dimethyl acetylenedicarboxylate (DMAD). The three bridged imines studied were found to react with DMAD in totally different ways and produced most unusual products whose structures were proved using X-ray crystallography. Mechanistic explanations are provided for the formation of these novel and totally unexpected products. * 6-Methylidene-3,3,7,7-tetramethylbicyclo[3.3.1]nonan-2-one was reacted with acetonitrile and sulfuric acid to deliberately combine molecular rearrangement with Ritter Reaction chemistry. Five different products were obtained and the pathway of formation of these products was uncovered. The structures of three of these rearranged substances were confirmed by X-ray methods. * The rare tricyclo[5.3.1.1 3,9]dodecane ring system is known to contain severe skeletal distortions due to the nature of its skeleton. These properties were investigated by means of X-ray determinations at two temperatures. It was found that although the bond lengths were little affected, several of the bond angles were highly anomalous. These had angles far from the ideal tetrahedral value and, in some cases, were close to planar (120 degrees). The molecular motion of the skeleton was also investigated using variable temperature NMR measurements and energy values for the twisting motion involved were determined. * Schroeter and Vossen's Red Salt, first discovered in 1910, was investigated in detail by NMR and X-ray spectroscopy. The detailed structure of this most unusual compound was determined for the first time. * The Red Salt is based on the bicyclo[3.3.0]octane ring system and can be converted into several synthetically useful derivatives, including a tetraester and the 3,7-diketone. The former was shown to exist completely in the enolised tautomeric form (like Meerwein's Ester), and the latter was used as a synthetic entry for making diquinoline substituted analogues of interest in host-guest chemistry.

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27

Barbiero, Gennaro. "Chemistry of biphenoxy radicals." Thesis, National Library of Canada = Bibliothèque nationale du Canada, 1997. http://www.collectionscanada.ca/obj/s4/f2/dsk2/tape16/PQDD_0026/NQ29884.pdf.

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28

Soriano, Del Amo David. "Pseudo-dynamic combinatorial chemistry." Thesis, McGill University, 2009. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=32577.

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Pseudo-dynamic combinatorial chemistry (pDCC) combines the synthesis, screening and destruction of combinatorial libraries to kinetically resolve inhibitors based on their affinity for a target. In our proof-of-principle studies, a library of dipeptides was formed in the presence of a target, carbonic anhydrase (CA), and a destruction mechanism, a protease. Since the target and the protease were separated by a dialysis membrane, only the proportion of dipeptides that was not bound to the target was available for destruction and therefore, the rate of hydrolysis of the pseudo-dynamic combinatorial library (pDCL) could be correlated to the librarie's relative affinity for the target. The first set of proof-of-principle pDCC experiments were found to be flawed. Rather than reflecting the binding affinity of the library for the target, the final product distribution reflected the protease's substrate specificity. The main problems with these pDCLs were insufficient and imbalanced rate of destruction of the peptides in the absence of the target, pH drift, and insufficient permeability across 1000 MWCO cellulose ester membranes. A dipeptide amide based pDCL that was efficiently cleaved by thermolysin was designed. The new pDCL could be used in pH 7.5 75 mM HEPES, 16.6 mM CaCl2 buffer, provided that the chambers were limited by 3500 MWCO membranes. A 4th generation pDCC experiment that evolved reflecting the library's affinity for the target was performed. In order to study pDCC behavior a simplified pDCC mimic (pDCCm) was designed. In pDCCm, synthesis was replaced by a static library of compounds and destruction by dilution. The design of a pDCCm based kinetic model led to a
La chimie combinatoire pseudo dynamique (pDCC) combine la synthèse, le criblage et la destruction de libraires combinatoires afin de sélectionner cinétiquement des inhibiteurs sur la base de leur affinité pour une cible. Nos études préliminaires ont été basées sur une librairie de dipeptides formés en présence de l'anhydrase carbonique (CA) comme cible et détruits grâce à une protéase. Étant donné que la cible et la protéase étaient séparées par une membrane de dialyse, seuls les dipeptides non complexés avec la cible étaient susceptibles d'être détruits. Ainsi, la vitesse d'hydrolyse des membres de la librairie combinatoire pseudo-dynamique (pDCL) peut correspondre aux affinités relatives des molécules pour la cible. Les premières expériences prototypes de pDCC étaient défectueuses. Plutôt que de refléter l'affinité des membres de la librairie pour la cible, la distribution finale des produits reflétait la préférence de la protéase pour les substrats. Les principaux problèmes de ces pDCL étaient: une vitesse de destruction des peptides insuffisante et inégale en l'absence de la cible, une déviation progressive du pH et une perméabilité insuffisance au travers les membranes d'ester de cellulose 1000 MWCO. Une pDCL basée sur des amides dipeptidiques, aptes à être efficacement clivés par thermolysine a été élaborée, et utilisée avec succès. Afin d'étudier les pDCC, une expérience modèle simplifiée (pDCCm) a été créée. Dans ce modèle, la synthèse a été remplacée par une librairie statique de molécules et la destruction par une dilution. Le design d'un modèle cinétique basé sur la pDCCm a mené à la cr

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29

Zeng, Xiaofeng. "Mechanisms for Solvolytic Elimination and Substitution Reactions Involving Short-lived Carbocation Intermediates." Doctoral thesis, Uppsala University, Organic Chemistry, 2002. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-2565.

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Solvolysis reactions of a range of tertiary substrates in largely aqueous solvents were studied in such respects as β-deuterium kinetic isotope effects, linear free energy relationships and stereochemistry.

Solvolysis of the fluorene derivatives 9-methyl–9-(2´-X-2´-propyl)fluorene (1-X, X = Cl, Br, OOCCF₃) involves a very short-lived carbocation intermediate. The fraction of alkene is increased by addition of general bases, which can be expressed by a Brφnsted parameter β = 0.07. The kinetic deuterium isotope effects vary with solvent composition in a way which is not consistent with a common carbocation intermediate which has time to choose between dehydronation and addition of a solvent water molecule.

In the absence of bases, the reaction of 4-chloro-4-(4´-nitrophenyl)pentan-2-one (2-Cl) proceeds through a short-lived carbocation intermediate yielding 4-(4´-nitrophenyl)-2-oxopent-4-ene (2-t-ne)as the main elimination product. Addition of acetate ion and other weak bases results in the base-promoted E2 (or E1cb) reaction to give (E)-4-(4´-nitrophenyl)-2-oxopent-3-ene (2-E-ne) and (Z)-4-(4´-nitrophenyl)-2-oxopent-3-ene(2-Z-ne). There is no evidence for a water-promoted E2 (or E1cb) reaction.

The stereochemistry studies of elimination from (R,S and S,R)-[1-(3´-fluoro)phenyl-2-methyl]cyclopentyl-p-nitrobenzoate (3-PNB) and its (R,R and S,S)isomer 3´-PNB and (R,S and S,R)-[1´-(3´´-fluoro)phenyl-2´-methylcyclopentyl]-2,2,2-trifluoroacetate(3-OOCCF3) exclude the concerted pericyclic elimination mechanism for formation of the alkene 1-(3´-fluoro)phenyl-2-methylcyclopentene(3-m-ne). The effects of added thiocyanate ion and halide ions on the solvolysis reaction are discussed.

Mass spectrometry analysis showed complete incorporation of the labeled oxygen from solvent water into the product 2-hydroxy-2-phenyl-3-butene (4-OH), confirming that it is the tertiary carbon-oxygen bond that is broken in the acid-catalyzed solvolysis of 2-methoxy-2-phenyl-3-butene (4-OMe). The mechanism for the dominant formation of the less stable 4-OH is discussed.

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30

Roth, Peter. "Asymmetric transfer hydrogenation of aromatic ketones and azirines with NH-ligands." Doctoral thesis, Uppsala University, Organic Chemistry, 2002. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-2679.

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The Ru(arene)[(1S, 3R, 4R)-3-(Hydroxymethyl)-2-azabicyclo[2.2.1]heptane catalyst was optimized as ligand in the asymmetric transfer hydrogenation of ketones and resulted in increased activity and enantioselectivity of the catalyst. Dioxolane substitution at the rear end of the amino alcohol ligand and introduction of a (R)-methyl substituent yielded a catalyst that reduced acetophenone in 96% enantiomeric excess in 90 minutes with a substrate to catalyst molar ratio of 5000. A diversity of substituted aromatic ketones was reduced with excellent rate and enantioselectivity. Based on experimental and computational results, a study of the origin of the enantioselectivity was conducted. A combination of electrostatic, steric, dispersion forces and solvation effects was suggested to be the cause of the stereo discrimination. A set of amino sulfides built upon the 2-azabicyclo and the cyclohexane structures were prepared and tested as ligands in the enantioselective transfer hydrogenation of acetophenone with [IrCl(COD)]₂ as metal precursor. With this type of catalysts, the reaction rates were good but the enantioselectivity unsatisfactory with 70% as the highest obtained enantiomeric excess. The first enantioselective reduction of aromatic 2H-azirines was accomplished by using the asymmetric transfer hydrogenation protocol. Aromatic azirines were reduced to yield chiral aziridines with up to 72% enantiomeric excess and good yields. The enantioselectivity and reactivity of the reaction were strongly influenced by substituents on the aromatic and aliphatic moiety of the substrate.

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31

Karimi, Farhad. "[¹¹C]Carbon Monoxide in Palladium- / Selenium-Promoted Carbonylation Reactions : Synthesis of ¹¹C-Imides, Hydrazides, Amides, Carboxylic Acids, Carboxylic Esters, Carbothioates, Ketones and Carbamoyl Compounds." Doctoral thesis, Uppsala University, Organic Chemistry, 2002. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-2931.

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[¹¹C]Carbon monoxide in low concentrations has been used in palladium- or seleniummediated carbonylation reactions such as the synthesis of ¹¹C-imides, hydrazides, amides, carboxylic acids, esters, carbothioates, ketones and carbamoyl compounds.

In these reactions aryl iodides have been used in most cases. However, less reactive aryl triflate, chloride and bromides were activated using tetrabutylammonium iodide.

The reactivities of nucleophiles may have influence on the radiochemical yield of the ¹¹Clabelled compounds. Carboxyamination of aryl halides using aniline derivatives yielded 10% of the corresponding ¹¹C-amide. However, the radiochemical yields increased significantly when the aniline derivatives were treated with lithium bis(trimethylsilyl)amide. In contrast, this reagent did not improve the radiochemical yields when primary amines such as methylamine and benzylamine were used. In these cases the radiochemical yields were improved by using pempidine.

¹¹C-Esterification usually gave low yields. However, the radiochemical yields of ¹¹C-esters could be improved by using magnesium bromide and pempidine.

An excess of ligand may have a significant impact on palladium-promoted carbonylation reaction. The radiochemical yields of ¹¹C-ketones were improved when using excess amounts of tri-o-tolylphosphine.

(¹³C)Carbon monoxide may be utilized for the synthesis of ¹³C-substituated compounds in order to confirm the position of ¹¹C-labelling.

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Karimi, Farhad. "[11C]Carbon Monoxide in Palladium- / Selenium-Promoted Carbonylation Reactions : Synthesis of 11C-Imides, Hydrazides, Amides, Carboxylic Acids, Carboxylic Esters, Carbothioates, Ketones and Carbamoyl Compounds." Doctoral thesis, Uppsala universitet, Avdelningen för organisk kemi, 2002. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-2931.

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[11C]Carbon monoxide in low concentrations has been used in palladium- or seleniummediated carbonylation reactions such as the synthesis of 11C-imides, hydrazides, amides, carboxylic acids, esters, carbothioates, ketones and carbamoyl compounds. In these reactions aryl iodides have been used in most cases. However, less reactive aryl triflate, chloride and bromides were activated using tetrabutylammonium iodide. The reactivities of nucleophiles may have influence on the radiochemical yield of the 11Clabelled compounds. Carboxyamination of aryl halides using aniline derivatives yielded 10% of the corresponding 11C-amide. However, the radiochemical yields increased significantly when the aniline derivatives were treated with lithium bis(trimethylsilyl)amide. In contrast, this reagent did not improve the radiochemical yields when primary amines such as methylamine and benzylamine were used. In these cases the radiochemical yields were improved by using pempidine. 11C-Esterification usually gave low yields. However, the radiochemical yields of 11C-esters could be improved by using magnesium bromide and pempidine. An excess of ligand may have a significant impact on palladium-promoted carbonylation reaction. The radiochemical yields of 11C-ketones were improved when using excess amounts of tri-o-tolylphosphine. (13C)Carbon monoxide may be utilized for the synthesis of 13C-substituated compounds in order to confirm the position of 11C-labelling.

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Winberg, Karl Johan. "Carborane Derivatives for Nuclide Therapy and Imaging : Synthesis and Radio-labelling." Doctoral thesis, Uppsala : Acta Universitatis Upsaliensis : Univ-bibl. [distributör], 2003. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-3561.

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Bates, Richard Simon. "Arene ruthenium chemistry." Thesis, University of Nottingham, 1990. http://eprints.nottingham.ac.uk/11890/.

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This thesis describes the synthesis and reactivity studies of new arene-ruthenium(II) and arene-ruthenium(O) complexes. Ultrasound has been investigated as an alternative energy source, with the overall aim of synthesising arene ruthenium clusters. Chapter 1 gives an introduction and summary of the known arene ruthenium chemistry reported to date. Chapter 2 reports the synthesis of (CGH6)Ru(C2H4)2 and (MeC6H4CHMe2)Ru(C2H4)2. Low temperature protonation studies generated (C6H6)Ru(H)(CZH4)2' and (MeC6H4CHMe2)Ru(H)(C2H4)7ý. These are observed by 1H nmr spectroscopy to undergo two dynamic processes, rotation of the ethylene ligands and an exchange between the hydride and the hydrogens of the ethylenes. On protonation with trifluoroacetic acid (C6H6)Ru(02CCF3)2 has been shown to be the final product. Nucleophilic substitution investigations of the bis(ethylene) complexes has determined that the arene is more labile than the coordinated ethylene. Chapter 3 reports the generation of a reactive intermediate, [(MeC6H4CHMez)Ru(THF)2]", and the reactions it undergoes. The synthesis and stereochemistry of the new complexes [(MeC6H4CHMe2)RuBr(C3H5)] and Ru(H)[(C6H40) (OPh)2][P(OPh)3]3 are reported. Chapter 4 describes the successful synthesis of the project goal, with the formation of the trimer [(MeC. H., CHMe2)3Ru3Se,_1` and the tetra nuclear species [(MeC6H4CHMe2)4Ru4H4]2'. Electrochemistry shows both complexes undergo two, one-electron reversible reductions to generate their neutral analogues. Ru3(CO)12 was formed when arene ruthenium carbonyl clusters were sought. Chapter 5 reports the formation and reactivity of arene ruthenium complexes containing nitrogen based ligands. The half sandwich complexes, (arene)RuCl2(NH2R) (arene = C6H6, R= Et, CMe, C6H4Me; McC6H4CHMe2, R=CMe3) and (C. H6)RuCl(NHZCGH4Me)Z' have been synthesised in good yield. However, these complexes are not synthetically useful as substrates for cluster synthesis, although (C6H6)RuC12(NH2CMe3) can be converted to the mixed ethoxide-halide dimer, [(C6H6)Ru(OEt)]2Cl`. Me3SiN3 on reaction with [(MeC6H4CHMe2)RuC12]2 affords [(MeC6H4CHMe2)RuCl(N3)]Z. An X-ray crystal structure determination of this complex showed the nitrogens bridging the two ruthenium atoms are pyramidal rather than the expected planar in geometry. [(MeC6H4CHMe2)RuCl(N3)]2 undergoes chloride loss to form the triply bridged dimer, [(MeCGH4CHMe2)RuCl(N3)z]', and bridge cleavage to form [(MeC, H4CHMe2)RuCl(N3)PPh3]. The latter complex is believed to undergo disproportionation in solution. Conclusions and future directions of the project are discussed in chapter. 6. The appendix provides a discussion of ultrasound proposed structure.

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35

Sang, Lingzi, and Lingzi Sang. "Spectroscopy Investigation of Molecular Processes at Organic/Metal Oxide and Organic/Metal Interfaces in Organic Photovoltaic Devices." Diss., The University of Arizona, 2015. http://hdl.handle.net/10150/566987.

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The purpose of this Dissertation is to investigate the chemistry at interfaces between organic active materials and two electrodes, namely organic metal oxide cathode and metal anode, in organic photovoltaic (OPV) devices. Poor compatibility and energy level mismatch at organic/transparent metal oxide (TCO) interfaces is a long standing challenge which limits interfacial electron transfer efficiency. Phosphonic acid modifiers on TCO surfaces are able to improve interface compatibility and energy alignment. Chapters 3 and 4 in this Dissertation investigate the fundamental formation, quality and orientation of phosphonic acid monolayers on indium-doped zinc oxide (IZO) surfaces, a model TCO. Metal electrode deposition on organic active layer materials is a common last step of OPV device fabrication. Chapters 5-8 in this Dissertation explore possible molecular processes at organic-metal interfaces when metal deposition occurs under ultra-high vacuum conditions. Choosing octylphosphonic acid (OPA), F₁₃-octylphosphonic acid (F₁₃OPA), pentafluorophenyl phosphonic acid (F₅PPA), benzyl phosphonic acid (BnPA), and pentafluorobenzyl phosphonic acid (F₅BnPA) as a representative group of modifiers, Chapter 3 describes polarization modulation-infrared reflectance-absorbance spectroscopy (PM-IRRAS) of binding and molecular orientation on IZO substrates. Considerable variability in molecular orientation and binding type is observed with changes in PA functional group. OPA exhibits partially disordered alkyl chains, but on average, the chain axis is tilted 57° from the surface normal; F13OPA tilts 26° with mostly tridentate binding; the F₅PPA ring orients 72° from the surface normal with a mixture of bidentate and tridentate binding; the BnPA ring orients 59° from normal with a mixture of bidentate and tridentate binding, and the F₅BnPA ring orients 45° from normal with a majority of bidentate with some tridenate binding. These trends are consistent with what has been observed previously for the effects of fluorination on orientation of phosphonic acid modifiers. The results from PM-IRRAS are well correlated with recent results on similar systems from near-edge x-ray absorption fine structure (NEXAFS) and density functional theory (DFT) calculations. Overall, these results indicate that both surface binding geometry and intermolecular interactions play important roles in dictating orientation of PA modifiers on TCO surfaces. This work also establishes PM-IRRAS as a routine method for SAM orientation determination on complex oxide substrates. In addition to orientation studies the effect of PA deposition method on the formation of close-packed, high-quality monolayers is investigated in Chapter 4 for SAMs fabricated by solution deposition, microcontact printing, and spray coating. The solution deposition isotherm for perfluorinated benzylphosphonic acid (F₅BnPA) on IZO is studied using PM-IRRAS at room temperature as a model PA/TCO system. Fast surface adsorption occurs in the first minute; however, well-oriented high-quality SAMs are reached only after ~48 h, presumably through a continual process of molecular adsorption/desorption accompanied by molecular reorientation. Two other rapid, soak-free deposition techniques, microcontact printing and spray coating, are also explored. SAM quality is compared for deposition of phenyl phosphonic acid (PPA), F₁₃-octylphosphonic acid (F₁₃OPA), and perfluorinated benzyl phosphonic acid (F₅BnPA) by solution deposition, microcontact printing and spray coating using PM-IRRAS. In contrast to microcontact printing and spray coating techniques, 48-168 h solution depositions at both room temperature and 70 °C result in contamination- and surface etch-free close-packed monolayers with good reproducibility. SAMs fabricated by microcontact printing and spray coating are much less well ordered.Oligothiophenes are building blocks of the popular organic donor materials polythiophene and P3HT. In Chapters 6 and 7, interfacial reactions of the model thiophene-based oligomers, ɑ-sexithiophene (ɑ-6T) and 2, 2’:5’, 2”-terthiophene (ɑ-3T), with vapor deposited Ag, Al, Mg and Ca are investigated using surface Raman spectroscopy under ultra-high vacuum conditions. Results indicate that Al and Ca cause reduction of ɑ-6T to tetrahydrothiophene and calcium sulfite, respectively, with Al exhibiting less reactivity than Ca. Partial electron donation from the sulfur atom lone pair electrons to vacant Ag and Mg d or p orbitals is observed, inducing formation of polaron states at the interface. Inter-ring C-C bond rotation is also induced by this electron sharing betweenɑ-6T and both Ag and Mg. This unexpected evolution of ɑ-6T interfaces with low work function metals alters the interfacial energetics through the formation of “gap” states which ultimately impact device performance. Vapor deposited Ag forms nanoparticles on the surface and induces considerable surface enhanced Raman scattering (SERS) of the ɑ-3T along with a change in molecular symmetry and formation of Ag-S bonds; no other reaction chemistry is observed. Vapor deposited Al and Ca exhibit chemical reaction withɑ-3T spectrum initiated by metal-to-3T electron sharing. For Al, the resulting product is predominantly amorphous carbon (a-C) through initial radical formation and subsequent decomposition reactions. For Ca, the spectral evidence suggests two pathways: one leading to ɑ-3T polymerization and the other resulting in thiophene ring opening, both initiated by radical formation through Ca-to-ɑ-3T electron transfer. In Chapter 8, metal penetration depth into ɑ-3T and ɑ-6T films is investigated and compared between Ag, Al, Mg and Ca using Raman and X-ray photoelectron spectroscopies. Mg exhibits the greatest penetration with no observable surface metallization on 50 ML (15 nm) OT surfaces. Ag shows moderate penetration and metallization ability with no reaction chemistry when in contact with ɑ-6T. Al and Ca exhibit the least penetration and greatest metallization abilities, possibly due to reaction chemistry occurring between Al (or Ca) and ɑ-6T. Al and Ca both penetrate up to 10-14 nm intoɑ-6T layers. The penetration process for Ca consists of two distinct phases. Ca tends to be more evenly distributed throughout the entire ɑ-6T film and reduce the native ɑ-6T until the composition of the top 5-7 nm of the ɑ-6T film becomes constant; beyond this point, further Ca deposition penetrates and completely reduces ɑ-6T into CaS throughout the entire 10-14 nm thickness. Al atoms are more concentrated within the top 5-7 nm of the film and gradually penetrate deeper into the film. These results reveal significant but varying depths of the impact of deposited metals on OT thin films during physical vapor deposition; these results further reinforce the critical role of interfacial chemistry on organic electronic device performance.

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36

Anderson, Michele Lynn 1968. "Characterization of organic/organic' and organic/inorganic heterojunctions and their light-absorbing and light-emitting properties." Diss., The University of Arizona, 1997. http://hdl.handle.net/10150/282555.

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Increasing the efficiency and durability of organic light-emitting diodes (OLEDs) has attracted attention recently due to their prospective wide-spread use as flat-panel displays. The performance and efficiency of OLEDs is understood to be critically dependent on the quality of the device heterojunctions, and on matching the ionization potentials (IP) and the electron affinities (EA) of the luminescent material (LM) with those of the hole (HTA) and electron (ETA) transport agents, respectively. The color and bandwidth of OLED emission color is thought to reflect the packing of the molecules in the luminescent layer. Finally, materials stability under OLED operating conditions is a significant concern. LM, HTA, and ETA thin films were grown in ultra-high vacuum using the molecular beam epitaxy technique. Thin film structure was determined in situ using reflection high energy electron diffraction (RHEED) and ex situ using UV-Vis spectroscopy. LM, HTA, and ETA occupied frontier orbitals (IP) were characterized by ultraviolet photoelectron spectroscopy (UPS), and their unoccupied frontier orbitals (EA) estimated from UV-Vis and fluorescence spectroscopies in combination with the UPS results. The stability of the molecules toward vacuum deposition was verified by compositional analysis of thin film X-ray photoelectron spectra. The stability of these materials toward redox processes was evaluated by cyclic voltammetry in nonaqueous media. Electrochemical data provide a more accurate estimation of the EA since the energetics for addition of an electron to a neutral molecule can be probed directly. The energetic barriers to charge injection into each layer of the device has been correlated to OLED turn-on voltage, indicating that these measurements may be used to screen potential combinations of materials for OLEDs. The chemical reversibility of LM voltammetry appears to limit the performance and lifetimes of solid-state OLEDs due to degradation of the organic layers. The role of oxygen as an electron trap in OLEDs has also been verified electrochemically. Finally, a more accurate determination of the offset of the occupied energy levels at the interface between two organic layers has been achieved via in situ monitoring of the UPS spectrum during heterojunction formation.

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37

Lapierre, Keith. "Exploring Students’ Interpretations of Reactions and Self-Efficacy Beliefs in Organic Chemistry in a Redesigned Organic Chemistry Curriculum." Thesis, Université d'Ottawa / University of Ottawa, 2019. http://hdl.handle.net/10393/39887.

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Organic Chemistry has been described as a challenging and confusing course for undergraduate students. Novices in the field have been struggling to understand fundamental concepts relating to organic mechanisms and organize their knowledge around surface features such as functional groups rather than deep underlying features. At the University of Ottawa, a new “Mechanistic patterns and principles” curriculum was designed and implemented, organized by the underlying mechanistic patterns that govern reactions rather than the traditional surface features approach. The redesigned curriculum emphasizes principles of reactivity in organic chemistry and is organized in a gradient of difficulty. The three studies included within this work act as part of a larger evaluation of the redesigned curriculum, specifically investigating an instrument to assess the formation of expertise in organic chemistry and an instrument to capture self-efficacy beliefs in organic chemistry as students progress throughout the curriculum. In the first two studies, an open and closed online categorization task was delivered to Organic Chemistry II students at both the beginning and end of their course. The open sort provided insights regarding how participants choose to sort, while the closed sort measured participants' ability to categorize reactions according to their underlying mechanistic pattern. In the first study, we provide an in-depth analysis of the changes in expertise that occur with respect to the expertise of their choices and ability. Findings from this work demonstrated a positive shift from students attending to surface to process-oriented features in the open sort, as well as an increase in students’ ability in the closed sort. The following-up study investigates the relationship between the expertise demonstrated by participants in the open and closed sorts. Additionally, this work compares these measures of expertise against varies other metrics, including a high-stakes categorization task, and academic performance to increase the validity, and probes at the reliability of findings. Findings from this work demonstrate a strong relationship between the expertise demonstrate in the online task and academic performance, as well as describe an evolving relationship between the expertise demonstrated in students’ choice and ability as they progress throughout the course. While previous work in the evaluation of the curriculum demonstrated that students possess greater ability, it is unknown whether this also translates to an increase in their beliefs about their abilities. The last study included within this work moves beyond cognitive outcomes of the curriculum to investigating the role of self-efficacy beliefs in the curriculum. Self-efficacy beliefs are defined as an individual’s belief in their capability to perform a specific task or objective successfully. This work intends to construct and validate a task-specific, multi-dimensional self-efficacy beliefs instrument for undergraduate students in the domain of organic chemistry. Pre-administration validity evidence, including test content and response process validity, was collected. Data for internal structure validity evidence was collected from a single administration with Organic Chemistry I students (N=78) to 7-factor structure within the final 39 item instrument. Due to the small sample size, these results are interpreted with extreme caution. Future work with this instrument aims to improve the validity evidence collected by expanding the sample size and evaluate the influence curriculum on self-efficacy beliefs, and who, based on demographic variables, may be benefiting the most from the transformed curriculum.

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38

Stringer, Graham Howard. "Studies in organoruthenium chemistry." Thesis, University of Oxford, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.315819.

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39

Jones, Beverly Ann. "The chemistry of isonitriles." Thesis, Bangor University, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.481089.

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40

Clawson, P. "Chemistry of carbonyl ylides." Thesis, University of Nottingham, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.373346.

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41

Mughal, Zulficar Ali. "Chemistry of the anthracyclinones." Thesis, University of Bradford, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.236480.

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42

Fitton, Helen Lesley. "Studies in cyclopropene chemistry." Thesis, University of Newcastle Upon Tyne, 1993. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.335136.

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43

Akuamoah, Robert Kwado. "Studies in chromene chemistry." Thesis, University of Newcastle Upon Tyne, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.358888.

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44

Schofield, J. M. "Studies in pyridoazepine chemistry." Thesis, University of Salford, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.376869.

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45

Harris, P. "Some chemistry of nitroacetamides." Thesis, University of Manchester, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.234211.

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46

Thorpe, Heidi Ruth. "Chemistry of allene oxides." Thesis, Loughborough University, 1997. https://dspace.lboro.ac.uk/2134/13751.

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Chapter One reviews aspects of the chemistry of allene oxides reported in the chemical literature. The review is organised into three sections describing the available methods for the preparation of allene oxides, the reactions of allene oxides and allene oxides in biological systems. Chapter Two discusses attempts to develop new methods for the generation and trapping of allene oxides. Firstly, an unsuccessful attempt to employ a selenoxide elimination to generate an allene oxide is described. This is followed by a section detailing an improved method for the generation and in situ capmre of allene oxides with alcohols. Sodium alkoxides were found to trigger elimination in β,γ-epoxy-β-trimethylsilyl mesylates to afford allene oxides and also act as the nucleophilic trapping component. This methodology was used to synthesise a range of α alkoxyketones. Attempts to employ other nucleophiles in this process are also discussed. Chapter Three describes how the successful chemistry described in Chapter Two was modified in order to generate and trap chiral, non-racemic allene oxides. The preparation of homochiral β,γ-epoxy-β-trimethylsilyl mesylates and their subsequent reaction with potassium alkoxides at low temperature under aprotic conditions is described. The α alkoxyketone products were found to be of high enantiomeric excess and the absolute configuration of the product was determined in one case. Finally, attempts to effect a threecomponent coupling of an aIlene oxide, by reaction of an allene oxide with a nucleophile and subsequently an electrophile, are discussed. Chapter Four describes pioneering work towards a general method for the preparation of methylene cyclic sulfites as potential allene oxide equivalents is presented. A series of such compounds were prepared by reaction of α-hydroxyketones with thionyl chloride and via selenoxide elimination chemistry. Chapter Five describes the detailed experimental work undertaken in this thesis.

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47

Ndamyabera, Christophe Adrien. "Porous metal-organic frameworks for sorption of volatile organic compounds." Doctoral thesis, Faculty of Science, 2021. http://hdl.handle.net/11427/33877.

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Metal-organic frameworks (MOFs) present potential for various applications such as gas sorption, gas storage, sensing, drug delivery, and catalysis. This attracts researchers to design and synthesize MOFs that can respond to a specific application. In this thesis, mixed ligands 34pba and 44pba ligands (34pba = 3-(4-pyridyl)benzoate, and 44pba = 4-(4-pyridyl)benzoate) and Co2+ metal salts were used to synthesize porous MOFs {[Co(34pba)(44pba)]·DMF}n (1) and {[Co(34pba)(44pba)]·(C3H6O)}n (2), with DMF = N,N'-dimethylformamide and C3H6O = acetone through solvothermal reaction. These two relate to each other through hinge-like expansion or contraction of the guest-accessible void. The use of Zn2+ as a metal ion led to an isostructural MOFs [Zn(34pba)(44pba)]·DMF}n (3) of 1. Using 34pba as a single ligand and Cu2+ as the metal ion led to the formation of a 2D [(Cu(34pba)2]·DMF) (4) while a little variation of solvent mixture resulted in a 3D {[CuCl2(34pba)2]∙solvent}n (7) structures. The functionalized ligands 44paba and 34paba (34paba = 3-(pyridyn-4-ylmethyl)aminobenzoate, 44paba = 4-(pyridyn-4- ylmethyl)aminobenzoate) were used with Cu2+ centre to prepare [Cu(44paba)·(H2O)·(DMF)]n (5) and {[Cu3(34paba)5(H2O)2]·(DMF)2}n (6), both of which are 1D structures. The activated MOFs 1d and 3d from (1 and 2) were used for the adsorption of volatile organic compounds (VOCs) and gases. In all tested guest molecules, there was higher sorption capacity in 1d which could be attributed to some gate opening process occurring which does not occur in 3d. Some effects responding to the sorption such as the change of colour in 1d were characterized. This colour change may be associated with the d-d, metal to ligand charge transfer, or π to π* transitions in coordination complex. Crystal structures and their stability, sorption properties and selectivity were characterized by single crystal X-ray diffraction, thermogravimetric analysis, differential scanning, hot stage microscopy, powder X-ray diffraction, infrared spectroscopy, and proton viii nuclear magnetic resonance (1H NMR) analysis. This thesis also reports the effect of methanol on discrete complexes of cis-dichloro-bis(ethylenediamine)cobalt(III) chloride (Coen) that led to the formation of a new crystal structure upon the removal of the water of hydration. The lattice energies calculated prove that Coen is more stable to allow a quick reversible sorption.

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48

Kao, Chi-Yueh. "Thin films of organic-based magnetic semiconductors for organic spintronics." The Ohio State University, 2012. http://rave.ohiolink.edu/etdc/view?acc_num=osu1343748166.

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49

Lin, Hsiao-Chu. "Charge Transfer Processes across Organic/Electrode Interfaces in Organic Photovoltaics." Diss., The University of Arizona, 2013. http://hdl.handle.net/10150/312512.

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Charge transfer efficiency at organic/electrode interfaces affects the performance organic photovoltaics (OPVs). It is hypothesized that the charge collection efficiency at organic/electrode interfaces is influenced by the structure of the first molecular layer adjacent to the electrode surface. Two differently oriented monolayers composed of two phosphonic acid (PA) functionalized zinc phthalocyanine (ZnPc) molecules, one with four PAs attached peripherally (ZnPcPA₄), one at each quadrant, and another that is functionalized with one PA (ZnPcPA), were tethered to indium tin oxide (ITO) surfaces as models for the donor/transparent conducting oxide (TCO) interface in OPVs to address the relationship between molecular orientation and electron transfer kinetics across the organic/ITO interface. The electron transfer rate constants across the monolayer/ITO interface were measured using potential modulated attenuated total reflectance (PM-ATR) spectroscopy in TE and TM polarizations, which allows rate constants to be determined for subpopulations of molecules that are oriented predominately in-plane and out-of-plane, respectively. The templating effect of the tethered monolayer on sequential layers of donor material for ZnPcPA and ZnPcPA₄ monolayers was assessed by depositing a few layers of CuPc on ZnPcPA- and ZnPcPA₄-modified ITO. The performance of OPV devices fabricated on ITO modified with these two monolayers was compared and correlated to their orientation and energy alignments with other layers in the devices. The dependence of kinetics of electron transfer on overpotential was studied using monolayer-tethered ZnPcPA on ITO. Measurements of apparent heterogeneous electron transfer rate constants (kapp) as a function of applied potential across the ZnPcPA/ITO interface were acquired using PM-ATR at various dc biases (Edc). With varying Edc imposed on the electrode, the fraction of adsorbed molecules in reduced or oxidized states is changed, and both the energetics and kinetics of the electrode reaction are affected. The results were discussed and compared to theoretical predictions. The photoinduced charge harvesting and photocurrent generation were assessed using a clicked ZnPc-perylene diimide (PDI) donor-acceptor assembly tethered to ITO via a PA anchoring group. This ZnPc-PDI donor-acceptor assembly was used to investigate the mechanism of photoinduced charge transfer and hole-capture by ITO in the presence of a solution phase redox mediator.

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50

Schultz, Erwin. "New aspects of organochalcogen chemistry." Thesis, National Library of Canada = Bibliothèque nationale du Canada, 1999. http://www.collectionscanada.ca/obj/s4/f2/dsk1/tape3/PQDD_0032/NQ64663.pdf.

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Dissertations / Theses on the topic 'Organic Chemistry'

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