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Studies on chromium and tungsten complexes with polypyrazolyl ligands and related speciesWilliams, Geoffrey K. January 1992 (has links)
No description available.
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Atomistic materials modeling of complex systems carbynes, carbon nanotube devices and bulk metallic glasses /Luo, Weiqi, January 2008 (has links)
Thesis (Ph. D.)--Ohio State University, 2008. / Title from first page of PDF file. Includes bibliographical references (p. 142-155).
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Synthesis of polysubstituted-1, 4-quinones and allylsilanes via alkenyl Fischer carbene complexes.January 1993 (has links)
by Chi-Ching Mak. / Thesis (M.Phil.)--Chinese University of Hong Kong, 1993. / Includes bibliographical references (leaves 65-70). / Acknowledgement --- p.i / Abbreviation --- p.ii / List of spectra --- p.iii / Contents --- p.iv / Abstract --- p.v / Chapter Part One: --- "Synthesis of Poly substituted-1,4-Quinones" / Chapter 1.1 --- Introduction / Chapter 1.2 --- Results and discussion --- p.9-16 / Chapter 1.3 --- Conclusion --- p.17 / Chapter Part Two: --- Synthesis of Allylsilanes / Chapter 2.1 --- Introduction --- p.18-25 / Chapter 2.2 --- Results and discussion --- p.26-34 / Chapter 2.3 --- Conclusion --- p.35 / Experimental Section --- p.36-64 / References --- p.65-70 / Spectra --- p.71-86
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Kinetic studies of [3+2] cycloaddition of Fischer carbene complexes with nitrones.January 1994 (has links)
by Ming Lok Yeung. / Thesis (M.Phil.)--Chinese University of Hong Kong, 1994. / Includes bibliographical references (leaves 54-56). / ACKNOWLEDGMENT --- p.i / ABBREVIATION --- p.ii / ABSTRACT --- p.iii / CONTENTS --- p.iv / Chapter I. --- INTRODUCTION --- p.1 / Chapter II. --- RESULTS AND DISCUSSION --- p.8 / Chapter II-1 --- [3+2] CYCLOADDITION OF FISCHER CARBENE COMPLEXES WITH NITRONES --- p.8 / Chapter II-2 --- KINETIC STUDIES OF THE [3+2] CYCLO ADDITION --- p.18 / Chapter III. --- CONCLUSION --- p.35 / Chapter IV. --- EXPERIMENTAL --- p.36 / Chapter V. --- APPENDIX --- p.49 / Chapter V. --- REFERENCES --- p.54 / Chapter VI. --- LIST OF SPECTRA --- p.57 / Chapter VII. --- SPECTRA --- p.58
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Studies of Metathesis for Materials Applications: Present and Future PossibilitiesMarleau-Gillette, Joshua 23 January 2013 (has links)
Compounds containing multiple metal-carbon bonds are now widely used as catalysts for organic and materials synthesis. Among such transformations, olefin metathesis (OM) occupies a position of pre-eminent significance. Alkyne metathesis holds great promise, but remains in a much lower state of development. The OM-directed work in this thesis sought to advance the state of the art in living, Ru-catalyzed ringopening metathesis polymerizations (ROMP). Currently, the first- and third-generation Grubbs initiators, which exhibit the ease of handling characteristic of the late metal ruthenium, dominate ROMP applications. These initiators are characterized by extremes of reactivity, however. We describe the first ruthenium initiator capable of living ROMP at RT, irrespective of monomer bulk. Polydispersity indices as low as 1.03 are routinely attainable, and excellent control is maintained in synthesis of diblock copolymers from sterically demanding and sterically unencumbered monomers. Work on alkyne metathesis sought to expand existing understanding of the features that influence stability and reactivity in ruthenium carbynes. A classification system was developed in which Class A carbynes were defined as those that readily undergo conversion into an M=C entity (e.g. vinylidene, allenylidene, or alkylidene); Class B carbynes those that have a stable carbyne functionality. Four Ru carbyne complexes, all initially regarded as prospective Class B carbynes, were selected for study. Investigation of their reactivity resulted in categorization of several as Class A species, and development of design criteria that may open the door to assembly of stable, well-defined carbyne complexes of ruthenium.
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Studies of Metathesis for Materials Applications: Present and Future PossibilitiesMarleau-Gillette, Joshua 22 January 2013 (has links)
Compounds containing multiple metal-carbon bonds are now widely used as catalysts for organic and materials synthesis. Among such transformations, olefin metathesis (OM) occupies a position of pre-eminent significance. Alkyne metathesis holds great promise, but remains in a much lower state of development. The OM-directed work in this thesis sought to advance the state of the art in living, Ru-catalyzed ringopening metathesis polymerizations (ROMP). Currently, the first- and third-generation Grubbs initiators, which exhibit the ease of handling characteristic of the late metal ruthenium, dominate ROMP applications. These initiators are characterized by extremes of reactivity, however. We describe the first ruthenium initiator capable of living ROMP at RT, irrespective of monomer bulk. Polydispersity indices as low as 1.03 are routinely attainable, and excellent control is maintained in synthesis of diblock copolymers from sterically demanding and sterically unencumbered monomers. Work on alkyne metathesis sought to expand existing understanding of the features that influence stability and reactivity in ruthenium carbynes. A classification system was developed in which Class A carbynes were defined as those that readily undergo conversion into an M=C entity (e.g. vinylidene, allenylidene, or alkylidene); Class B carbynes those that have a stable carbyne functionality. Four Ru carbyne complexes, all initially regarded as prospective Class B carbynes, were selected for study. Investigation of their reactivity resulted in categorization of several as Class A species, and development of design criteria that may open the door to assembly of stable, well-defined carbyne complexes of ruthenium.
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Studies of Metathesis for Materials Applications: Present and Future PossibilitiesMarleau-Gillette, Joshua January 2013 (has links)
Compounds containing multiple metal-carbon bonds are now widely used as catalysts for organic and materials synthesis. Among such transformations, olefin metathesis (OM) occupies a position of pre-eminent significance. Alkyne metathesis holds great promise, but remains in a much lower state of development. The OM-directed work in this thesis sought to advance the state of the art in living, Ru-catalyzed ringopening metathesis polymerizations (ROMP). Currently, the first- and third-generation Grubbs initiators, which exhibit the ease of handling characteristic of the late metal ruthenium, dominate ROMP applications. These initiators are characterized by extremes of reactivity, however. We describe the first ruthenium initiator capable of living ROMP at RT, irrespective of monomer bulk. Polydispersity indices as low as 1.03 are routinely attainable, and excellent control is maintained in synthesis of diblock copolymers from sterically demanding and sterically unencumbered monomers. Work on alkyne metathesis sought to expand existing understanding of the features that influence stability and reactivity in ruthenium carbynes. A classification system was developed in which Class A carbynes were defined as those that readily undergo conversion into an M=C entity (e.g. vinylidene, allenylidene, or alkylidene); Class B carbynes those that have a stable carbyne functionality. Four Ru carbyne complexes, all initially regarded as prospective Class B carbynes, were selected for study. Investigation of their reactivity resulted in categorization of several as Class A species, and development of design criteria that may open the door to assembly of stable, well-defined carbyne complexes of ruthenium.
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SELECTIVITY OF METATHESIS REACTIONS CATALYZED BY SUPPORTED COMPLEXES OF GROUP VIWackerow, Wiebke 11 1900 (has links)
The general objective of this thesis is the analysis of selective reactions for group VI
grafted metal complexes via methods and principles of SOMC. For this objective, three
approaches have been chosen.
The first chapter is an introduction to the topic of selectivity in catalysis, emphasizing
heterogeneous catalysis and more specifically the different approaches to support
catalysts on surfaces. The concept of catalysis by design is introduced as a new way to
use the surface as a ligand.
Chapter 2 presents the results of a library of well-defined catalysts of group VI with
identical catalytic functionality, but different ligand environment. The results reveal, that
metal-carbynes are able to switch their catalytic reactivity based on the substrate that
they are contacted with. The difference in reaction mechanisms and the differing
reactivities towards the substrates are presented. It can be concluded that the classical
ROMP is selectively achieved with cyclic alkene substrates leading to polymers whereas
cyclic alkanes yield exclusively higher and lower homologues of the substrate without
polymeric products.
Chapter 3 presents the study of olefin metathesis of cis-2-pentene with metal-carbynes
of group VI, where the selectivity of the catalyst library towards yield of cis-/trans products
is analyzed. It is presented, that the ligand environment of the catalysts is showing an
influence in the selectivity. Rates of cis/trans isomerization of the products are high and
are approaching thermodynamic equilibrium at high conversion. Product isomerization,
thermodynamic equilibrium and reactivity differences between liquid phase and gas
phase products are analyzed.
Chapter 4 presents the full characterization of tungsten-hydrides by selective
transformation into tungsten-hydroxides. These newly discovered well-defined tungstenhydroxides are fully characterized by ICP, TEM, DRIFT, double quantum and triple
quantum solid-state NMR. The presented results allow to predict that tungsten-hydrides
on KCC-1700 are present as two distinct species. Catalysis results with cyclooctane show,
that due to burial of the complexes in the KCC-1700 surface the tungsten-hydrides are less
active towards cyclic alkane metathesis reactions with bulky cyclooctane than the metalcarbyne complexes.
Chapter 5 is giving a conclusion of results and an outlook for catalytic applications of the
generated tungsten-hydroxides of chapter 4.
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Transporte de portadores minoritários que justificam o regime de ressonância eletrônica em sistemas de carbynesOLIVEIRA, Antonio Wanderley 24 February 2016 (has links)
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Previous issue date: 2016-02-24 / Uma das metas para a expansão do conhecimento em eletrônica molecular pode ser encontrada no projeto relacionado com a criação de circuitos em nanoescala com base em características de corrente-tensão não lineares, composto por moléculas ligadas a eletrodos metálicos sob a ação de um campo elétrico externo. O desenvolvimento de dispositivos eletrônicos moleculares que utilizam sistemas exibindo recursos semelhantes como materiais semicondutores intrínsecos é uma das metas a serem atingidas por uma extensa pesquisa em nanotecnologia. Assim, este trabalho tem como objetivo a expansão do conhecimento não só do transporte eletrônico, mas também as características físicas que justificam o regime de ressonância para o transporte eletrônico, como a condutância e Espectroscopia de Voltagem de Transição. Foi investigado teoricamente o transporte de carga eletrônica em um sistemamolecular composto por estruturas de carbyne levando em conta as variações nos tipos de ligações−≡− (ligações simples e triplas para cada carbono). Os cálculos e aproximações ab initio são realizados para investigar a distribuição de estados de elétrons através da molécula na presença de um campo elétrico externo. Este novo dispositivo nanoeletrônico suscitará vantagem para o projeto de grandes circuitos orgânicos/metálicos híbridos 1D com um aumento do fluxo eletrônico que é importante para as necessidades da nanotecnologia. / One of the goals for the expansion of knowledge in molecular electronics may be found in the Project related to the creation of nanoscale circuits based on nonlinear current–voltage characteristics composed by molecules connected to metallic electrodes under the action of an external electric field. The development of molecular electronic devices using systems exhibiting similar feature as intrinsic semiconductor materials is one of the goals to be achieved by an extensive research in nanotechnology. Thus, this work aims at expanding of knowledge not only of the electronic transport, but also the physical features that justify the resonant regime for electronic transport, such as conductance and Transition Voltage Spectroscopy. We theoretically investigate the electronic charge transport in a molecular system composed by carbyne structures taking into account the variations in the bonds −≡− type (simple and triple bonds for each carbon). Ab initio calculations approximations are performed to investigate the distribution of electron states over the molecule in the presence of an external electric field. This new nanoelectronic device raise up advantage for the design of large 1D hybrid organic/metallic circuits with an increased electronic flow that is importante for the needs of nanotechnology.
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