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Dissertations / Theses on the topic 'Organometallic Chemistry'

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Published: 4 June 2021
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1

Chatakondu, Kalyan. "Organometallic intercalation chemistry." Thesis, University of Oxford, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.258017.

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2

Polywka, M. E. C. "Mechanistic organometallic chemistry." Thesis, University of Oxford, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.253399.

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3

Brown, Stephen L. "Mechanistic organometallic chemistry." Thesis, University of Oxford, 1986. http://ora.ox.ac.uk/objects/uuid:96218480-9b1d-4d53-9d1d-033e2b451818.

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A number of organometallic transformations related to proposed elementary steps in the reductive polymerization of carbon monoxide are discussed. The use of isonitrile as model ligands for carbon monoxide, with which they are isoelectronic, is proposed. Investigations show that alkyl migration to isonitrile is preferred over migration to carbon monoxide. Iminoformyl products due to hydride migration to isonitrile are not, however, observed. Syntheses of a range of cationic complexes of the type [ (η5-C5H5)M(L)2(CNR)]+, [(η5-C9H7)Ru(L)2(CNR)]+ and [(η5-C9H7)M(L)2(CO)]+ (M = Fe, Ru; L = CO, phosphine) are described. In two cases, addition of hydride to the isonitrile cations is followed by protonation on work-up to give aminocarbene complexes. These are inert to further reduction under the conditions employed. The majority of isonitrile cations lose the isonitrile ligand to give good yields of metal hydride complexes. A mechanism involving ring-slippage of the hydrocarbon ligand is implicated. Hydride addition to η5-C9H7 complexes results, in the majority of cases, in loss of the hydrocarbon ligand from the complex and recovery of indane. Evidence for the intermediacy of metal formyl complexes in a number of hydride donation reactions is presented. These formyl complexes are formed from carbonyl hydride complexes either under moderate CO pressure or in THF solution. Hydride complexes lacking a carbonyl ligand are found to be inert. Finally, two reactions, one involving an alkyl migration reaction catalyzed by silver(I) salts, and the other involving the reduction of a metal acyl ligand to metal alkyl, are combined to demonstrate a model for carbon chain growth at a metal centre. The synthesis of an iron pentanoyl complex, followed by a decomplexation reaction, gives pentanoic acid in which all the catbon atoms are potentially directly derived from carbon monoxide. This is the first synthesis of a single homologous acid from carbon monoxide.
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4

Ortuño, Maqueda Manuel Ángel. "Scope of computational organometallic chemistry. Structure, reactivity and properties." Doctoral thesis, Universitat Autònoma de Barcelona, 2014. http://hdl.handle.net/10803/285645.

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La química organometálica se define como el área de conocimiento que une el mundo orgánico (ligando) con el inorgánico (metal), aprovechando lo mejor de ambos. Un aspecto interesante de los compuestos con metales de transición es la capacidad de realizar transformaciones químicas que no se pueden llevar a cabo fácilmente usado química convencional. Entre los retos que la química organometálica puede abordar se incluyen energías renovables, nuevos materiales y síntesis de compuestos de alto valor añadido. En este contexto, la química computacional juega un papel muy importante a la hora de entender los fenómenos químicos. La inmensa cantidad de técnicas disponibles permite analizar distintos tipos de enlace, proponer mecanismos de reacción, mejorar procesos catalíticos e incluso estimar propiedades espectroscópicas. En resumen, esta tesis cubre diferentes aspectos de la química organometálica desde un punto de vista computacional. El grueso de resultados se divide en tres capítulos: Estructura, Reactividad y Propiedades. En Estructura (i) se analiza la geometría de compuestos paramagnéticos de Pt(III) con el objetivo de distinguir entre estructuras plano-cuadradas y de tipo balancín, y (ii) se estudia la presencia de interacciones agósticas en especies insaturadas de Pt(II). En Reactividad (i) se evalúan los efectos estéricos y electrónicos de carbenos N-heterocíclicos en reacciones de activación C–H mediadas por platino, (ii) se explica el rol de la base en la etapa de transmetalación de reacciones de acoplamiento cruzado tipo Suzuki–Miyaura, y (iii) se proponen posibles mecanismos para justificar los productos observados en reacciones de vinilación con silanos catalizadas por paladio. En Propiedades (i) se predicen las constantes de acidez de varios complejos de dihidrógeno (Fe, Ru y Os) en agua, y (ii) se estiman los desplazamientos químicos de resonancia magnética nuclear de 103Rh en complejos de Rh(bisfosfina), correlacionándolos con distancias de enlace Rh–P. Como conclusión general, esta tesis demuestra como la química computacional se puede aplicar adecuadamente para explicar diversos tipos de problemas en química organometálica.
Organometallic chemistry stands for the area of expertise which manages to join organic (ligand) and inorganic (metal) worlds, taking advantage from both of them. One interesting feature of transition metal species is the possibility of promoting chemical transformations that cannot simply be performed using straightforward chemistry. The challenges that organometallic chemistry can address concern renewable energies, new materials, and fine chemical synthesis, among others. Under this scene, computational chemistry can play a major role in understanding chemical phenomena. The extensive toolbox of available techniques allows to analyse bonding situations, propose reaction mechanisms, improve catalytic processes, or estimate spectroscopic properties. In a nutshell, the current dissertation covers different aspects of organometallic chemistry from a computational point of view. The body of results is divided into three main chapters: Structure, Reactivity and Properties. Structure (i) analyses the geometry of paramagnetic Pt(III) compounds in order to discern between square-planar and see-saw dispositions and (ii) evaluates the presence of agostic interactions in low-coordinate Pt(II) species. Reactivity (i) studies the steric and electronic properties of N-heterocyclic carbenes in Pt-mediated C–H bond activations, (ii) unravels the role of the base in Suzuki–Miyaura cross-coupling transmetalation processes, and (iii) proposes feasible mechanisms of Pd-catalysed Si-based vinylation reactions to account for the different products experimentally observed. Properties (i) predicts the acid constants of several transition metal (Fe, Ru, Os) dihydrogen complexes in water and (ii) estimates the 103Rh NMR chemical shifts of Rh(bisphosphine) species, building correlations with Rh–P bond distances. As general conclusion, this thesis illustrates how computational chemistry can successfully be applied to explain a wide number of different chemical problems in the organometallic field.
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5

Leckey, N. T. "Studies in organometallic chemistry." Thesis, University of Ulster, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.378730.

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6

Wierzchleyski, Adam Tomasz. "Diastereoisomeric control in organometallic chemistry." Thesis, Imperial College London, 1995. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.261719.

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7

Michaelidou, Despo M. "Synthetic studies in organometallic chemistry." Thesis, University of Oxford, 1993. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.358726.

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8

Corradi, Marco Michael. "Aspects of d'o organometallic chemistry." Thesis, University of Sussex, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.241717.

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9

Nairn, Jacqueline G. M. "Organometallic chemistry of triosmium clusters." Thesis, University of Edinburgh, 1995. http://hdl.handle.net/1842/15481.

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The interaction of transition metal carbonyl clusters with unsaturated cyclic and polycyclic ligand systems continues to stimulate ongoing research and this thesis is concerned mainly with the reactions of triosmium carbonyl clusters with such compounds. Chapter one contains a brief summary of triosmium dodecacarbonyl chemistry, incorporating both synthesis and reactivity. The arene chemistry of mononuclear complexes and cluster compounds is also discussed. Over the last decade there has been serious debate on the validity of the cluster-surface analogy; the boundary conditions are addressed herein. Chapter two details alternative synthetic routes to the compound M3(CO)9(μ-η2..η2..η.2-C6H6) [M = Ru, Os]. A series of substituted 1,3-cyclohexadiene ligands have also been prepared and reacted with the cluster Os3(CO)10(MeCN)2. The successful synthesis of the bis-benzene cluster Os3(CO)6(μ3-η2..η2..η2.-C6H6)(η6-C6H6) is reported in chapter three. The systematic stepwise reaction of Os3(CO)9(μ3-η2..η2..η2-C6H6) with trimethylamine-N-oxide and 1,3-cyclohexadiene leads to the formation of a range of benzene-diene clusters, all of which have been fully characterised. Their isomeric and fluxional behaviour has also been studied. The reactions of acenaphthylene, C12H8, a stable tricyclic system with 12 π-electrons available for bonding, are reported for Ru3(CO)12 and Os3(CO)12 in chapter four. The resulting compounds demonstrate the range of bonding modes adopted by this flexible ligand.
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10

Williams, Michael Lloyd. "New aspects of organometallic chemistry /." Title page, contents and abstract only, 1985. http://web4.library.adelaide.edu.au/theses/09PH/09phw725.pdf.

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11

Peatt, Anna C. (Anna Clare-Doreen) 1976. "New reaction media for organometallic chemistry." Monash University, School of Chemistry, 2003. http://arrow.monash.edu.au/hdl/1959.1/5829.

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12

Qin, J. "Studies in organometallic solid state chemistry." Thesis, University of Oxford, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.379942.

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13

King, Jennifer L. "Organometallic chemistry in supercritical fluid solution." Thesis, University of Nottingham, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.262952.

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14

Jordan, Linda. "Organometallic linkers for solid-phase chemistry." Thesis, University of Glasgow, 2004. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.400783.

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15

Cartwright, Jonathan. "Organometallic chemistry of ruthenium phosphine complexes." Thesis, University of Warwick, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.307976.

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16

Ryan, C. P. "Advances in organometallic and protein chemistry." Thesis, University College London (University of London), 2010. http://discovery.ucl.ac.uk/20307/.

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This thesis describes two areas of scientific investigation. The first contains a description of a study on the synthesis of biotinylated and fluoresceinylated bromomaleimide based reagents. Upon synthesis, the ability of these reagents to add reversibly to cysteine containing proteins is investigated by a series of LCMS experiments. A single point mutant (L111C) of the SH2 domain of the Grb2 adaptor protein, containing a single cysteine residue, is chosen as an ideal protein for study. Thus biotinylated and fluoresceinylated mono and dibromomaleimide reagents are added to Grb2 at 0°C, 21 °C and 37 °C for 2 h at pH 7 and 8 to give protected Grb2-bromomaleimide adducts in high yield and removed using 100 eq of beta-mecaptoethanol for 4 h to return original Grb2 protein intact. Reversibility is shown to be abolished by hydrolysis of the maleimide motif, a process more prevalent in the fluoresceinylated and dibrominated maleimide reagents than for the biotinylated and monobrominated reagents. LCMS is used to investigate the insertion of these reagents reversibly into the single disulfide bridge of somatostatin, a process shown to be complete within 1 h at 21 °C and pH 6. Reduction using 100 eq of beta-mecaptoethanol is shown to take place within 1 h. Additionally no hydrolysis is observed at pH 6, suggesting that with careful control of pH, reversibility of the bromomaleimide reagents can be switched on and off. The second part of the thesis contains a study on mechanistic aspects of organopalladium catalysis, particularly the factors affecting the final reductive elimination stage of the palladium catalysed alkyl amination reaction. DFT calculations have been used to obtain a number of energy level diagrams for the potential energy surface of Pd(IBu)(neopentyl)(morpholide), the three coordinate palladium complex believed to be the species from which reductive elimination takes place. From this it has been found that two different pathways are available; reductive elimination or morpholide promoted C-H activation of the neopentyl motif, the latter of which was favoured. The reaction pathway for reductive elimination from Pd(IBu)(neopentyl)(morpholide) is compared with Pd(IBu)(phenyl)(morpholide), Pd(PCyp3)(neopentyl)(morpholide) and Pd(IBu)(methyl)(morpholide), to show that the phenyl system is considerably lower in energy. The energy requirements for (i) reductive elimination, (ii) morpholide promoted C-H activation and (iii) β-hydride elimination from Pd(IBu)(2-dimethylpropyl)(morpholide) are compared, and shown to be in the order of energy (i)>(ii)>(iii). Additionally, the rate of reaction increases as the number of available reaction sites increases, again making reductive elimination the least favoured process. Offline ESI(+)-MS analysis have been used to monitor the reaction progress of Pd(IBu)(neopentyl)(morpholide) and Pd(IBu)(phenyl)(morpholide) three coordinate complexes. Whilst transient palladium-bound species can be observed for Pd(IBu)(phenyl)(morpholide), for Pd(IBu)(neopentyl)(morpholide) this is not the case, an artefact of the superiority of the sp2 phenyl system over the sp3 alkyl system.
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17

Abdelsalam, Mansour. "Synthesis of piperidines using organometallic chemistry." Thesis, University of Sheffield, 2013. http://etheses.whiterose.ac.uk/4069/.

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18

Wilkinson, Della Ann. "Organometallic chemistry of metal carbonyl clusters." Thesis, University of Cambridge, 1990. https://www.repository.cam.ac.uk/handle/1810/272963.

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19

Gregory, M. F. "Organometallic intermediates." Thesis, University of Nottingham, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.356021.

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20

Gordon, Charles M. "Organometallic intermediates." Thesis, University of Nottingham, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.334789.

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21

Bhandari, Sonali. "Organometallic tetrazoles." Thesis, University of Bath, 1998. https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.390309.

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22

Cooper, Robert Thomas. "η8-Permethylpentalene titanium chemistry." Thesis, University of Oxford, 2012. http://ora.ox.ac.uk/objects/uuid:c4c3911b-1924-4e2f-a750-d07599900756.

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The focus of this thesis is the synthesis of organometallic complexes incorporating the η8-permethylpentalene titanium moiety (η8-Pn*Ti), their characterisation, and their reactivity with small molecules. Chapter One summarises the chemistry of the pentalene molecule, from its instability in the free state to the incorporation of the hydrocarbon into organometallic complexes. The chapter continues with a review of the coordination modes available to Pn and concludes with a brief discussion on the effects of permethylation of hydrocarbon ligands and the advent of permethylpentalene (Pn*). Chapter Two documents the improved synthesis of [Pn*TiCl(μ-Cl)]2 utilising isomeric control imparted on the Pn* synthon, Pn*(SnMe3)2. This protocol permits access to a variety of methylated compounds through metathesis chemistry, of which five have been crystallographically elucidated, revealing the fold angle to be reliant on an interplay between steric and electronic factors. Mono-, bi- and trimetallic {Pn*TiMe2, [Pn*TiMe(μ-Cl)]2 and [Pn*Ti(μ-Me)]2(μ-CH2), and [Pn*TiMe(μ-Me)2]2Mg respectively} species were synthesised dependent on the methylating agent employed and they displayed varying thermal stabilities, with the dimeric nature of [Pn*TiMe(μ-Cl)]2 proving crucial in the formation of [Pn*Ti(μ-Cl)]2(μ-CH2). Chapter Three describes the incorporation of classical organometallic ligands into the Pn*Ti moiety, including the first examples of benzyl, alkyl, aryl, allyl and η1-Cp bound to a PnTi fragment. Seven complexes have been structurally characterised including the first ever crystal structure of a π-hydrocarbon bound Ti species bearing two CH2tBu groups, Pn*Ti(CH2tBu)2, and the fluxional mixed hapticity complex Pn*Ti(η5-Cp)(η1-Cp), whose η1-Cp rearranges via a 1,2-sigmatropic shift. Chapter Four investigates the reactivity of the monomeric dialkyls, Pn*TiR2 (R = Me, CH2Ph, CH2SiMe3 and CH2tBu) with CO2, CO and H2. All four compounds demonstrate “normal” insertion of the CO2 moiety into both Ti-R bonds, revealing a symmetrical bidentate coordination of the RCO2 units. Computational studies have highlighted two competing pathways for their reaction with CO, dependent on the concentration of CO and size of R, which results either in formation of an enediolate or a titanoxirane. The reaction with H2 yields the fascinating trimeric mixed valence, [Pn*Ti(μ2-H)]3(μ3-H), the first structurally characterised example of a trimeric Ti-H species and the first to include a Ti-(μ3-H) moiety. (Pn*TiCl)2(μ-O) is formed by the action of adventitious H2O and possesses a linear Ti-O-Ti bridge with a degree of Ti-O double bond character, supported by crystallographic data and DFT calculations. Chapter Five discusses ethylene polymerisation studies on the monomeric dialkyl complexes Pn*TiR2 (R = Me, CH2Ph, CH2SiMe3 and CH2tBu) using the activators [Ph3C][B(C6F5)4], [PhNMe2H][B(C6F5)4], AliBu3 and H2. Chapter Six presents full experimental procedures for all of the syntheses and reactions outlined in Chapters Two to Five. Chapter Seven details characterising data for all novel compounds, and crystallographic data in the form of CIF files may be found in the electronic version.
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23

Humphrey, Mark Graeme. "Aspects of organometallic chemistry, particularly metal alkynyl and cluster chemistry." Title page, contents and abstract only, 2002. http://web4.library.adelaide.edu.au/theses/09SD/09sdh9267.pdf.

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Includes bibliographical references. Details research carried out into the nonlinear optical properties of metal alkynyls, chiefly organoruthenium complexes, showing that these complexes can be designed to have very large NLO coefficients. Also demonstrates the utility of spectroscopic, electrochemical and copmutational aids as predictive tools for NLO materials. Also examines cluster synthesis, reactivity and physical properties using ruthenium clusters and hard-donor ligands, affording a series of cluster complrxes that provide structural models for industrially-important hydrotreating intermediates.
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24

Fitzpatrick, Kevin. "Organometallic chirality recognition." Thesis, University of Oxford, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.359451.

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25

Seymour, L. C. "Chiral organometallic ligands." Thesis, University of Oxford, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.279979.

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26

Moss, James Edward. "The Synthesis and Organometallic Chemistry of NonamethyIfluorene." Thesis, University of Oxford, 2007. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.491509.

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The focus of this thesis is the synthesis and organometallic chemistry of the nonamethylfluorene ligand (Flu*). Chapter One summarises the properties and uses of the fluorene molecule and the incorporation of both the neutral and deprotonated forms of the ligand into organometallic complexes. The chapter concludes with a discussion of the properties that are bestowed upon organometallic compounds containing fully methylated ligands, detailing the need for nonamethylfluorene. Chapter Two describes a relatively high yielding total synthesis of the fully methylated fluorene, Flu*H, using techniques and equipment that are amenable to most laboratories. All but one of the precursors have been crystallographically characterised, and this analysis shows in all cases a twisted fluorene skeleton due to unfavourable close contacts between methyl groups. Octamethyldibenzofulvene has been radically coupled to form an ethane bridged ligand set using a technique not previously used for fluorene. Chapter Three documents the interaction of the neutral polymethylated fluorenes Flu*H and Flu'H with Cr, Fe and Mn. Both mono and bimetallic complexes have been isolated, and many have been crystallographically characterised. In the monometallic case, haptotropic shifts are seen for both Fe and Cr, but deprotonation of the Mn complex yields a previously unknown coordination mode of fluorene. DFT studies of the protonated and deprotonated bimetallic Cr complexes give an indication of the mode of metal-ligand binding, and this is confirmed by a crystallographic study. Bimetallic Fe complexes have been shown to be active catalysts in the dechlorination of PCBs, toxic environmental pollutants. Chapter Four describes the synthesis of Flu* transfer reagents; the crystal structure of the lithiate Flu*Li.TMEDA has been determined and shows a twisted fluorene skeleton. DFT studies on both the protonated and deprotonated, methylated and nonmethylated fluorenes have been performed to examine the distribution of charge in these molecules. Chapter Five discusses the interaction of the transfer reagents described in Chapter Four with a variety of metal precursors. Reasons for the observed lack of stability of Flu* containing complexes are given. The synthesis and molecular structure of complexes of Zr and In are reported; the Zr compound represents the first crystallographically characterised mono-fluorenyl Zr complex not containing a supporting heteroatom. The interaction of EBFlu*2- with metal precursors is also examined. Chapter Six describes the synthesis of mono and bimetallic Co complexes of octamethylfluorenone. Crystal structure determinations show that the Cp*Co fragment dearomatises both six membered rings in the fluorenone, only the second example ofthis type ofcoordination. Chapter Seven contains experimental procedures, Chapter Eight details characterising data for all new compounds, and crystallographic data in the form of CIF files may be found in the electronic Appendix, found on the compact disc at the back of this thesis.
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27

Lunniss, Julie Amanda. "Organometallic chemistry of some hydrido osmium cluster." Thesis, University of Cambridge, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.279819.

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28

Suman, Priya. "The inorganic and organometallic chemistry of paracyclophanes." Thesis, Imperial College London, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.299296.

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29

Davin, Thomas J. "Computational chemistry of organometallic and inorganic species." Thesis, University of Glasgow, 2009. http://theses.gla.ac.uk/925/.

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This thesis presents computational investigations of problems related to redox processes and structural rearrangement in inorganic systems. Density functional theory has been used to gain insight into the origin and nature of such reactions. The work presented concerns two main topics: hydrogenase-like systems containing an Fe2 core and carbonphosphorus cluster compounds. In chapters II and III, we describe the impact of reduction, an important phenomenon in the H2 production catalytic cycle, on a hydrogenase-like model. In collaboration with Talarmin and co-workers who have conducted careful electrochemical studies, we have used DFT to identify structures of species observed in cyclic voltammetry. We have also studied the binding of a proton to similar systems and, through the calculation of chemical shifts and coupling constants, confirmed the structures of iron hydrides observed by 1H NMR spectroscopy. In chapter V we focus on carbon-phosphorus systems that can exist in 2 or more isomeric forms. We address first the case of a system of formula C6H4P3 which has the right valence configuration to exist either as a planar structure or as a 3-dimensional cluster (nido according to Wade’s rules). We then examine whether it is possible to control the preferred conformation by the addition of substituents on the phenyl ring. Finally, we look at the rearrangement of a planar diphosphene into a cage isomer and try to understand the mechanism and in particular the role of the protonation in the conversion from planar to 3-dimensional structure.
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30

Prior, Neville D. "Some organometallic chemistry of osmium carbonyl clusters." Thesis, University of Cambridge, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.257045.

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31

Nahar, Saifun. "The chemistry of mixed-metal organometallic clusters." Thesis, University of Cambridge, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.624749.

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32

Crossman, Martin Charles. "Teflate : an exotic ligand in organometallic chemistry." Thesis, University of Leicester, 1995. http://hdl.handle.net/2381/34070.

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The work described within this thesis is concerned with the preparation and characterization of organometallic teflate (-OTeF5) complexes. Herein are reported a range of novel organometallic species utilizing metals from much of the transition series. The cyclopentadienyl complexes, Cp2M(OTeF5)2 [M = Ti , Zr, Hf , Mo ,W] are readily prepared by halide/teflate metathesis reactions of Cp2MCI2 with HOTeF5, and are considered as the first high valent organometallic teflate compounds. Fluoride/teflate metathesis may also be exploited with the carbonyl fluorides and carbonyl phosphine fluorides of osmium and iridium. This route provides evidence for the first instance of an Ir-OTeF5 bond. Non-metathetical methods for introducing the OTeF5 ligand are examined with the oxidation reactions of xenon bisteflate with ; M2(CO)10 [M = Mn , Re], M3(CO)12 [M = Ru , Os], lr4(CO)12 and Ru(CO)3(PPh3)2. This new procedure for preparing low valent metal teflate compounds is assessed and compared with the analogous xenon difluoride reactions. Protonation of Os3(CO)12 in a strong acid (AHF) results in the formation of a hydride bridged cation, [Os3(CO)12H]+. The crystal structure of [Os3(CO)12H] + [W2O2F9]- is reported. The reactivity of cis-(HO)2Tep4, a potential bidentate ligand of high electronegativity is investigated with a variety of compounds ; Cp2TiCl2, cis-(PEt3)2PtCl2 and MFe [M = Mo , W, Te].
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33

Kingsley, Andrew James. "Studies in early transition metal organometallic chemistry." Thesis, Durham University, 1998. http://etheses.dur.ac.uk/4846/.

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The work in this thesis is separated into two sections: Chapters 1 to 6 are concerned with the synthesis and characterisation of amide functionalised cyclopentadienyl complexes of Group 4, 5, 6 and 8 transition metals. Chapters 7 to 9 involve a study into complexes containing potential a-agostic interactions. Chapter 1 provides an introduction to functionalised cyclopentadienyl complexes and also to the ligand C(_5)H(_5)(CH(_2))(_3)N(H)Me. Chapter 2 describes the synthesis of the Group 6 complexes of tungsten and molybdenum, M[ƞ(^5):ƞ(^1)-C(_5)H(_4)(CH(_2))(_3)NMe](NR)(_2) by different routes, their chemistry, and subsequent reactions. Chapter 3 covers the preparation of the Group 4 complexes of zirconium and titanium, M[ƞ(^5):ƞ -C(_5))H(_4)(CH(_2))(_3)NMe](C(_5)H(_5))Cl, their subsequent reactions, and potential as olefin polymerisation catalysts. Chapter 4 contains the synthesis of the Group 5 complexes of niobium and tantalum, M[ƞ(^5):ƞ(^1)-C(_5)H(_4)(CH(_2))(_3)NMe](N(^t)Bu)(NH(^t)Bu).Chapter 5 deals with the preparation of the Group 5 and 6 vanadium and chromium chloride complexes M[ƞ(^5):ƞ(^1)-C(_5)H(_4)(CH(_2))(_3)NMe]Cl, their reactions, and potential as olefin polymerisation catalysts. Chapter 6 descibes the preparation of some iron complexes. The synthesis of the ferrocene, Fe[ƞ(^5)-C(_5)H(_4)(CH(_2))(_3)N(H)Me](_2), and the bridged carbonyl complex, {Fe[ƞ(^5):ƞ(^1)-C(_5)H(_4)(CH(_2))(_3)N(H)Me](CO)(μ-CO)}(_2), are described. Chapter 7 provides an introduction to a-agostic interactions, the use of the Isotopic Perturbation of Resonance (IPR) technique as a means of characterisation, and the preparation of deuterated starting materials to perform such investigations. Chapter 8 investigates the complexes MeTiC(_3)L (L = dme, tmeda, diphos), W(N(^t)Bu)(_2)Me(_2), and Mo(N-(_2),(_6)-(^i)Pr(_2)C(_6)H(_3))(_2)Me(_2) for a-agostic interactions, using the IPR technique Chapter 9 describes the synthesis of and investigation for a-agostic bonds in zirconium and titanium neopentyl chloro complexes MNp(_x)Cl(_4-x) (x = 1 - 4).The Appendices outline the preparative and analytical methods used, and X-ray crystallographic data.
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34

Lin, Bing. "Organometallic chemistry of transition metal polyyne complexes." Thesis, University of Cambridge, 1993. https://www.repository.cam.ac.uk/handle/1810/272565.

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35

Griffiths, Clare. "The organometallic chemistry of some ethynylpyridine complexes." Thesis, University of Cambridge, 2003. https://www.repository.cam.ac.uk/handle/1810/272042.

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36

Lovett, Victoria Jane. "Synthesis of amino acids using organometallic chemistry." Thesis, University of Sheffield, 2013. http://etheses.whiterose.ac.uk/5416/.

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37

Wong, Chun Kin. "The chemistry of organometallic derivatives of oligoacetylenic silanes." HKBU Institutional Repository, 2002. http://repository.hkbu.edu.hk/etd_ra/424.

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38

Bowser, Richard. "Photopolymerisation using organometallic initiators." Thesis, City University London, 1993. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.358010.

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39

Atkinson, Francis Louis. "Redox-active organometallic complexes." Thesis, University of Bristol, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.386221.

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40

Jackson, Patricia A. "Mixed-metal organometallic clusters." Thesis, University of Cambridge, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.304280.

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41

Coverdale, James P. C. "Catalytic organometallic anticancer complexes." Thesis, University of Warwick, 2017. http://wrap.warwick.ac.uk/99039/.

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Half-sandwich complexes of ruthenium, iridium, and more recently osmium, have shown promise as anticancer agents. Many of these ‘piano-stool’ complexes appear to target the redox balance in cells. Separately, similar complexes have been investigated for the catalysis of hydrogenation reactions, with many examples achieving high turnover frequencies and enantioselectivities. This thesis is concerned with achieving in cell catalysis to increase drug potency and generate selectivity for cancer cells. A series of eighteen Os(II) and Ir(III) complexes, of the type [M(ηx-arene)(diamine)] (Os-arene: p-cymene, biphenyl, or m-terphenyl; Ir-arene: Cp*, CpxPh, or CpxBip), were synthesised and fully characterised. The structures were derived from a Ru(II) transfer hydrogenation catalyst [Ru(η6-p-cymene)(TsDPEN)], TsDPEN = N-tosyl-diphenyl-ethylenediamine. The complexes were isolated as 16-electron amido catalysts, which were highly stable in solution and upon storage, unlike their 16-electron Ru(II) counterparts, and were highly active for asymmetric transfer hydrogenation of ketones. Os complexes afforded enantiomerically-pure alcohols with high conversion and enantioselectivity (> 99%) at rates exceeding those of the existing Ru catalyst. Two Os and Ir complexes were explored for the conversion of NADH to its oxidised form (NAD+) under physiologically-relevant conditions. Antiproliferative activities determined in 14 human cell lines correlated with experimentally-determined hydrophobicities. Typically, Os catalysts were found to be more active than their Ir counterparts, though were internalised by cancer cells to a lesser degree, suggestive of a more potent in-cell mechanism of action. Structural modifications identified an apparent inert site of substitution on the sulfonamide substituent. Furthermore, their potency towards cancer cells was increased in combination with L-buthionine sulfoximine, an inhibitor of glutathione synthesis. Acute in vivo toxicities were determined in zebrafish, and all compounds investigated exhibited lower toxicities than the Pt anticancer drug, cisplatin. The complexes were shown to generate reactive oxygen species (ROS) in cancer cells, and similarly generated ROS in zebrafish. Transfer hydrogenation catalysis was explored under physiologically-relevant conditions using sodium formate as a biologically-compatible hydride source. Osmium complexes catalysed the reduction of pyruvate, a key metabolite in cells, to either L-lactate or D-lactate, selectively (ca. 83% ee). Upon co-administration of the catalyst and sodium formate, cancer cell proliferation was decreased by up to 13× (relative to cells treated with the catalyst alone), while no sodium formate effect was determined in non-cancerous cells. Importantly, the treatment of cells with a particular enantiomer of the Os catalyst and sodium formate facilitated the in cell reduction of pyruvate to D-lactate, providing, to the best of my knowledge, the first example of a synthetic catalyst carrying out asymmetric transfer hydrogenation chemistry in cells.
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42

Peori, M. Brad (Michael Brad). "New synthetic routes to organometallic dendrimers." Thesis, McGill University, 2001. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=33819.

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The incorporation of organometallic motifs into dendrimers offers significant potential in building macromolecular species with desired properties for heterogenizing homogeneous catalysis. To this end, poly-phosphorus monomers O=P[O(CH 2)3PPh2]3, P[O(CH2) nPPh2]3, PhP[O(CH2)nPPh 2]2 (where n = 3, 10) were prepared, and their complexation chemistry with [mup-Cl)(1,5-C8H12)Rh]2 was examined. It led a new route to contruct multimetallic compounds, in which the evolving structure is controlled by the phosphorus units yielding either typical spherical or non-spherical macromolecules. Selected polymetallic complexes formed using these poly-phosphorus ligands were found to be active catalysts for olefin hydrogenation. A novel divergent synthetic route to starburst dendritic structures was also developed by preparing monomers such as Si[O(CH2 )nPPh2]4, MeSi[O(CH2) nPPh2]3 (where n = 3, 10, 16), and Me2Si[O(CH 2)nPPh2]2 (where n = 3, 10). They were then linked with transition metals to produce starburst organometallic dendrimers Si[O(CH 2)nPPh2Ni(CO)2PPh3] 4, MeSi[O(CH2)nPPh2Ni(CO)2PPh 3]3 (where n = 3, 10, 16), Me2Si[O(CH2) nPPh2Ni(CO)2PPh3]2 (where n = 3, 10) and Si[O(CH2)nPPh2RhCl(1,5-COD)] 4, MeSi[O(CH2)nPPh2RhCl(1,5-COD)] 3 (where n = 3, 10, 16) Me2Si[O(CH2)nPPh 2RhCl(1,5-COD]2 (where n = 3, 10).
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43

Khattar, Rajesh. "Aspects of organometallic chemistry of some osmium clusters." Thesis, University of Cambridge, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.328690.

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44

Siriwardene, D. K. "Some organometallic chemistry of tungsten and related studies." Thesis, University of Oxford, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.382672.

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45

Goff, Simon E. J. "Organometallic chemistry at high pressures and low temperatures." Thesis, University of Nottingham, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.338521.

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46

Marshall, Robert. "Preparation of bimetallic catalysts by surface organometallic chemistry." Thesis, Open University, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.265345.

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47

Dutkiewicz, Michal Seweryn. "Organometallic neptunium complexes : synthesis, structure and reduction chemistry." Thesis, University of Edinburgh, 2017. http://hdl.handle.net/1842/25503.

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The aim of the work described in this thesis was to develop a more extensive knowledge of the chemistry of neptunium compounds by making rare, air- and moisture sensitive, low formal oxidation state neptunium compounds with full structural and synthetic characterization. The thesis contains three results chapters. Chapter one introduces neptunium chemistry as a background to the results presented. The first review on the molecular non-aqueous neptunium chemistry is provided and the literature reports to date discussed in the context of this. Chapter two describes exploratory synthetic and structural investigations of the organoneptunium complexes supported by the cyclopentadienyl anion, Cp = (C5H5)-, and the (trimethylsilyl)cyclopentadienyl anion, Cp' = (C5H4[Si(CH3)3])-. The syntheses of [Np(Cp)3]n and Np(Cp')3 complexes are detailed and the effect of the trimethylsilyl group of the ligand on the structure and reactivity have been investigated. Complexes were characterized by single crystal X-ray diffractometry, NMR and ATR(IR) spectroscopy. Both organoneptunium complexes were studied in reactions designed to expand the neptunium redox envelope. Notably, the complex Np(Cp')3 is reduced by KC8 in the presence of 2.2.2-cryptand to afford a product assigned as neptunium(II) complex, K(2.2.2-cryptand)[Np(Cp')3] that is thermally very unstable above approx. -10 ºC, in direct analogy to previously reported uranium, thorium and lanthanide complexes of the general formula, K(2.2.2-cryptand)[M(Cp')3]. The reaction between Np(Cp)3Cl and KCp in THF afforded the unanticipated K[NpIII(Cp)4] product as a result of a single-electron reduction presumably arising from Np–C σ-bond homolysis reactivity. This behaviour appears to be unique amongst the actinides for the An(IV)/An(III) redox couple. Chapter three focuses on oxo-bridged homo and heterometallic complexes. The reaction of NpCp3 with dioxygen afforded not only the simple oxide, (μ-O)[An(Cp)3]2, but also a small quantity of the unexpected new trinuclear oxo- neptunium(IV) compound [{(Cp3Np)(μ-O)}2{Np(Cp)2}], which interestingly contains the rare C2v-symetric [An(Cp)2]2+ structural moiety. This oxo-bridged environment is not paralleled in uranium chemistry. The two isostructural oxides, (μ-O)[An(Cp)3]2 (An = U, Np), allow a comparative study of the magnetic exchange phenomena between the two actinide centres demonstrating an exceedingly strong antiferromagnetic coupling, which is largely independent of the communicated Kramers NpIV (5f3, 4I9/2) or non-Kramers UIV (5f2, 3H4) ions. To design heterobimetallic systems, the uranyl(VI) complexes, [(UVIO2)(THF)(H2L)], supported by the calix[4]pyrrole Schiff base macrocycles, H4LOct and H4LEt, were singly-reduced to uranyl(V) with either of the actinide complexes Np(Cp)3 or U(Cp)3, affording isostructural [(Cp3)AnIVOUVO(THF)(H2L)]. Preliminary investigations of the magnetism of the AnIV-O-UV are reported, although their analysis gave counterintuitive results. Chapter four explores the redox chemistry and molecular and electronic structure of neptunium(III) complexes of the doubly deprotonated trans-calix[2]benzene[2]pyrrole, H2(LAr), macrocycle which has a unique π-bonding potential and conformational flexibility. Interestingly, the reactions with neptunium(IV) chloride yielded mono- and dinuclear neptunium(III) complexes, [(LAr)NpCl] and [(LAr)Np2Cl4(THF)3], with a subsequent elimination of the ligand radical; both complexes adopted η6:κ1:η6:κ1 bis(arene) sandwiched structural motif. In a direct analogy to the redox behaviour occurring in the salt metathesis between Np(Cp)3Cl and KCp, the spontaneous reduction derives from the favourable Np(IV)/Np(III) redox system. The reduction of complex [(LAr)NpCl] with NaK3 in DME produces near-black solutions consistent with [NpII(LAr)(DME)] that in the absence of excess NaK3 gradually convert to the metallated (LAr-H)3- neptunium(III) complex, [K(DME)(LAr-H)NpIII(OMe)]2, featuring the actinide centre bound with a ‘metallocene-type’ geometry provided by the two η5-bound pyrrolides of the ligand. The neptunium(III) compounds were characterized in the solid state by single crystal X-ray diffractometry, ATR(IR) spectroscopy and in a solution by NMR and UV-Vis-NIR spectroscopy.
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48

Sundavadra, Bharat Viram. "The organometallic chemistry of alkyne-bridged bimetallic complexes." Thesis, University of Cambridge, 1993. https://www.repository.cam.ac.uk/handle/1810/272569.

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49

TIANA, DAVIDE. "ORGANOMETALLIC CHEMISTRY FROM THE INTERACTING QUANTUM ATOM APPROACH." Doctoral thesis, Università degli Studi di Milano, 2010. http://hdl.handle.net/2434/150071.

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The Interacting Quantum Atoms approach(IQA) is a recent development of Bader’s QTAM(Quantum Theory of Atoms in Molecules). During the PhD studies the use of pseudopotential inside IQA was implemented allowing the study of transition metal compounds with this techniques. Furthermore IQA concepts were joined with Ponèc’s DAFH (Domain Avaraged Fermi Hole) giving the so-called IQA-EDF-DAFH analysis (EDF= electron-number distribution function) which provide a complete description of the chemical bond in terms of electron density. In order to make benchmark of this new technique classic metal-organic molecules like metal carbonyls, metal hydrides and simple metal dimeric compounds were studied.
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50

Caffyn, Andrew James Morris. "The chemistry of ligand bridged complexes." Thesis, University of Cambridge, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.306343.

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