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Дисертації з теми "Polynuclear Transition Metal Complexes"

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Автор: Grafiati

Опубліковано: 7 вересня 2023

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1

Sun, Ziming. "Polynuclear transition metal complexes and single-molecule magnets /." Diss., Connect to a 24 p. preview or request complete full text in PDF format. Access restricted to UC campuses, 1998. http://wwwlib.umi.com/cr/ucsd/fullcit?p9906469.

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2

Young, George Hansen. "Reactions of transition-metal propargyl complexes with polynuclear metal carbonyls /." The Ohio State University, 1989. http://rave.ohiolink.edu/etdc/view?acc_num=osu1487672631602474.

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3

Ahmed, Ejaz, and Michael Ruck. "Chemistry of polynuclear transition-metal complexes in ionic liquids." Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden, 2014. http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-138716.

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Анотація:

Transition-metal chemistry in ionic liquids (IL) has achieved intrinsic fascination in the last few years. The use of an IL as environmental friendly solvent, offers many advantages over traditional materials synthesis methods. The change from molecular to ionic reaction media leads to new types of materials being accessible. Room-temperature IL have been found to be excellent media for stabilising transition-metal clusters in solution and to crystallise homo- and heteronuclear transition-metal complexes and clusters. Furthermore, the use of IL as solvent provides the option to replace high-temperature routes, such as crystallisation from the melt or gas-phase deposition, by convenient room- or low-temperature syntheses. Inorganic IL composed of alkali metal cations and polynuclear transition-metal cluster anions are also known. Each of these areas will be discussed briefly in this contribution
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4

Stephens, Peter M. B. "Polynuclear transition metal complexes of tetraazamacroycles and their derivatives." Thesis, University of Kent, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.385273.

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5

Lacy, O. M. "Synthesis, structure and reactivity of polynuclear transition metal complexes." Thesis, University of Newcastle Upon Tyne, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.370145.

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6

Ahmed, Ejaz, and Michael Ruck. "Chemistry of polynuclear transition-metal complexes in ionic liquids." Royal Society of Chemistry, 2011. https://tud.qucosa.de/id/qucosa%3A27774.

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Анотація:

Transition-metal chemistry in ionic liquids (IL) has achieved intrinsic fascination in the last few years. The use of an IL as environmental friendly solvent, offers many advantages over traditional materials synthesis methods. The change from molecular to ionic reaction media leads to new types of materials being accessible. Room-temperature IL have been found to be excellent media for stabilising transition-metal clusters in solution and to crystallise homo- and heteronuclear transition-metal complexes and clusters. Furthermore, the use of IL as solvent provides the option to replace high-temperature routes, such as crystallisation from the melt or gas-phase deposition, by convenient room- or low-temperature syntheses. Inorganic IL composed of alkali metal cations and polynuclear transition-metal cluster anions are also known. Each of these areas will be discussed briefly in this contribution.
Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG-geförderten) Allianz- bzw. Nationallizenz frei zugänglich.

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7

Ibrahim, Masooma [Verfasser]. "Polynuclear Transition Metal-Oxo Complexes Stabilized by Heteropolytungstates / Masooma Ibrahim." Bremen : IRC-Library, Information Resource Center der Jacobs University Bremen, 2012. http://d-nb.info/1035217686/34.

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8

Organtzis, Stefanos. "Polynuclear transition metal complexes containing azido and pyrazolinato bridging ligands." Thesis, University of Manchester, 2008. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.496513.

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Анотація:

Following the discovery that a single molecule can behave as a magnet, the field of research on magnetism has become of great interest to scientists. A large number of polynuclear compounds have been produced and studied worldwide over the past two decades, in an effort to obtain better single molecule magnets (SMMs). The synthesis of such compounds involves mainly first row transition metals and a wide range of bridging ligands.

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9

Taylor, Stephanie Merac. "Calixarene supported transition metal clusters." Thesis, University of Edinburgh, 2013. http://hdl.handle.net/1842/7770.

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This thesis describes a series of calix[n]arene polynuclear transition metal and lanthanide complexes. Calix[4]arenes possess lower-rim polyphenolic pockets that are ideal for the complexation of various transition metal and lanthanide centres. Surprisingly however, with only a few exceptions, the coordination chemistry of p-tBucalix[ 4]arene (TBC[4]), p-tBu-calix[8]arene (TBC[8]) and p-tBuhomotrioxacalix[ 3]arene (TBOC[3]) with paramagnetic transition metal ions for the purpose of making and studying magnetically interesting molecules is unknown. Chapter two describes the reaction of TBC[4] with manganese salts in the presence of an appropriate base (and in some cases co-ligand) resulting in the formation of a family of calixarene-supported [MnIII 2MnII 2] clusters (1-7) that behave as Single-Molecule Magnets (SMMs). These are: [MnIII 2MnII 2(OH)2(TBC[4])2(DMF)6]·2MeOH (1), [MnIII 2MnII 2(OH)2(TBC[4])2(DMF)4(H2O)2]·4MeOH·2DMF (2), [MnIII 2MnII 2(OH)2(TBC[4])2(DMF)6]·2.8MeOH (3), [MnIII 2MnII 2(OH)2(TBC[4])2(DMF)4(EtOH)(H2O)] (4), [MnIII 2MnII 2(OH)2(TBC[4])2(DMSO)6]·2MeOH·2DMSO (5) , [MnIII 2MnII 2(OH)2(TBC[4])2(DMSO)6] (6) and [MnIII 2MnII 2(OH)2(C[4])2(MeOH)6]·4MeOH (7). Variation in the alkyl groups present at the upper-rim of the cone allows for the expression of a degree of control over the self-assembly of these SMM building blocks, whilst retaining the general magnetic properties. The presence of various different ligands around the periphery of the magnetic core has some effect over the extended self-assembly of these SMMs. Chapter three describes how the combination of complementary cluster ligands; sodium phenylphosphinate and the N,O-chelate 2-(hydroxy-methyl)pyridine (hmpH) with TBC[4] results in the formation of two new calixarene-supported clusters. This being an unusual [MnIIIMnII]2 dimer of dimers [MnIIIMnII(O2P(H)Ph)(DMF)2(MeOH)2]2 (8) and a ferromagnetic [Mn5] cage that displays the characteristic bonding modes of each support [MnIII 3MnII 2(OH)2(TBC[4])2(hmp)2(DMF)6](TBC[4]-H)·xDMF ·xH2O (9). Chapter four details how using oxacalix[3]arenes can tune the nature of the metal binding site, by introduction of ≥ 1 ethereal bridge. This results in Mn(II) rather than Mn(III) bonding in the phenolic pocket, and that these components self-assemble with additional Mn(II) and Mn(III) ions to form a [Mn10] supertetrahedron with an unusual oxidation state distribution, [MnII 6MnIII 4O4(TBOC[3])4(Cl)4(DMF)3]∙3.3H2O ∙ 1.5DMF (10). Chapter five introduces a family of lanthanide complexes formed using TBC[8]. Variation in the experimental conditions employed in the reaction of TBC[8] with lanthanide salts (LnX3) provides access to Ln1, Ln2, Ln4, Ln5, Ln6, Ln7 and Ln8 complexes, [Gd(TBC[8]-2H)Cl(DMSO)4]·MeCN·H2O·(DMSO)2·hex (11), [CeIV 4(TBC[8]-6H)2(μ3- O)2(DMF)4]·(DMF)5·hex·MeCN (12), [TbIII 5(TBC[8]-5H)(μ4-O)(μ3- OH)4Cl(DMSO)8(H2O)3]Cl3·(DMSO)2(hex)2 (13), [CeIV 6(TBC[8]-6H)2(μ4-O)2(μ2-OMe)4(μ2- O)2(DMF)4]·(DMF)6·hex (14), [Dy7(TBC[8]-7H)(TBC[8]-6H)(μ4-O)2(μ3-OH)2(μ2- OH)2(DMF)9]·(DMF)3 (15) and [Gd8(TBC[8]-7H)2(μ4-CO3)2(μ5-CO3)2(μ2-HCO2)2(DMF)8] (16), with all polymetallic clusters containing the common bi-nuclear lanthanide fragment. Closer inspection of the structures of the polymetallic clusters reveals that all but one (Ln8) are in fact based on metal octahedra or the building blocks of octahedra.

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10

Hashiguchi, Ryota. "Studies on Polynuclear Metal Complexes and Low-Dimensional Mixed-Valence Halogen-Bridged Transition Metal Complexes Based on them." 京都大学 (Kyoto University), 2017. http://hdl.handle.net/2433/225426.

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11

Chmela, Jiří [Verfasser], and W. M. [Akademischer Betreuer] Klopper. "Theoretical Optical Spectroscopy of Polynuclear Transition Metal and Lanthanoid Complexes / Jiří Chmela ; Betreuer: W. M. Klopper." Karlsruhe : KIT-Bibliothek, 2016. http://d-nb.info/1124902945/34.

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12

Chandra, Anirban. "Synthesis of Bioinspired Dioxygen Reduction Catalysts Involving Mono and Polynuclear Late Transition Metal Complexes and Spectroscopic Trapping of Reactive Intermediates." Doctoral thesis, Humboldt-Universität zu Berlin, 2021. http://dx.doi.org/10.18452/22579.

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Анотація:

Die selektive Funktionalisierung nicht aktivierter C−H-Bindungen und die Disauerstoffreduktionsreaktion (ORR) sind extrem wichtig bei der Beschäftigung mit verschiedenen technologischen Problemstellungen wie der Energiekrise, der Synthese kommerziell relevanter organischer Verbindungen usw. Die Nutzung molekularen Sauerstoffs als reichlich vorhandenes und umweltverträgliches Oxidationsmittel ist von großem Interesse in der Entwicklung bioinspirierter synthetischer Oxidationskatalysatoren. Die katalytische Vier-Elektronen-Reduktion von Disauerstoff zu Wasser erlangte auch immer größere Aufmerksamkeit wegen ihrer Bedeutung in der Brennstoffzellentechnologie. Natürlich vorkommende Metalloenzyme aktivieren Disauerstoff durch die Nutzung günstiger Übergangsmetalle (z.B. Eisen, Nickel, Mangan und Kupfer) und weisen diverse oxidative Reaktivitäten auf. Des Weiteren werden solche Reaktionen unter Umgebungsbedingungen mit hoher Effizienz und Stereoselektivität durchgeführt. Deshalb kann die Isolierung und Charakterisierung hochvalenter Metall-Disauerstoff-Intermediate (wie Metall-Superoxo-, Metall-Peroxo-, Metall-Hydroperoxo- und Metall-Oxo-Verbindungen) eine Menge nützlicher Informationen über die Reaktionsmechanismen liefern und daher hilfreich für die zukünftige Entwicklung effizienterer Katalysatoren sein. Diese Arbeit hat die Chemie verschiedener Metall-Disauerstoff-Intermediate von end-on-1,2-Peroxo-dicobalt(III)-Spezies bis zu Superoxo-nickel(II)-Kernen erforscht. Detaillierte spektroskopische Untersuchungen sowie Reaktivitätsstudien der Intermediate wurden durchgeführt, um den Zusammenhang zwischen ihrer elektronischen Struktur und ihren Reaktivitätsmustern aufzuklären. In meiner Arbeit untersuchte ich den Effekt der ‚Struktur-Aktivität-Beziehung‘ verschiedener Metall-Disauerstoff-Intermediate gegenüber exogener Substrate. Diese Arbeit zeigte auch den Einfluss des Designs geeigneter Liganden auf das Verhalten eines gegebenen reaktiven Metall-Disauerstoff-Systems.
Selective functionalization of unactivated C−H bonds and dioxygen reduction reaction (ORR) are extremely important in the context of addressing various technological issues such as energy-crisis, synthesis of commercially important organic compounds, etc. The utilization of molecular oxygen as an abundant and environmentally benign oxidant is of great interest in the design of bioinspired synthetic oxidation catalysts. The catalytic four-electron reduction of dioxygen to water has also merited increasing attention because of its relevance to fuel cell technology. Naturally occurring metalloenzymes activate dioxygen by employing cheap transition metals (e.g. iron, nickel, manganese, and copper) and exhibit diverse oxidative reactivities. Moreover, such reactions are carried out under ambient conditions with high efficiency and stereospecificity. Therefore, the isolation and characterization of the high-valent metal-dioxygen intermediates (such as metal-superoxo, -peroxo, -hydroperoxo, and -oxo can provide a lot of useful information about the reaction mechanisms and is therefore helpful for the future design of more efficient catalysts. This thesis has explored the chemistry of different metal-dioxygen intermediates ranging from bridging end-on μ-1,2-peroxo-dicobalt(III) species to nickel(II)-superoxo cores. Detailed spectroscopic and reactivity studies of the intermediates have been performed to reveal the correlations between their electronic structures and reactivity patterns. In my present thesis, I investigated the effect of the ‘structure-activity relationship’ of different metal-dioxygen intermediates towards exogenous substrates. This thesis also demonstrated the impact of suitable ligand design on the behaviour of a given metal-dioxygen reactive system.

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13

Diehl, Marcel [Verfasser]. "Polynuclear dioxolene complexes with redox-active transition metals – novel synthesis routes, characterization and capabilities / Marcel Diehl." Mainz : Universitätsbibliothek Mainz, 2016. http://d-nb.info/1105421090/34.

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14

Chandra, Anirban [Verfasser]. "Synthesis of Bioinspired Dioxygen Reduction Catalysts Involving Mono and Polynuclear Late Transition Metal Complexes and Spectroscopic Trapping of Reactive Intermediates / Anirban Chandra." Berlin : Humboldt-Universität zu Berlin, 2021. http://d-nb.info/1230406808/34.

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15

Gourdon, André. "Synthèse et étude structurale de clusters de fer contenant un hétéroatome du type carbure, nitrure, phosphure." Paris 6, 1986. http://www.theses.fr/1986PA066404.

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16

Marzak, Saïd. "Complexes du cuivre (i) construits sur le fragment (ms::(4))**(2-) (m=mo,w) : role du ligand thiocyanate dans l'edification de composes heterometalliques a structure infinie." Paris 6, 1988. http://www.theses.fr/1988PA066401.

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Preparation de complexes du type (nr::(4))::(n)(cu::(4)(ncs)::(4)ms::(4)), m=mo, w, r=me, et et n=2 ou 3. Selon la taille du cation, obtention de macrostructures bidimensionnelles ou tridimensionnelles; l'insertion du cation pph::(4)**(+) conduit a la formation d'une structure infinie de chaines lineaires

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17

Xu, Zhiqiang. "The magnetism and coordination chemistry of mononuclear and polynuclear complexes of copper(II) and other first row transition metal ions derived from open-chain diazine (N-N) ligands." Thesis, National Library of Canada = Bibliothèque nationale du Canada, 1998. http://www.collectionscanada.ca/obj/s4/f2/dsk2/ftp02/NQ36217.pdf.

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18

Clarisse, Jade. "Croissance cristalline de polymères de coordination : synthèse, suivi calorimétrique et caractérisation structurale." Thesis, Lyon 1, 2013. http://www.theses.fr/2013LYO10269/document.

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Les polymères de coordination poreux appelés Metal Organic Frameworks (MOF) sont envisagés pour des développements et applications prometteuses dans la catalyse par exemple. La compréhension des mécanismes de synthèse et leurs croissances cristallines restent cependant un défi. Actuellement, seules quelques études in-situ ont été réalisées pour rationnaliser la synthèse des MOFs, comme des suivis par résonance magnétique nucléaire, par spectroscopie de masse ou par diffraction des rayons X en dispersion d'énergie. Nous proposons, l'analyse thermodifférentielle qui est une technique plus aisée à mettre en oeuvre et permet un suivi calorimétrique en continu pour identifier les phénomènes thermiques régissant la synthèse tels que la réaction de formation et la cristallisation. Grâce à ces analyses thermiques, le domaine réactionnel est déterminé et l'importance des différents paramètres influençant la synthèse sont étudiés, comme la température et les vitesses de chauffage et de refroidissement ainsi que la concentration des réactifs. Ce suivi calorimétrique a été appliqué à la synthèse de nouveaux composés de coordination poreux à base d'un dérivé tetra acide carboxylique de la porphyrine pour en comprendre les étapes réactionnelles importantes. La détermination des structures cristallines montre que certains appartiennent à la classe des Porphyrin Paddle-Wheel Frameworks. De nouvelles approches pour la synthèse de MOFs sont également proposées, en utilisant des ligands organiques acides, imines, oximes et bases de Schiff
Porous coordination polymers so called Metal Organic Frameworks (MOFs) are considered for promising development and applications such as in catalyst. However, the understanding of the synthesis mechanisms and crystal growth is a challenge. Currently, only a few in-situ studies have been done to rationalize the synthesis of MOFs, such as monitoring by nuclear magnetic resonance, mass spectroscopy and energy dispersive X-ray diffraction. In this manuscript the differential scanning calorimetry is proposed as an easier technique to implement that allows a continuous calorimeter tracking to identify the phenomena which govern the synthesis such as the formation reaction and crystallization temperatures. With such thermal analyses, the temperature range of the reaction was determined and the importance of various parameters influencing the synthesis was studied, such as heating temperatures and cooling speeds or reactant concentration. This was applied to the synthesis of new porous coordination compounds based on porphyrin acid derivative in order to understand the important reaction steps. Crystal structure determinations show that some are Porphyrin Paddle-Wheel Frameworks. New approaches to the MOFs synthesis are also proposed using organic ligands like acids, imines, oximes and Schiff bases

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19

Soules, Régis. "Proprietes cooperatives de complexes polymetalliques des ligands squarate et thiosquarate." Toulouse 3, 1987. http://www.theses.fr/1987TOU30178.

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Etude de l'emploi d'un coordinat assembleur qui puisse par coordination avec le centre metallique utilise (metaux de transition du groupe viii) aboutir a un agencement a une dimension des motifs moleculaires par empilement d'entites monomeres ou par formation de chaines. Par utilisation du coordinat squarate sous ses formes oxygenees et soufrees, obtention d'un certain nombre de complexes de pt, pd, ni et cu repondant aux criteres fixes. Etude des structures de ces composes, de leurs proprietes physiques et de la relation structure-propriete. La nature du coordinat comme le caractere specifique de l'arrangement structural ont ete discutes pour une approche de la comprehension de la nature de ces proprietes physiques

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20

Iasco, Olga. "Aimants moléculaires à base de clusters polymétalliques : synthèse, structures cristallines et étude des propriétés magnétiques." Phd thesis, Université Claude Bernard - Lyon I, 2011. http://tel.archives-ouvertes.fr/tel-00838606.

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Les molécules-aimants, ou Single-Molecule Magnets en anglais, sont des complexes polymétalliques qui possèdent la propriété remarquable de se comporter individuellement comme des aimants. Synthétisées selon les méthodes de la chimie de coordination elles sont devenues l'objet d'une intense activité de recherche multidisciplinaire à l'interface de la chimie et de la physique. C'est dans ce contexte que se situe notre travail de thèse qui nous a conduit à synthétiser plusieurs séries de complexes polynucléaires nouveaux puis a les caractériser cristallographiquement et étudier leurs propriétés magnétiques dont les résultats sont présentés dans ce mémoire. Le premier chapitre présente l'approche théorique, expérimentale et les avancées scientifiques principales dans le domaine des molécules-aimants. Le deuxième chapitre concerne quatre séries de composés obtenus avec des ligands de type oxime. Deux de ces composés [Mn3]n et [Mn6] sont des complexes homonucléaires à base de manganèse et les deux autres [Ln2Cu2] et [Ln3Cu8] (LnIII = Dy, Gd, Tb, Y) des complexes hétéronucléaires CuII - LnIII. D'après les études magnétiques nous avons constaté que [Mn3]n, [Dy2Cu2] et [Dy3Cu8] se comportent comme des molécules-aimants mais que [Mn6] ne manifeste pas les propriétés d'une molécule-aimant. Le troisième chapitre concerne un composé tetranucléaire [Mn4] et une série de complexes dodecanucléaires [Ln4Cu8] (LnIII = Dy, Gd, Tb, Y) obtenus avec des ligands de type benzoxazoles. Les études des propriétés magnétiques ont mis en évidence le couplage antiferromagnétique des ions Mn dans le cubane [Mn4]. Pour la série [Ln4Cu8] (LnIII = Dy, Gd, Tb, Y) sur la base du complexe d'yttrium le couplage Cu-Cu a été négligé et pour le complexe [Gd4Cu8] nous avons mis en évidence des interactions Cu-Gd ferromagnétiques et Gd-Gd antiferromagnétiques. Les mesures faites sur le composé [Dy4Cu8] ont mis en évidence le comportement caractéristique d'une molécule-aimant. Le dernier chapitre présente les résultats obtenues pour un complexe tetradécanucléaire à valence mixte MnII - MnIII [Mn14] que nous avons obtenu a partir d'un ligand de type base de Schiff et dans lequel coexistent des interactions antiferromagnétiques et ferromagnétiques entre les ions manganèse avec un zero-field splitting important. La conclusion générale fait le bilan de nos résultats et donne quelques perspectives ouvertes par notre travail.

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21

Saad, Ahmad K. "Mixed polynuclear complexes." Thesis, University of East Anglia, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.235686.

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22

Wilson, L. M. "Electron-transfer properties of polynuclear complexes." Thesis, University of East Anglia, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.374277.

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23

Barthram, Anita Marie. "Metal-metal interactions in polynuclear complexes of ruthenium and osmium." Thesis, University of Bristol, 2000. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.326683.

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24

Beckler, Robert Kendall. "Polynuclear metal complexes as model mixed oxide catalysts." Diss., Georgia Institute of Technology, 1987. http://hdl.handle.net/1853/11897.

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25

Liu, Hongying. "Syntheses, structures, and catalysis of polynuclear metal complexes." Diss., Georgia Institute of Technology, 1989. http://hdl.handle.net/1853/30561.

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26

Graham, A. "Binuclear and polynuclear metal complexes with bulky ligands." Thesis, University of Edinburgh, 2001. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.651687.

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This thesis presents routes to transition metal complexes of pyridonate and carboxylate ligands. Low nuclearity complexes with triphenyl acetate and 1^strow transition metals of the formula [M₄(OMe)₄(O₂CCPh₃)₄(MeOH)₄] (M = Co, Ni or Zn) have been synthesised and mark a change from reactions with other carboxylates which produce linear trinuclear complexes. Molecular modelling studies investigate the close contacts that arise if triphenyl acetate is incorporated into a linear trinuclear compound to establish whether steric interactions are controlling reactivity. High nuclearity complexes with cobalt and nickel have been, made, many of which extend the range of complexes in which the metal atoms form a centred tricapped trigonal prism. These complexes all contain [M₁₀(OH)₆(O₂CCPh₃)₆(xhp)₆]²⁺ (xhp = a pyridone anion substituted at the six position) core with metal atoms capping the triangular faces of the centred prism. A variant on previous trapped trigonal prisms is also presented, in which the cap metal atoms cap the prism edges. In other complexes the metal atoms form new topologies, ranging from hexa- to octanuclear. In some complexes sodium atoms are also incorporated into the polynuclear cages. Reaction conditions for formation of these cages was investigated. Variation of the metal salt from chloride to nitrate influences both the yield of high nuclearity complexes and the timescale over which they are formed. The choice of recrystallisation solvent affects the cage formed. For example. hexanuclear and heterometallic octanuclear cobalt complexes follow identical syntheses except for the recrystallisation solvent. The means by which counterion and recrystallisation solvent influence reactivity is unclear.

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27

Graham, Alasdair. "Dinuclear and polynuclear metal complexes with bulky ligands." Thesis, University of Edinburgh, 2001. http://hdl.handle.net/1842/12051.

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28

Kaur, Gurpreet. "Structure and reactivity of dinuclear and polynuclear metal complexes." Thesis, University of Canterbury. Chemistry, 2014. http://hdl.handle.net/10092/9945.

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This thesis documents the successful syntheses of six novel 2,2':6',2"-terpyridine-amine based polydentate ligands and a range of mono-, di-, and polynuclear complexes derived from them. The ability of some dinuclear complexes to affect the rate of hydrolysis of the phosphate diester group in the DNA model compound, bis-p-nitrophenyl phosphate (BNPP) has also been explored. Owing to the presence of two potential ligating groups in each polydentate ligand, a number of dinuclear, tetranuclear and serendipitous supramolecular architectures have been produced and characterised during this research. The polydentate ligands were synthesised by stepwise functionalisation of the progenitor ligand, 4'-(2"'-toluyl)-2,2':6',2"-terpyridine (L2.1), at its ortho methyl position via free radical bromination, and where various amine groups were appended by nucleophilic substitution reactions. The detailed ligand syntheses, and characterisation are discussed in Chapter 2, along with the crystal structures of some ligands. Chapter 3 describes coordination chemistry of 4'-(2"'-toluyl)-2,2':6',2"-terpyridine with transition metal ions. Thirteen new complexes of Ni(II), Cu(II), Zn(II) and Ag(I) are reported, where Ag(I) produced a striking spiral shaped polymer with L2.1 having unusual „hyperdentate‟ nitrogen atoms. Two polydentate ligands, 4'-[2"'-{(2-pyridylmethyl)aminomethyl}phenyl]-2,2':6',2"-terpyridine, L2.3, and 4'-[2"'-{bis(2-pyridylmethyl)aminomethyl}phenyl]-2,2':6',2"-terpyridine, L2.4, produced six different dinuclear and tetranuclear metal complexes (Chapter 4). The Zn(II) dinuclear complexes were used to study kinetics of hydrolysis of BNPP, and the enhanced rates were reported compared to the analogous mononuclear complexes. The detailed experimental methodology and results are discussed in Chapter 5. The most interesting outcome of this research was formation of the box and wheel shaped complexes, where the ligand L2.3 binds with different metal ions via different coordination modes. The box shaped tetranuclear complexes were synthesised deliberately via structural control over the coordination chemistry of terpyridine-type site of L2.3, where the coordination flexibility of the pendent picolylamine-type site of the ligand was used to bind with other metal ions. The tetranuclear [M¹₂M²₂(L2.3)₄X₂]⁶⁺ box shaped complexes were formed when two divalent M¹ ions bridge between the ligands to produce octahedral bis-terpyridine type complex M¹(L2.3)₂, and then two divalent M² ions link two M¹(L2.3)₂ units together through picolylamine binding sites, where X = Cl⁻, Br⁻, CH₃COO⁻; M¹ = Fe(II), Zn(II), Ni(II); M² = Zn(II), Cu(II). The bis-bidentate bridging ligand terephthalate was also deliberately encapsulated in the middle of Fe₂Zn₂L2.3 box to produce the complex where X₂ = terephthalate. These structures invite speculation that it may be possible to bind and react molecules within these boxes. In a more fortuitous outcome, Ni(II) ions were found to bind to both sites of L2.3 to give, exclusively, an unprecedented decanuclear wheel-shaped structure. A halide ion occupies the central position in the wheel, with Br⁻ being preferred over Cl⁻. The detailed crystal structures, and properties of the wheels shaped Ni₁₀(L2.3)₁₀ complexes are discussed in Chapter 6.

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29

Coxall, Robert Andrew. "Structural studies of some mononuclear and polynuclear metal complexes." Thesis, University of Newcastle Upon Tyne, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.299640.

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30

Barron, Andrew Ross. "Transition metal aluminohydride complexes." Thesis, Imperial College London, 1986. http://hdl.handle.net/10044/1/37935.

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31

Jasim, Naseralla. "Transition metal bifluoride complexes." Thesis, University of York, 2000. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.323538.

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32

Veighy, Clifford Robert. "Novel cyclopentadienyl transition metal complexes." Thesis, University of Southampton, 2001. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.327366.

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33

Zard, P. W. "Transition metal complexes with pyrimidinethiones." Thesis, Imperial College London, 1988. http://hdl.handle.net/10044/1/47322.

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34

Johnson, Donald Martin. "Cyanoscorpionates and Transition Metal Complexes." Digital Commons @ East Tennessee State University, 2010. https://dc.etsu.edu/etd/1725.

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Анотація:

The new dihydrobis(4-cyano-3-tert-butylpyrazolylborate) ligand has been synthesized. Isolated crystals of the thallium complex were collected and structurally characterized by X-ray diffraction. Transition metal complexes of the ligand are currently under investigation.

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35

Marsden, C. "The synthesis and reactivity of di- and polynuclear mixed metal complexes." Thesis, University of Bristol, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.356224.

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36

Choi, Wing-kin Sam. "Synthesis, photophysics and photochemistry of mono- and polynuclear complexes of gold /." Hong Kong : University of Hong Kong, 1995. http://sunzi.lib.hku.hk/hkuto/record.jsp?B17591168.

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37

蔡永健 and Wing-kin Sam Choi. "Synthesis, photophysics and photochemistry of mono- and polynuclear complexes of gold." Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 1995. http://hub.hku.hk/bib/B31234781.

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38

Jayaweera, P. Pradeep M. "Laser spectroscopic and spectroelectrochemical studies of some mono- and polynuclear metal complexes." Thesis, Queen's University Belfast, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.337013.

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39

Little, I. "Synthesis, structures and reactions of polynuclear metal complexes with unsaturated carboxylic acids." Thesis, University of Newcastle Upon Tyne, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.373055.

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40

Holder, Alan John. "Studies on transition metal macrocyclic complexes." Thesis, University of Edinburgh, 1987. http://hdl.handle.net/1842/10961.

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41

Cheung, Wai Man. "Transition metal complexes with dichalcogenoimidodiphosphinate ligands /." View abstract or full-text, 2007. http://library.ust.hk/cgi/db/thesis.pl?CHEM%202007%20CHEUNG.

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42

Redfern, C. M. "Electronic structure of transition metal complexes." Thesis, University of Oxford, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.235094.

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43

Mobbs, B. E. "Arene transition metal complexes in synthesis." Thesis, University of Oxford, 1985. http://ora.ox.ac.uk/objects/uuid:4c7030d4-297e-4af8-a622-d5b4963fc0a3.

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This thesis deals with the applications of organopalladium and organochromium chemistry to the functionalisation of the benzopyran ring system, at a variety of oxidation levels. Section I demonstrates the functionalisation of 3-, 6-, and 8-bromochromones via palladium (0) insertion into the C-Br bond. The resultant arylpalladium species are shown to undergo addition to the least substituted end of a variety of olefins including methyl acrylate, acrylonitrile and styrene. Subsequent palladium-hydride elimination leads to overall palladium catalysed vinylation of the chromone and the synthesis of a number of novel compounds. Vinylation occurs regiospecifically at the site of chromone bromination and is shown to allow clean substituent introduction into each of the three sites. The palladium catalysed reaction of 3,6-dibromo-chromone with methyl acrylate leads to vinylation at both the C3 and C6 positions. Carbonylation of the 6-bromochromone in ethanol or butanol leads to the 6-ethyl or 6-butyl esters respectively. The palladium catalysed vinylation of the 6-bromochromone with ethyl vinyl ether leads to a mixture of products from addition of the chromone to either end of the olefin. With p-bromophenol or p-bromo-N,N-dimethylaniline the reaction gives exclusively the acetylated product arising from addition to the more substituted end of the olefin. This change in orientation is rationalised by considering the polarisation of the olefin and the arylpalladium species. Section II demonstrates the functionalisation of chroman and 4-chromanol via coordination to the Cr(CO)₃ moiety. (η⁶-Chroman)Cr(CO)₃ is synthesised and is shown to undergo regiospecific ring deprotonation at C8 under kinetic conditions or regiospecific benzylic deprotonation at C4 under thermodynamic conditions. The resultant anions are quenched with alkyl halides, aldehydes, Eschenmoser's salt and methyl disulphide resulting in selective functionalisation of either site. No mixed products are observed. The uncomplexed arene is shown to be totally unreactive under identical conditions. (η⁶-4-Chromanol)Cr(CO)₃ is synthesised and is shown to undergo regiospecific C8 ring deprotonation by comparison with authentic samples of the C5 and C8 methylated alcohols. Protection of the hydroxyl group as its methyl, t-butyldimethylsilyl or methoxymethyl ethers is found not to alter the regiochemistry of deprotonation. The 4-chromanol t-butyldimethylsilyl and tri-i-propylsilyl ethers are synthesised and coordinated to the metal unit. Cleavage of the silyl ethers is shown to proceed with loss of stereochemistry, indicating C-0 bond cleavage.

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44

Bridgewater, Brian Michael. "Sterically hindered chiral transition metal complexes." Thesis, Durham University, 1998. http://etheses.dur.ac.uk/5022/.

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This thesis describes the synthesis, characterization and study of a series of organometallic compounds which all contain the same new ligand, l-phenyl-3-methyl-4,5,6,7-tetrahydroindenyl. The ligand forms a chiral complex once coordinated, and is relatively bulky when compared with ligands such as cyclopentadienyl or 4,5,6,7-tetrahydroindenyl.Chapter one of this thesis introduces cyclopentadienyl ligand chirality, cyclopentadienyl metal complex chirality and sterically demanding cyclopentadienyl systems. The synthesis and chemistry of tetrahydroindenes and some applications of chiral cyclopentadienyl metal complexes and their bulky analogues are also reviewed. Chapter two describes modifications to a literature preparation of the tetrahydroindenone precursor of the new tetrahydroindenyl ligand which lead to higher yields. The synthesis of the ligand itself is described, as well as the synthesis of a benzylidene-substituted hexahydroindene, which demonstrates a limitation in the flexibility of the synthetic route chosen. The synthesis, characterization and various properties of the following iron(II) compounds are discussed in chapter two; bis-l-phenyl-3-methyl- 4,5,6,7-tetrahydroindenyl iron (II), 2.3, l-phenyl-3-methyl-4,5,6,7-tetrahydroindenyl iron(II) dicarbonyl dimer, 2.4, and l-phenyl-3-methyl-4,5,6,7-tetrahydroindaiyl methyl dicarbonyl iron(II), 2.5. For all these iron complexes, the solid state molecular structures and the absolute configuration of the chiral ligand were determined using single crystal X-ray d iffraction. For 23 and 2.4, three isomers are possible, two enantiomers that are collectively termed the rac-isomer and a third isomer, the meso- isomer. Cyclic voltammetric studies on 2.3 indicate that it has a reversible one electron oxidation at 0.187 V (with respect to a non-aqueous Ag/AgCl standard electrode). The difference between this and the reversible one electron oxidation for (η-C(_5)H(_5))(_2)Fe (with respect to the same standard) is -0.314 V, therefore 2.3 is shown to be much more easily oxidized than (η-C(_5)H(_5))(_2)Fe. The solution-state infi-a-red spectrum of 2.4 is explained, with reference to a literature analysis of the unsubstituted analogue [CpFe(CO)(_2)](_2). The steric forces present in the various molecular environments are discussed in connection with the degree of phenyl-ring tilt relative to the cyclopentadienyl mean plane and the deviation of the other cyclopentadimyl substituents away from the metal centre. Subsequent reactions of compounds 2.4 and 2.5 are described. Attempts to make linked analogues of the new ligand are summarized in chapter two. In chapter three, two Zr(rV) compounds are prepared, bis (l-phenyl-3-methyl-4,5,6,7-tetrahydroindenyi) zirconium(fV) dichloride, 3.1, and bis (l-phenyl-3-methyl-4,5,6,7-tetrahydroindenyl) dimethyl zirconium(TV), 3.2. Upon crystallization, rac-3.1 spontaneously resolves into crystals containing only one enantiomer. The similarities and differences in the spectroscopic data for the iron(n) compounds of chapter two and the zirconium(IV) compounds of chapter three are discussed and possible explanations offered . The solid state molecular structures of 3.1 and 3.2 were determined by single crystal X-ray diffraction. Experimental details are given in chapter four, whilst the characterizing data are presented in chapter five. Details of the X-ray structure determinations are given in Appendix A.

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45

Wardell, E. M. "EXAFS studies on transition metal complexes." Thesis, University of Manchester, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.377729.

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46

Blunden, Ralph Benedict. "Novel early transition metal cyclopropenyl complexes." Thesis, University of Sussex, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.360552.

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47

Atkins, Andrew J. "Studies on transition metal macrocyclic complexes." Thesis, University of Edinburgh, 1993. http://hdl.handle.net/1842/11664.

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48

Usher, Peter I. "Electrochemical studies of transition metal complexes." Thesis, University of Edinburgh, 1995. http://hdl.handle.net/1842/11492.

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This thesis is concerned with the spectroscopic, electrochemical and spectroelectrochemical investigation of a range of transition metal species, all containing the ligand 2,2'-bipyridine (bpy). All the complexes studied exhibit rich electrochemistry and electronic absorption spectra. Chapter one details the electrochemical and spectroelectrochemical techniques used in this work, and presents a brief overview of the reasons why we study transition metal complexes in this manner. Chapter two is concerned with the solvent dependent behaviour of complexes of the form [M(bpy)₂(CN)₂] (M = Fe, Ru or Os). The electrochemistry, UV/visible spectroscopy and spectroelectrochemistry of these complexes in a range of solvents is described, and both reduced and oxidised forms of the complex are investigated. The solvent dependent characteristics of the complexes are compared with a range of solvent parameters, and show best agreement with Acceptor Numbers. Analysis of epr data for the oxidised complexes, and spectroelectrochemical experiments suggest that the solvent interaction responsible for this behaviour is minimised on removal of an electron. Chapter three details a range of mono- and bi-metallic complexes containing Ru(bpy)₂ or Fe(bpy)₂ units and poly-aromatic bridging ligands. The electrochemistry UV/visible spectroscopy and spectroelectrochemistry of these complexes is described. Chapter four details the attempted synthesis of three complexes utilising cyanide ligands as a bridge between two metal centres. These complexes are based around either a [Ru(bpy)₂(CN)₂] or [Pt(bpy)(CN)₂] centre. The electrochemistry UV/visible spectroscopy and spectroelectrochemistry of the products is reported, and the likely nature of the products is discussed.

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49

Reid, Gillian. "Studies on transition metal macrocyclic complexes." Thesis, University of Edinburgh, 1989. http://hdl.handle.net/1842/12853.

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50

Cooper, Glyn. "Photoelectron spectroscopy of transition metal complexes." Thesis, University of Oxford, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.670392.

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