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"A cobalt analogue of Cp*Co(PMe3)Me(OTf) (Cp* = 1, 2, 3, 4, 5 - pentamethylcyclopenta-dienyl, OTf = OSO2CF3), in Chapter 2, was attempted to be synthesized and studied for electrophilic C-H bond activation. Three new cobalt complexes Cp*Co(PMe3)(Me)2, Cp*Co(PMe3)(OTf)2 and Cp*Co(PMe3)(Me)(I) were synthesized. The 1H NMR spectrum showed a new material formed after mixing Cp*Co(PMe3)(Me)2 and Cp*Co(PMe3)(OTf)2 in 1:1 ratio. In Chapter 3, five carboxylate ligated iridium complexes (dmPhebox)Ir(O2CR)2(H2O) (R = -CH3(known compound), -CH2CH3, -CMe3, - CH2C6H5, -CH=CMe2) were designed and synthesized to understand the carboxylate ligand effects on the reactivity of the complex for alkane dehydrogenation. Results from the kinetic study showed that different R groups of the carboxylate iridium complexes can affect the reactivity with octane in the ??H elimination step. The rate constants for octane formation with different carboxylate ligands follow the order R = -CH=CMe2 > -CMe3 > -CH2CH3 > -CH3 > -CH2C6H5. In contrast, there is no significant effect of carboxylate ligand on the rate of the C-H activation step at 160 ʻC. These experimental results support the findings in the previously reported density functional theory (DFT) study of the (dmPhebox)Ir complex in alkane C-H activation. In Chapter 4,5 and 6, hydrogen transformation during the dehydrogenation and hydrogenation of N-heterocycles with a cobalt pincer catalyst, hydrogenation of alkenes with Fe(II) precursors, and hydrogenation of alcohols and dehydrogenation of ketones with a Cp*Rh(III) catalyst were investigated. The results of the acceptorless, reversible dehydrogenation and hydrogenation of N-heterocycles suggests a bifunctional dehydrogenation pathway and a non-bifunctional hydrogenation mechanism. The iron catalysts described in Chapter 5 operate via a metal-ligand cooperative pathway via a stepwise hydride transfer and then proton transfer mechanism. The Cp*Rh(III) catalysts in Chapter 6 decompose upon heating to give nanoparticles."--Pages xi-xii.
Straight from the frontier of scientific investigation . . . PROGRESS in Inorganic Chemistry Nowhere is creative scientific talent busier than in the world of inorganic chemistry. And the respected Progress in Inorganic Chemistry series has long served as an exciting showcase for new research in this area. With contributions from internationally renowned chemists, this latest volume reports the most recent advances in the field, providing a fascinating window on the emerging state of the science. "This series is distinguished not only by its scope and breadth, but also by the depth and quality of the reviews." --Journal of the American Chemical Society. "[This series] has won a deservedly honored place on the bookshelf of the chemist attempting to keep afloat in the torrent of original papers on inorganic chemistry." --Chemistry in Britain. CONTENTS OF VOLUME 47 Terminal Chalcogenido Complexes of the Transition Metals (Gerard Parkin, Columbia University) * Coordination Chemistry of Azacryptands (Jane Nelson, Vickie McKee, and Grace Morgan, The Queen's University, Northern Ireland) * Polyoxometallate Complexes in Organic Oxidation Chemistry (Ronny Neumann, Hebrew University of Jerusalem, Israel) * Metal-Phosphonate Chemistry (Abraham Clearfield, Texas A&M University) * Oxidation of Hydrazine in Aqueous Solution (David M. Stanbury, Auburn University) * Metal Ion Reconstituted Hybrid Hemoglobins (B. Venkatesh, J. M. Rifkind, and P. T. Manoharan, Sophisticated Instrumentation Centre, IIT, Madras, India) * Three-Coordinate Complexes of "Hard" Ligands: Advances in Synthesis, Structure, and Reactivity (Christopher C. Cummins, Massachusetts Institute of Technology) * Metal-Carbohydrate Complexes in Solution (Jean-Francois Verchere and Stella Chapelle, Universite de Rouen, France; Feibo Xin and Debbie C. Crans, Colorado State University).
Transition metals and their complexes have an important impact on chemistry and are found in many application in life in general. Ruthenium and rhodium are two members of noble metals and proved to be suitable for anticancer activity. With the aim of changing the coordination environment in ruthenium and rhodium complexes, this thesis presents a series of Ru(II) polypyridyl and Rh(III) pincer-type complexes. All new Ru(II) and Rh(III) complexes were characterized by NMR spectroscopy, ESI-MS spectrometry and UV-Vis spectrophotometry . For some of the complexes a single crystal X-ray crystallography was performed. The substitution reactions of Ru(II) and Rh(III) complexes with mononucleotides, oligonucleotides and amino acids were studied quantitatively by UV-Vis spectroscopy. Measurements of the activation enthalpies and entropies for all synthesized complexes are supporting an associative mechanism for the substitution process. NMR spectroscopy studies were performed on some Ru(II) complexes where after the hydrolyses of the metal-Cl bond the complexes are capable to interact with guanine derivatives forming monofunctional adducts via N7 atom. The interactions of Ru(II) and Rh(III) complexes with fully complementary 15-mer and 22-mer duplexes of DNA and fully complementary 13-mer duplexes of RNA were studied by UV-Vis spectroscopy. The interactions of ruthenium(II) and rhodium(III) complexes with calf thymus and herring testes DNA were examined by absorption using UV-Vis spectroscopy, fluorescence emission spectral studies by ethidium bromide displacement studies and viscosity measurements. ; eng