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The tetradentate thioether Si(CH[subscript]2SBu[superscript]t)[subscript]4 was used to synthesize the complete series of copper(I) complexes Cu[subscript]2Si(CH[subscript]2SBu[superscript]t)[subscript]4X[subscript]2 (X = C1, Br, I). Interestingly, a single X-ray diffraction study of the chloro derivative revealed the presence of both four-coordinate tetrahedral and three-coordinate trigonal planar copper centers. The adamantyl-substituted dithioether Me[subscript]2Si(CH[subscript]2SAd)[subscript]2 has been readily synthesized and it is the first member of the Me[subscript]2Si(CH[subscript]2SR)[subscript]2 (R = alkyl, aryl) family of ligands to be structurally characterized. Reactivity studies towards monovalent coinage metal ions have produced simple 1:1 and 1:2 complexes {Me[subscript]2Si(CH[subscript]2SAd)[subscript]2}CuX (X = C1, Br, I), and [Cu{Me[subscript]2Si(CH[subscript]2SAd)[subscript]2}[subscript]2]PF[subscript]6. Significantly, the bulky substituents on the thioether preclude the generation of polymeric species such as those isolated for R = Me and result instead in the formation of rare examples of three-coordinate trigonal planar Cu(I) thioether complexes. Furthermore, these are the first such complexes exhibiting [CuS[subscript]2X] coordination spheres. In a similar vein, the dinuclear gold complexes Au[subscript]2{Me[subscript]2Si(CH[subscript]2SAd)[subscript]2}X[subscript]2 (X = C1, Br), each of which displays a fairly strong intramolecular Au...Au aurophilic interaction, are obtained instead of the polymeric species isolated for closely related but less sterically demanding thioether ligands [e.g., Me[subscript]2Si(CH[subscript]2SMe)[subscript]2]. The new complexes have been characterized by a variety of analytical and spectroscopic techniques, including electrospray ionization mass spectroscopy (ESIMS). An overview of the coordination chemistry of Me[subscript]2Si(CH[subscript]2SAd)[subscript]2 towards other transition metal ions such as Ag(I), Cd(II) and Hg(II) will be also discussed.
Covers the vastly expanding subject of oxidative processes mediated by copper ions within biological systems Copper-mediated biological oxidations offer a broad range of fundamentally important and potentially practical chemical processes that cross many chemical and pharmaceutical disciplines. This newest volume in the Wiley Series on Reactive Intermediates in Chemistry and Biology is divided into three logical areas within the topic of copper/oxygen chemistry— biological systems, theory, and bioinorganic models and applications—to explore the biosphere for its highly evolved and thus efficient oxidative transformations in the discovery of new types of interactions between molecular oxygen and copper ion. Featuring a diverse collection of subject matter unified in one complete and comprehensive resource, Copper-Oxygen Chemistry probes the fundamental aspects of copper coordination chemistry, synthetic organic chemistry, and biological chemistry to reveal both the biological and chemical aspects driving the current exciting research efforts behind copper-oxygen chemistry. In addition, Copper-Oxygen Chemistry: Addresses the significantly increasing literature on oxygen-atom insertion and carbon-carbon bond-forming reactions as well as enantioselective oxidation chemistries Progresses from biological systems to spectroscopy and theory, and onward to bioinorganic models and applications Covers a wide array of reaction types such as insertion and dehydrogenation reactions that utilize the cheap, abundant, and energy-containing O2 molecule With thorough coverage by prominent authors and researchers shaping innovations in this growing field, this valuable reference is essential reading for bioinorganic chemists, as well as organic, synthetic, and pharmaceutical chemists in academia and industry.
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This thesis addresses the coordination chemistry and reactivity of copper and gold complexes with a focus on the elucidation of (i) the metal-mediated activation of σ-bonds and (ii) the migratory insertion reaction. Both processes are of considerable importance in organometallic chemistry, but remain elusive for Cu and Au complexes. In this work, the author contributes significant advances: The first σ-SiH complexes of copper are experimentally and computationally characterized, yielding valuable insights into σ-bond activation processes for copper. Evidence for a highly unusual migratory syn insertion of unsaturated organic molecules into the gold-silicon bond of silylgold (I) complexes is provided and the corresponding mechanism identified. The intermolecular oxidative addition of σ-SiSi, σ-CC and σ-CX (X=halogen) bonds with molecular gold (I) complexes is studied in detail, effectively demonstrating that this reaction, usually considered to be impossible for gold, is actually highly favored, provided an adequate ligand is employed. The use of small-bite angle bis (phosphine) gold (I) complexes allows for the first time the oxidative addition of σ-CC and σ-CX bonds for gold (I). These results shed light on an unexpected reactivity pattern of gold complexes and may point the way to 2-electron redox transformations mediated by this metal, opening up new perspectives in gold catalysis.
Comprehensive Coordination Chemistry II (CCC II) is the sequel to what has become a classic in the field, Comprehensive Coordination Chemistry, published in 1987. CCC II builds on the first and surveys new developments authoritatively in over 200 newly comissioned chapters, with an emphasis on current trends in biology, materials science and other areas of contemporary scientific interest.
Homogeneous catalysis is the success story of organometallic chemistry. Since the discovery of hydroformylation by O. Roelen in 1938, catalytic applications have paved the way of organometallic compounds in industry. Bulk and fine chemicals, and even natural products are being produced via homogeneous organometallic catalysis. The enormous breadth of this topic in view of both basic research and industrial application is met in this three volume handbook edited jointly by W. A. Herrmann and B. Cornils. The list of contributors reads like a who-is-who in organometallic chemistry and homogeneous catalysis. In this handbook, experts will find the current state-of-the-art in their field and advanced students will benefit from the concise treatment of important catalytic reactions and processes. With its balanced presentation of the truly interdisciplinary topic and its outstanding editor- and authorship, the 'Cornils/Herrmann' is beyond common standards. Now in its second, completely revised and enlarged edition!