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Two new bidentate thioether ligands, the dialkylbis[(alkylthio)methyl]silanes Ph[subscript]2Si(CH[subscript]2SMe)[subscript]2 and Me[subscript]2Si(CH[subscript]2SBu[superscript]t)[subscript]2, have been synthesized and fully characterized. Reactivity studies led to the isolation of group 11 and 12 metal halide complexes, all of which have d[superscript]10 electronic configurations. The full characterization of these complexes, including NMR spectroscopy and elemental analysis, will be described in this thesis. Reactivity studies of R'[subscript]2Si(CH[subscript]2SR)[subscript]2 (R' = Ph, Me; R = Me, Bu[superscript]t) towards monovalent coinage metal ions have produced simple 1:1 and 1:2 complexes {R'[subscript]2Si(CH[subscript]2SR)[subscript]2}CuX (X = C1, Br, I), {R'[subscript]2Si(CH[subscript]2SR)[subscript]2}AgX (X = NO[subscript]3, OTf) and [Ag{R'[subscript]2Si(CH[subscript]2SR)[subscript]2}[subscript]2]X (X = BF[subscript]4, SbF[subscript]). With Ph[subscript]2Si(CH[subscript]2SMe)[subscript]2, the majority of these 1:1 complexes showed dimeric structures, similar in most cases to the Me[subscript]2Si(CH[subscript]2SMe)[subscript]2 analogues. It was concluded that changing substituents on silicon did not affect considerably the geometry of the complexes. However, the bulky substituents on the thioether Me[subscript]2Si(CH[subscript]2SBu[superscript]t)[subscript]2 preclude the generation of polymeric (or dimeric) 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 some of the first complexes exhibiting [CuS[subscript]2X] coordination spheres. In a similar vein, the dinuclear gold complexes Au[subscript]2{Me[subscript]2Si(CH[subscript]2SBu[superscript]t)[subscript]2}X[subscript]2 (X = C1, Br), each of which displays a weak intramolecular Au...Au aurophilic interaction and photoluminescent properties, 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 spectrometry (ESIMS). An overview of the coordination chemistry of R'[subscript]2Si(CH[subscript]2SR)[subscript]2 towards other transition metal ions such as Cd(II) and Hg(II) will be also discussed.
ABSTRACT: The new acyclic tetradentate thioether ligand tetrakis[(methylthio)methyl]silane, has been synthesized with the goal of studying its coordination chemistry and comparing it with that of the recently prepared methyltris[(methylthio)methyl]silane, and other tridentate or tetradentate thioethers. This new tetradentate ligand was coordinated to the group 6 transition metals to give a complete series of thioether carbonyl complexes, where the sulfur ligand is bound to the metal center in either a bidentate or tridentate fashion. The dinuclear compounds were obtained from the reaction of LM(CO)4 and [Cu(NCMe)4]X (X = BF4 or PF6) in a 2:1 ratio, with the thioether serving as a bridging ligand between the two metals. Furthermore, six and seven-coordinated dihalo thioether complexes have also been prepared and structurally characterized.
ABSTRACT: The new thioethers MeSi and Si have been synthesized with the goal of investigating the effect of the tert-butyl substituents on their structure and coordination chemistry. These tridentate or tetradentate ligands are new members of existing families of acyclic thioethers. Reactivity studies of these newly synthesized ligands were performed by coordinating them to group 6 metal carbonyl derivatives. These complexes have been compared with the group 6 metal complexes of other thioether ligands to determine the electronic and steric differences that the tert-butyl group may cause. Spectroscopic and X-ray diffraction studies were performed to determine those effects.
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