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Methylzinc tetrahydroborate, [MeZnBH₄], has been prepared by two routes and the structure of the solid determined by X-ray crystallography to reveal helical polymers in which MeZn and BH₄ units alternate. The latter functions as a bidentate ligand with respect to each of the adjacent metal atoms. Investigation by mass spectrometry and matrix isolation shows that the vapour consists of an equilibrium mixture of monomeric and dimeric species. The pattern of infrared bands for the monomer is characteristic of a bidentate BH₄ group, a finding consistent with the results of DFT calculations. Disproportionation into [Me₂Zn] and [Zn(BH₄)₂] is a common feature of the chemistry of methylzinc tetrahydroborate, although it has been possible to isolate and characterize the adduct [MeZnBH₄.SMe₂]. The reaction between [B₄H₁₀ and [Me₂Zn] in the gas phase affords colourless acicular crystals of [(MeZn)₂B₃H₇] in yields of ca. 10%. This compound has been characterized by chemical analysis and by NMR and vibrational spectroscopy. X-ray crystallography reveals that the product is a dimer, [(MeZn)₂B₃H₇]₂, featuring two distinct zinc environments. Two B₃H₇ZnNe ligands, formally derived from B₃H₈ by replacement of a µ₂-H by a µ₂-ZnMe unit, each function in a bis(bidentate) manner linking together two other MeZn centres through pairs of Zn-H-B bridges. The structures of several aluminium tetrahydroborates in the solid phase have been investigated by X-ray diffraction. The structure of dimethylaluminum tetrahydroborate has been shown to consist of helical polymeric chains in which Me₂-Al and BH₄ units alternate. Here, too, the BH₄ groups exhibit bidentate ligation with respect to each of the adjacent metal atoms, although the degree of interaction between the metal centre and the BH₄ group is somewhat less than in [MeZnBH₄ ]. Solid aluminium tris(tetrahydroborate) exhibits two phases with a transition temperature in the range 180-195 K. Each phase is made up of discrete Al(BH ₄ )₃ units, the principal differences relating to the packing of the individual molecules. In the a phase the Al(BH ₄ )₃ molecules display an angle of 78.2° between the AlB₃ and Al(µ-H)₂ planes and are disposed about a 2₁ crystallographic screw axis; in the ß phase the molecular units conform to D_3h symmetry. Dimethylindium octahydrotriborate, [Me₂ lnB₃ H₈ ], has been synthesized by the reaction between trimethylindium and tetraborane(10) and characterized by chemical analysis and by NMR and vibrational spectroscopy. X-ray diffraction of a single crystal reveals that the solid consists of [Me₂ lnB₃ H₈] units, although there is evidence of charge separation in the sense [Me₂ln]⁺[B₃ H₈ ]^- and of secondary interaction between terminal hydrogen atoms and adjacent indium centres. The infrared spectrum of the matrix-isolated vapour is consistent with a monomeric structure similar to that of [Me₂ AlB₃ H₈].

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Thesis (Ph. D.)--University of Adelaide, Dept. of Chemical Engineering, 1999. / Includes bibliographical references (leaves 322-335).

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Thesis (Ph. D.)--University of Texas at Austin, 2002. / Vita. Includes bibliographical references. Available also from UMI Company.

Thesis (Ph. D.)--Oregon Graduate Institute, 2000.