Abstract
Hydrogenation of bis(trimethylsilylmethyl) zirconium complex [Zr(Me2TACD)(CH2SiMe3)2] (1), prepared by reacting [Zr(CH2SiMe3)4] with 1,7-dimethyl-1,4,7,10-tetraazacyclododecane (Me2TACD)H2, gave dinuclear alkyl hydride complex [Zr(Me2TACD)(CH2SiMe3)2(μ-H)2Zr(Me2TACD)] (2). According to NMR spectroscopic and single-crystal X-ray diffraction studies, 2 exhibits a Cs-symmetrical structure with two distinct zirconium centers, one eight- and the other seven-coordinate, bridged by an amido donor and two hydrides. Abstraction of the trimethylsilylmethyl groups by the weak Bronsted acid [NEt3H][B(3,5-C6H3Cl2)4] gave the monocationic mono(alkyl) dihydride [Zr(Me2TACD)(CH2SiMe3)(μ-H)2Zr(Me2TACD)][B(3,5-C6H3Cl2)4] (3) and the dicationic hydride complex [Zr(Me2TACD)(THF)2(μ-H)2Zr(Me2TACD)][B(3,5-C6H3Cl2)4]2 (4). X-ray crystallography of the cationic complexes 3 and 4 revealed a Cs-symmetrical dinuclear structure derived from that of 2.
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