Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 16, Issue 45, Pages 13429-13434Publisher
WILEY-BLACKWELL
DOI: 10.1002/chem.201002191
Keywords
coordination compounds; intermetallic bonding; main group elements; oligosilanes; silylenes; Mossbauer spectroscopy
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The reaction of the methimazolyl (mt, i.e., 2-mercapto-1-methylimidazolide) substituted silane Si(mt) 4 with SnCl2 and GeCl2 in dioxane affords the paddlewheel-shaped complexes [ClSi(mu-mt)(4)MCl] (M = Sn (1) and Ge (2), respectively). These compounds represent the first crystallographically characterized hexacoordinate silicon complexes comprising a Sn or Ge atom in the Si coordination sphere. An attempt to synthesize the related silicon compound 3 [ClSi(mu-mt)(4)SiCl]instead afforded the trisilane [ClSi(mu-mt)(4)Si-SiCl3] (3a), which provides the first crystallographic evidence for the feasibility of oligosilanes with adjacent hexacoordinate Si atoms. One of the hexacoordinate Si atoms of 3a features the unprecedented (Si2S4) Si skeleton. Natural bonding orbital (NBO) analyses of compounds 1, 2, 3a (and the target compound 3) revealed characteristics of M-II -> Si-IV (for 2 and 3) or M-I -> Si-IV (for 3a) dative bonding in the systems with M = Si and Ge, whereas compound 1 exhibits a covalent Sn-III-Si-III bond.
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