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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Variable coordination geometries via an amine-tethered-enamidophosphinimine ligand on cobalt
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Variable coordination geometries via an amine-tethered-enamidophosphinimine ligand on cobalt

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The synthesis of two new amine-tethered enamidophosphinimine donor sets is described and their coordination chemistry with cobalt(II) detailed. Deprotonation of the enamine tautomers of each system generates the lithium derivatives that are used in metathesis reactions with either anhydrous CoCl2 or CoCl2(THF)(1.5) to generate tetrahedral kappa(3)-(NNpNR) CoCl (where R = DIPP, 2,6-diisopropylphenyl; R = TMS, trimethylsilyl) or tetrahedral kappa(2)-(NNpNTMS)(2)Co, the latter likely due to the insolubility of the CoCl2. For the R = DIPP derivative, replacement of the chloride proceeds smoothly by methathesis with LiCH2SiMe3 and KBEt3H to generate the bulky alkyl derivative kappa(3)-(NNpNDIPP) CoCH2SiMe3, and the dihydride-bridged dimer kappa(2)-(NNpNDIPP) Co(2)(mu-H)(2), respectively; interestingly, the hydride dimer has the diethylaminoethyl arms uncoordinated. Reduction of kappa(3)-(NNpNDIPP) CoCl with KC8 under dinitrogen generates the p-arene complex, kappa(2):eta(6)-(NNpNDIPP) Co, and not the expected N-2 complex. In an attempt to generate a dinitrogen complex, we investigated the metathesis and reduction chemistry of the N-trimethylsilyl substituted phosphinimine cobalt derivative, kappa(3)-(NNpNTMS) CoCl. Although reaction with LiCH2SiMe3 produced the anticipated tetrahedral Co(II) alkyl complex kappa(3)-(NNpNTMS) Co(CH2SiMe3), reaction with KBEt3H and KC8 did not give the analogous products to that of the DIPP derivative; instead, the reaction with hydride was complicated and the only product isolated was the bis(ligand) derivative, kappa(2)-(NNpNTMS)(2)Co, while reaction with KC8 under N-2 generated the C-H activated complex kappa(4)-(NNpNSiMe2CH2) Co. Many of these complexes have been characterized by single-crystal X-ray analysis, elemental analysis and solution magnetic susceptibility measurements. In addition, a number of these derivatives were screened for their ability to act as catalyst precursors for the hydrosilylation of 1-hexene.

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