Bulletin of the Korean Chemical Society

Korean Chemical Society (대한화학회)
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A Novel Al-Bridged Trinuclear Iron(II) Bis(imino)pyridyl Complex with Catalytic Ethylene Polymerization Behavior

  • Long, Zerong (Xinjiang Uygur Autonomous Region Product Quality Supervision and Inspection Institute) ;
  • Li, Zhongquan (Tarim Oilfield) ;
  • Ma, Ning (State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou institute of Chemical Physics, Chinese Academy of Sciences) ;
  • Wu, Biao (State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou institute of Chemical Physics, Chinese Academy of Sciences)
  • Received : 2011.06.08
  • Accepted : 2011.06.10
  • Published : 2011.08.20
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Abstract

A self-assembled Al-bridged diiminopyridine-based ligand (3) was synthesized and characterized by FT-IR, ESI-MS and NMR spectroscopy. Electron spectral titrations were performed to confirm the formation of a novel trinuclear bis(imino)pyridyl iron(II) complex (4) upon addition of $FeCl_2$ into Al-bridged ligand 3 in methanol solution. Simultaneously, a typical bis(imino)pyridine-iron(II) complex (2) was synthesized and fully characterized. The X-ray crystal study of the iron(II) complex 2 disclosed a five-coordinate, distorted square-pyramidal structure with the tridentate N^N^N ligand and chlorides. The optimal molecular structure of 4 was obtained by means of molecular mechanics, which showed that each iron atom in the complex 4 is surrounded by two chlorides, a tridentate N^N^N ligand and one oxygen atom, supporting considerations about the possibility of six-coordinate geometry from MMAO or the ethylene access. A comparison of 4 with the reference 2 revealed a remarkable decrease of the catalytic activity and MMAO consumption (activity up to $0.41{\times}10^3\;kg\;{mol_{Fe}}^{-1}h^{-1}bar^{-1}$, Al/Fe = 650 for 4 and $7.02{\times}10^3\;kg\;{mol_{Fe}}^{-1}h^{-1}bar^{-1}$, Al/Fe = 1600 for 2).

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References

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