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Group iv complexes containing the benzotriazole phenoxide ligand as catalysts for the ring-opening polymerization of lactides, epoxides and as precatalysts for the polymerization of ethylene
Sreenath Pappuru, Eswara Rao Chokkapu, Debashis Chakraborty, Venkatachalam Ramkumar
Published in
2013
PMID: 24071827
Volume: 42
   
Issue: 46
Pages: 16412 - 16427
Abstract
A series of Ti(iv), Zr(iv) and Hf(iv) benzotriazole phenoxide (BTP) complexes were synthesized and characterized by various spectroscopic techniques, elemental analysis and X-ray crystallography. The monosubstituted Zr(iv) BTP complexes [(μ-L)Zr(OiPr)3]21-3 [L = C1BTP-H (1), TClBTP-H (2), pentBTP-H (3)] and tetrasubstituted Zr(iv), Hf(iv) complexes ZrL44-6 [L = C1BTP-H (4), TClBTP-H (5), pentBTP-H (6)] and HfL47-9 [L = C1BTP-H (7), TClBTP-H (8), pentBTP-H (9)] were prepared by the reaction of Zr(O iPr)4·(iPrOH) and Hf(O tBu)4 in toluene with the respective ligands in different stoichiometric proportions. The reaction between BTP and TiCl4 and ZrCl4 and HfCl4 in a 2:1 stoichiometric reaction resulted in the formation of disubstituted group IV chloride complexes L 2MCl210-12 [L = C1BTP-H, M = Ti, Zr and Hf]. The molecular structures of complexes 1, 4, 7, 10, 11, and 12 were determined by single-crystal X-ray studies. The X-ray structure of 1 reveals a dimeric Zr(iv) complex containing a Zr2O2 core bridged through the oxygen atoms of the phenoxide groups. Each Zr atom is distorted from an octahedral symmetry. These complexes were found to be active towards the ring-opening polymerization (ROP) of l-lactide (l-LA) and rac-lactide (rac-LA). Complex 1 produced highly heterotactic poly(lactic acid) (PLA) from rac-LA under melt conditions with narrow molecular weight distributions (MWDs) and well controlled number average molecular weights (Mn). Additionally, epoxide polymerizations using rac-cyclohexene oxide (CHO), rac-propylene oxide (PO), and rac-styrene oxide (SO) were also carried out with these complexes. The yield and molecular weight of the polymer was found to increase with the extension of reaction time. Compounds 1-12 were activated by methylaluminoxane (MAO) and show good activity for ethylene polymerization and produced high molecular weight polyethylene. © 2013 The Royal Society of Chemistry.
About the journal
JournalDalton Transactions
ISSN14779226
Open AccessNo
Concepts (53)
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    Chloride complexes
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    Ethylene polymerization
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    HIGH MOLECULAR WEIGHT POLYETHYLENES
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    NARROW MOLECULAR WEIGHT DISTRIBUTIONS
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    NUMBER AVERAGE MOLECULAR WEIGHT
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    OCTAHEDRAL SYMMETRY
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    Spectroscopic technique
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    Stoichiometric reaction
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    Chlorine compounds
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    Crystal atomic structure
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    Epoxy resins
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    Ethylene
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    Hafnium
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    Hafnium compounds
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    Ligands
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    Molecular weight distribution
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    Propylene
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    Ring opening polymerization
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    Styrene
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    Synthesis (chemical)
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    Titanium
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    X ray crystallography
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    X rays
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    Zirconium
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    Zirconium compounds
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    Benzotriazole
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    Coordination compound
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    DILACTIDE
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    Dioxane derivative
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    Epoxide
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    Ethylene derivative
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    Ligand
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    Metal
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    Phosphonic acid derivative
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    PHOSPHOROUS ACID
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    Triazole derivative
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    Article
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    Catalysis
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    Chemistry
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    Conformation
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    Magnetism
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    Polymerization
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    Synthesis
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    Coordination complexes
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    Crystallography, x-ray
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    Dioxanes
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    Epoxy compounds
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    Ethylenes
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    Magnetics
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    Metals
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    Molecular conformation
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    PHOSPHOROUS ACIDS
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    Triazoles