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Dimitra Theodosopoulou1, Miguel Alonso De La Pena1, Sary Abou Derhamine1

  • 1Univ Rennes, CNRS, Institut des Sciences Chimiques de Rennes (ISCR), UMR 6226, F-35042 Rennes, France. jean-francois.carpentier@univ-rennes.fr.

Dalton Transactions (Cambridge, England : 2003)
|June 7, 2023
PubMed
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New ansa-metallocene complexes with diverse substitutions were synthesized. These catalysts demonstrate high activity and selectivity for producing highly isotactic polypropylene (iPP) via propylene polymerization.

Area of Science:

  • Organometallic Chemistry
  • Polymer Science
  • Catalysis

Background:

  • Development of efficient catalysts for olefin polymerization is crucial for producing advanced polyolefins.
  • Ansa-metallocene complexes, particularly those based on group 4 metals, are well-established catalysts for producing stereoregular polyolefins.

Purpose of the Study:

  • To synthesize and characterize novel C1-symmetric group 4 ansa-metallocene complexes featuring Me2Si-bridged cyclopentadiene/indene proligands with diverse substitutions.
  • To evaluate the catalytic performance of these complexes in propylene polymerization.
  • To elucidate the polymerization mechanism using DFT calculations.

Main Methods:

  • Synthesis of Me2Si-bridged cyclopentadiene/indene proligands and their corresponding ansa-metallocene complexes.

Related Experiment Videos

  • Characterization using NMR spectroscopy, mass spectrometry, and X-ray crystallography.
  • Propylene polymerization studies using activated metallocene complexes (with MAO) in solution and supported systems (on SiO2-MAO).
  • Density Functional Theory (DFT) calculations for mechanistic studies.

    • Main Results:

    • A series of novel ansa-metallocene complexes were successfully synthesized and characterized.
    • The zirconocene complexes exhibited high catalytic activity in propylene polymerization, reaching up to 161,000 kg(PP) mol(Zr)-1 h-1 in solution and 636,000 kg(PP) mol(Zr)-1 h-1 in slurry bulk.
    • The catalysts produced highly isotactic polypropylenes (iPP) with high stereoregularity ([m]4 up to 96.5%) and high melting temperatures (Tm up to 157 °C).

    Conclusions:

    • The designed ansa-metallocene complexes are highly effective catalysts for producing isotactic polypropylene.
    • Catalyst performance can be tuned through structural modifications of the ligands.
    • DFT calculations support a 'chain-stationary' enchainment mechanism with a preference for 1,2-insertions.