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Accessing Valuable Ligand Supports for Transition Metals: A Modified, Intermediate Scale Preparation of 1,2,3,4,5-Pentamethylcyclopentadiene
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Lanthanoid-transition-metal bonding in bismetallocenes.

Mikhail V Butovskii1, Benjamin Oelkers, Tobias Bauer

  • 1Lehrstuhl Anorganische Chemie II, Universität Bayreuth, Universitätsstrasse 30, 95440 Bayreuth (Germany), Fax: (+49) 921-55-2157.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|February 7, 2014
PubMed
Summary

New bismetallocene compounds were synthesized using salt metathesis and alkane elimination methods. Salt metathesis offers an attractive alternative, especially when steric hindrance affects reaction rates in lanthanide chemistry.

Keywords:
lanthanummetal-metal interactionsmetallocenesrare earthstransition metals

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Area of Science:

  • Organometallic Chemistry
  • Lanthanide Chemistry
  • Coordination Chemistry

Background:

  • Bismetallocenes featuring lanthanide (Ln) and transition metal (TM) centers are of interest for their unique bonding and electronic properties.
  • Understanding the synthetic pathways and factors influencing their formation is crucial for developing new catalytic and materials applications.

Purpose of the Study:

  • To synthesize and characterize novel bismetallocene complexes, specifically [Cp2LuReCp2] and [Cp*2LaReCp2].
  • To compare the efficacy of salt metathesis and alkane elimination as synthetic strategies for these compounds.
  • To investigate the nature and strength of covalent bonding interactions between the Ln and TM centers and their dependence on synthetic conditions and ligand environment.

Main Methods:

  • Synthesis of bismetallocenes via salt metathesis in aromatic hydrocarbons and alkane elimination.
  • Characterization of the synthesized compounds.
  • Quantification of covalent bonding interactions using the delocalization index.
  • Computational modeling to understand the influence of Lewis acidity and coordination on bonding.

Main Results:

  • Successful synthesis of [Cp2LuReCp2] and [Cp*2LaReCp2] bismetallocenes.
  • Salt metathesis identified as a viable and often superior alternative to alkane elimination, particularly when steric hindrance is a factor.
  • Reaction rates in alkane elimination are sensitive to the ionic radius of the lanthanide ion.
  • Covalent bonding between Ln and TM cations was quantified, falling within the range typical for transition metal bonds.
  • Secondary interactions between the transition metal's Cp ligand and the Ln cation were observed and found to depend on the electron-donating ability of the TM atom.
  • Coordination of THF to the Lu atom significantly influences Lu-Ru and Lu-C bonding, indicating tunable Lewis acidity at the lanthanide center.

Conclusions:

  • Salt metathesis provides a robust synthetic route for bismetallocenes, overcoming limitations associated with alkane elimination, especially concerning steric hindrance.
  • The electronic structure and bonding in these bismetallocenes are influenced by the interplay between the lanthanide and transition metal centers, as well as ligand effects.
  • Tunable Lewis acidity at the lanthanide site offers a pathway to control the structural and bonding characteristics of these organometallic compounds.