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Reductive coupling of carbon monoxide by U(III) complexes--a computational study.

Georgina Aitken1, Nilay Hazari, Alistair S P Frey

  • 1Department of Chemistry, Oxford University, Inorganic Chemistry Laboratory, South Parks Road, Oxford, UK OX1 3QR.

Dalton Transactions (Cambridge, England : 2003)
|August 16, 2011
PubMed
Summary

Uranium complexes catalyze the reductive oligomerization of carbon monoxide (CO), forming yne diolate, deltate, and squarate structures. Density functional methods reveal spin density transfer from uranium to CO, crucial for these transformations.

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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes
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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes

Published on: April 10, 2015

Area of Science:

  • Organometallic Chemistry
  • Computational Chemistry
  • Uranium Chemistry

Background:

  • Uranium complexes are explored for their catalytic potential in small molecule activation.
  • Reductive oligomerization of carbon monoxide (CO) is a challenging chemical transformation.
  • Understanding the electronic structure of uranium organometallics is key to designing catalysts.

Purpose of the Study:

  • To model the reductive oligomerization of CO using uranium complexes.
  • To investigate the electronic interactions between uranium and CO during catalysis.
  • To propose reaction pathways for the formation of cyclic CO oligomers.

Main Methods:

  • Density functional theory (DFT) calculations were employed.
  • Orbital structure analysis of uranium complexes was performed.
  • Reaction mechanisms and intermediate structures were optimized.

Main Results:

  • CO binding to uranium induces spin density transfer to the CO ligand via U5f back-bonding.
  • A proposed pathway leads to the formation of yne diolate complexes through CO dimerization.
  • Optimized structures of yne diolate, deltate, and squarate complexes model experimental findings.

Conclusions:

  • Uranium complexes can facilitate the reductive oligomerization of CO.
  • Electronic structure calculations provide insights into the catalytic mechanism.
  • DFT modeling offers a viable approach to study complex organometallic reactions.