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NHCs as Neutral Donors towards Polyphosphorus Complexes.

Felix Riedlberger1, Stefano Todisco2, Piero Mastrorilli2

  • 1Institut für Anorganische Chemie, Universität Regensburg, 93040, Regensburg, Germany.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|August 4, 2020
PubMed
Summary
This summary is machine-generated.

Researchers report the first N-heterocyclic carbene (NHC) adducts with polyphosphorus iron complexes. These adducts exhibit dissociative equilibria in solution, influenced by NHC bulkiness, and a tantalum complex undergoes P-atom abstraction.

Keywords:
N-heterocyclic carbenesNMR spectroscopyironnucleophilic attackphosphorustantalum

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Area of Science:

  • Organometallic Chemistry
  • Main Group Chemistry
  • Coordination Chemistry

Background:

  • N-heterocyclic carbenes (NHCs) are versatile ligands in organometallic chemistry.
  • Polyphosphorus complexes offer unique bonding and reactivity.
  • Understanding ligand-metal interactions in these systems is crucial.

Purpose of the Study:

  • To synthesize and characterize the first adducts of NHCs with aromatic polyphosphorus iron complexes.
  • To investigate the reactivity of a tantalum-phosphorus complex with NHCs.
  • To elucidate reaction mechanisms using computational methods.

Main Methods:

  • Synthesis and isolation of neutral adducts between [Cp*Fe(η5-P5)] and various NHCs (IMe, IMes, IDipp).
  • Investigation of the solution-state behavior of these adducts, including dissociative equilibria.
  • Reaction of [Cp''Ta(CO)2(η4-P4)] with IMe, leading to P-atom abstraction.
  • Density Functional Theory (DFT) calculations to study reaction energetics and pathways.

Main Results:

  • Neutral adducts of NHCs with [Cp*Fe(η5-P5)] were successfully synthesized and isolated.
  • In solution, these adducts undergo rapid dissociation, with equilibrium influenced by the steric bulk of the NHC.
  • Reaction with [Cp''Ta(CO)2(η4-P4)] resulted in unprecedented P-atom abstraction, forming a cyclo-P3-containing anionic tantalum complex.
  • DFT calculations provided insights into the energetic feasibility of observed reaction pathways.

Conclusions:

  • The first NHC adducts with aromatic polyphosphorus iron complexes have been synthesized, revealing solution-state dissociative behavior dependent on NHC sterics.
  • A novel P-atom abstraction reaction was observed for a tantalum-phosphorus complex, yielding a unique anionic cyclo-P3 complex.
  • Computational studies support the proposed reaction mechanisms and energetics.