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T-shaped cationic CuI complexes with hemilabile PNP-type ligands.

Jarl Ivar van der Vlugt¹, Evgeny A Pidko, Dieter Vogt

¹Schuit Institute of Catalysis, Laboratory of Homogeneous Catalysis, Department of Chemistry and Chemical Engineering, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands. j.i.v.d.vlugt@tue.nl

Inorganic Chemistry

|April 30, 2008

Summary

This study explores the coordination chemistry of copper(I) iodide (CuI) with two PNP ligands. A hemilabile interaction led to a rare T-shaped copper complex with ligand 1A.

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Area of Science:

Coordination Chemistry
Organometallic Chemistry
Inorganic Chemistry

Background:

PNP ligands are crucial in coordination chemistry.
Copper(I) iodide (CuI) exhibits diverse coordination behaviors.
Understanding ligand-metal interactions is key to catalyst design.

Purpose of the Study:

To investigate the coordination behavior of CuI with two distinct PNP ligands: 1A (2,6-bis[(di-tert-butylphosphino)methyl]pyridine) and 1B (2,6-bis[(diphenylphosphino)methyl]pyridine).
To characterize the resulting copper complexes and elucidate the role of ligand structure in coordination geometry.
To explore the hemilabile nature of the pyridine N-donor atom in these complexes.

Main Methods:

Synthesis and characterization of copper(I) complexes with PNP ligands.
X-ray crystallography to determine the solid-state structures of the complexes.
Spectroscopic techniques (e.g., NMR, IR) for structural elucidation.
Theoretical calculations (e.g., DFT) to understand electronic properties and bonding interactions.

Main Results:

The coordination of CuI with ligand 1A (2,6-bis[(di-tert-butylphosphino)methyl]pyridine) yielded a rare T-shaped copper complex, attributed to a hemilabile interaction of the pyridine N-donor atom.
With ligand 1B (2,6-bis[(diphenylphosphino)methyl]pyridine), a tetracoordinated copper species was successfully isolated.
Theoretical calculations confirmed the weak interaction of the pyridine N donor in the 1A complex with the copper center.

Conclusions:

The hemilabile nature of the pyridine N-donor in PNP ligands significantly influences the coordination geometry of copper(I) complexes.
Ligand design, specifically the steric and electronic properties of the phosphine substituents, dictates the formation of different coordination motifs (T-shaped vs. tetracoordinated).
These findings contribute to the understanding of copper coordination chemistry and the development of novel catalytic systems.