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Characterizing pressure-induced uranium C-H agostic bonds.

Polly L Arnold1, Alessandro Prescimone2,3, Joy H Farnaby2,4

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High-pressure studies reveal that a diuranium(III) compound exhibits pressure-induced agostic interactions. Computational analysis confirms these interactions emerge at 3.2 GPa, influencing uranium-centered structural changes.

Keywords:
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Area of Science:

  • Organometallic Chemistry
  • High-Pressure Crystallography
  • Computational Chemistry

Background:

  • The study investigates the unique bonding and structural properties of low-coordinate uranium compounds.
  • Understanding the behavior of uranium under extreme conditions is crucial for various chemical applications.

Purpose of the Study:

  • To explore the structural response of a diuranium(III) complex to varying pressures.
  • To investigate the nature of metal-ligand interactions, specifically potential agostic interactions, under pressure.

Main Methods:

  • Variable, high-pressure single-crystal X-ray crystallography was employed to determine structural changes.
  • Density functional theory (DFT) calculations, including Quantum Theory of Atoms-in-Molecules (QTAIM) and Natural Bond Orbital (NBO) analyses, were performed.

Main Results:

  • The diuranium(III) compound [UN''2]2(μ-η(6):η(6)-C6H6) exhibits coupling through π- and δ-symmetric arene overlap.
  • Increasing pressure leads to decreased metal-metal separation and significant changes in close contacts between ligand CH bonds and uranium centers.
  • Agostic-type interactions between uranium and ligand CH groups, initially absent at ambient pressure, were computationally confirmed to form at 3.2 GPa.

Conclusions:

  • Pressure significantly influences the structural dynamics of the diuranium(III) complex, particularly concerning metal-ligand contacts.
  • The formation of agostic interactions at elevated pressures highlights the dynamic nature of bonding in low-coordinate uranium systems.
  • This research provides insights into the pressure-dependent behavior of organometallic uranium compounds.