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Comparison of Two Different Synthesis Methods of Single Crystals of Superconducting Uranium Ditelluride

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Transient Covalency in Molten Uranium(III) Chloride.

Dmitry S Maltsev^1,2, Darren M Driscoll¹, Yuanpeng Zhang³

¹Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.

Journal of the American Chemical Society

|July 23, 2024

Summary

High temperatures alter uranium (U) bonding in UCl3, creating shorter U-Cl bonds and increased U 5f orbital involvement. This reveals a unique bonding environment around U(III) at extreme conditions.

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Area of Science:

Inorganic Chemistry
Materials Science
Physical Chemistry

Background:

Uranium (U) is a key actinide element vital for nuclear fuels.
Understanding U's coordination chemistry and bonding at high temperatures is limited.
The role of U 5f orbitals in bonding under extreme conditions is not well-established.

Purpose of the Study:

To investigate the coordination chemistry and bonding of uranium trichloride (UCl3) at high temperatures.
To determine the effect of the solid-to-molten phase transition on U-ligand distances and bonding.
To elucidate the involvement of U 5f valence orbitals in bonding under extreme thermal conditions.

Main Methods:

Experimental techniques to study UCl3 at high temperatures.
Computational modeling to analyze bonding interactions.
Analysis of U-ligand distances and coordination environments.

Main Results:

Observed shrinkage of the average U-ligand distance in UCl3 during the solid-to-molten phase transition.
Formation of a notable fraction of short, transient U-Cl bonds.
Enhanced involvement of U 5f valence orbitals in the bonding interactions.

Conclusions:

Extreme temperatures induce significant changes in the bonding environment of U(III) in UCl3.
A heterogeneous bonding environment with distinct inner and outer coordination subshells is formed.
High temperatures promote enhanced participation of U 5f orbitals in chemical bonding.