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Uranium(VI) bis(imido) chalcogenate complexes: synthesis and density functional theory analysis.

Liam P Spencer1, Ping Yang, Brian L Scott

  • 1Materials, Physics and Applications Division, Los Alamos National Laboratory, MS J514, Los Alamos, New Mexico 87545, USA.

Inorganic Chemistry
|February 17, 2009
PubMed
Summary

New uranium(VI) complexes featuring bis(imido) and dichalcogenate ligands were synthesized. These complexes, including the first monodentate selenolate and tellurolate uranium(VI) compounds, show increasing covalent U-E bonds with larger chalcogenate donors.

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Area of Science:

  • Organometallic Chemistry
  • Uranium Chemistry
  • Coordination Chemistry

Background:

  • Uranium(VI) chemistry is crucial for understanding f-element behavior.
  • Synthesis of novel uranium complexes expands knowledge of its coordination sphere.
  • Chalcogenate ligands offer unique bonding properties.

Purpose of the Study:

  • To synthesize and characterize novel bis(imido) uranium(VI) dichalcogenate complexes.
  • To explore the bonding characteristics of uranium-chalcogen bonds.
  • To report the first monodentate selenolate and tellurolate complexes of uranium(VI).

Main Methods:

  • Synthesis of uranium(VI) complexes with general formulas U(N(t)Bu)2(EAr)2(OPPh3)2 and U(N(t)Bu)2(EAr)2(R2bpy).
  • Characterization of synthesized complexes.
  • Density functional theory (DFT) calculations to investigate electronic structure and bonding.

Main Results:

  • Successful preparation of trans- and cis-bis(imido) uranium(VI) dichalcogenate complexes.
  • The study reports the first monodentate selenolate and tellurolate complexes of uranium(VI).
  • DFT calculations reveal increasing covalent interactions in U-E bonds with larger chalcogenate donors and significant 5f and 6d orbital participation in U-S, U-Se, and U-Te bonds.

Conclusions:

  • Novel uranium(VI) dichalcogenate complexes have been synthesized and characterized.
  • The electronic structure calculations provide insights into the nature of the uranium-chalcogen bond.
  • This work expands the scope of known uranium coordination compounds and their bonding.