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A Uranium(II) Arene Complex That Acts as a Uranium(I) Synthon.

Mark D Straub1,2, Erik T Ouellette1,2, Michael A Boreen1,2

  • 1Department of Chemistry, University of California, Berkeley, California 94720, United States.

Journal of the American Chemical Society
|November 17, 2021
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Summary

This study reveals the electronic structure of a uranium complex, showing it acts as a U(I) synthon. The research details its reactivity as a reductant, forming new uranium compounds.

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Area of Science:

  • Organometallic Chemistry
  • Uranium Chemistry
  • Actinide Chemistry

Background:

  • Amidate-supported uranium complexes offer unique electronic properties.
  • Understanding the reduction states and reactivity of uranium is crucial for catalysis and materials science.

Purpose of the Study:

  • To synthesize and characterize novel anionic uranium complexes.
  • To investigate the electronic structure and redox behavior of these complexes.
  • To explore the reactivity of reduced uranium species with various substrates.

Main Methods:

  • Synthesis of uranium and thorium amidate complexes.
  • Two-electron reduction using KC8.
  • Spectroscopic characterization (EPR).
  • Magnetic susceptibility measurements.
  • Computational studies (DFT, CASSCF).
  • Reactivity studies with iodine, cycloheptatriene, and cyclooctatetraene.

Main Results:

  • Formation of an anionic bis(arene) complex [K[2.2.2]cryptand][U(TDA)2] (3) with a U(II) center and monoreduced arene.
  • Complex 3 acts as a U(I) synthon, reducing I2 to U(III)-U(III) species and CHT to a U(IV) complex.
  • Reaction with COT yields U(III) and U(COT)2, while complex 2 yields a U(IV)-U(IV) inverse sandwich complex.
  • Reduction of Th(TDA)4 (4) yields [K[2.2.2]cryptand][Th(TDA)3(THF)] (5) with a direduced arene.

Conclusions:

  • The electronic structure of complex 3 is a U(II) center with a monoreduced arene, behaving as a U(I) synthon.
  • The reactivity studies demonstrate the versatile reducing capabilities of the U(I) species.
  • The thorium complex 5 features a direduced arene bound to Th(IV), showcasing different redox behavior.