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Covalency-Driven Dimerization of Plutonium(IV) in a Hydroxamate Complex.

Mark A Silver1, Samantha K Cary1, Jared T Stritzinger1

  • 1Department of Chemistry and Biochemistry, Florida State University , Tallahassee, Florida 32306, United States.

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|May 27, 2016
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This summary is machine-generated.

Formohydroxamic acid reacts with plutonium(III) to form a Pu(IV) dimer. This dimer formation involves covalent bonding between plutonium 5f orbitals and the hydroxamate ligand, causing a distinct charge-transfer feature.

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Area of Science:

  • Inorganic Chemistry
  • Radiochemistry
  • Computational Chemistry

Background:

  • Formohydroxamic acid (FHA) is known to stabilize plutonium(III) oxidation states.
  • Hydroxamates act as both reductants and strong π-donor ligands in coordination chemistry.

Purpose of the Study:

  • To investigate the reaction between formohydroxamic acid and plutonium(III).
  • To elucidate the mechanism of plutonium oxidation and complex formation.
  • To characterize the electronic structure of the resulting plutonium complex.

Main Methods:

  • Experimental reaction of Pu(III) with FHA.
  • Spectroscopic analysis to identify complex formation and oxidation state.
  • Time-dependent density functional theory (TD-DFT) calculations.

Main Results:

  • Slow oxidation of Pu(III) to Pu(IV) was observed.
  • Formation of a dimeric plutonium(IV) complex, Pu2(FHA)8, was identified.
  • Evidence of covalency between Pu 5f orbitals and FHA π* orbitals was found.
  • A broad, intense ligand-to-metal charge-transfer (LMCT) band was observed and assigned.

Conclusions:

  • The reaction leads to unexpected Pu(IV) formation and dimerization.
  • Dimerization is driven by π-orbital covalency between plutonium and formohydroxamate.
  • TD-DFT calculations support the LMCT assignment and the observed electronic structure.