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  • NatureChem_Pulsed_2016_AIP_final

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Actinide covalency measured by pulsed electron paramagnetic resonance spectroscopy

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  • Alasdair Formanuik
  • Ariciu Ana-Maria
  • Fabrizio Ortu
  • Reece Beekmeyer
  • Andrew Kerridge
  • Floriana Tuna
  • Eric McInnes
  • David Mills
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<mark>Journal publication date</mark>06/2017
<mark>Journal</mark>Nature Chemistry
Issue number6
Volume9
Number of pages6
Pages (from-to)578-583
Publication StatusPublished
Early online date26/12/16
<mark>Original language</mark>English

Abstract

Our knowledge of actinide chemical bonds lags far behind our understanding of the bonding regimes of any other series of elements. This is a major issue given the technological as well as fundamental importance of f-block elements. Some key chemical differences between actinides and lanthanides—and between different actinides—can be ascribed to minor differences in covalency, that is, the degree to which electrons are shared between the f-block element and coordinated ligands. Yet there are almost no direct measures of such covalency for actinides. Here we report the first pulsed electron paramagnetic resonance spectra of actinide compounds. We apply the hyperfine sublevel correlation technique to quantify the electron-spin density at ligand nuclei (via the weak hyperfine interactions) in molecular thorium(III) and uranium(III) species and therefore the extent of covalency. Such information will be important in developing our understanding of the chemical bonding, and therefore the reactivity, of actinides.

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© 2016 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.