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Spectroscopic and computational investigation of actinium coordination chemistry

Author

Listed:
  • Maryline G. Ferrier

    (Los Alamos National Laboratory)

  • Enrique R. Batista

    (Los Alamos National Laboratory)

  • John M. Berg

    (Los Alamos National Laboratory)

  • Eva R. Birnbaum

    (Los Alamos National Laboratory)

  • Justin N. Cross

    (Los Alamos National Laboratory)

  • Jonathan W. Engle

    (Los Alamos National Laboratory)

  • Henry S. La Pierre

    (Los Alamos National Laboratory)

  • Stosh A. Kozimor

    (Los Alamos National Laboratory)

  • Juan S. Lezama Pacheco

    (Stanford University)

  • Benjamin W. Stein

    (Los Alamos National Laboratory)

  • S. Chantal E. Stieber

    (Los Alamos National Laboratory
    California State Polytechnic University)

  • Justin J. Wilson

    (Los Alamos National Laboratory
    Cornell University)

Abstract

Actinium-225 is a promising isotope for targeted-α therapy. Unfortunately, progress in developing chelators for medicinal applications has been hindered by a limited understanding of actinium chemistry. This knowledge gap is primarily associated with handling actinium, as it is highly radioactive and in short supply. Hence, AcIII reactivity is often inferred from the lanthanides and minor actinides (that is, Am, Cm), with limited success. Here we overcome these challenges and characterize actinium in HCl solutions using X-ray absorption spectroscopy and molecular dynamics density functional theory. The Ac–Cl and Ac − O H 2 O distances are measured to be 2.95(3) and 2.59(3) Å, respectively. The X-ray absorption spectroscopy comparisons between AcIII and AmIII in HCl solutions indicate AcIII coordinates more inner-sphere Cl1– ligands (3.2±1.1) than AmIII (0.8±0.3). These results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique AcIII chemical behaviour.

Suggested Citation

  • Maryline G. Ferrier & Enrique R. Batista & John M. Berg & Eva R. Birnbaum & Justin N. Cross & Jonathan W. Engle & Henry S. La Pierre & Stosh A. Kozimor & Juan S. Lezama Pacheco & Benjamin W. Stein & S, 2016. "Spectroscopic and computational investigation of actinium coordination chemistry," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms12312
    DOI: 10.1038/ncomms12312
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    Cited by:

    1. Jennifer N. Wacker & Joshua J. Woods & Peter B. Rupert & Appie Peterson & Marc Allaire & Wayne W. Lukens & Alyssa N. Gaiser & Stefan G. Minasian & Roland K. Strong & Rebecca J. Abergel, 2024. "Actinium chelation and crystallization in a macromolecular scaffold," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

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