Spectroscopic and computational investigation of actinium coordination chemistry

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. Chantal E. Stieber and Justin J. Wilson
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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
Justin J. Wilson: Los Alamos National Laboratory

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: 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.

Date: 2016
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DOI: 10.1038/ncomms12312

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