Spectroscopic and computational investigation of actinium coordination chemistry

Ferrier, Maryline Ghislaine; Batista, Enrique Ricardo; Berg, John M.; Birnbaum, Eva R.; Cross, Justin Neil; Engle, Jonathan Ward; La Pierre, Henry S.; Kozimor, Stosh Anthony; Lezama Pacheco, Juan S.; Stein, Benjamin W.; Stieber, S. Chantal E.; Wilson, Justin J.

doi:10.1038/ncomms12312

Title: Spectroscopic and computational investigation of actinium coordination chemistry

Journal Article · Wed Aug 17 00:00:00 EDT 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms12312· OSTI ID:1338756

Ferrier, Maryline Ghislaine ^[1]; Batista, Enrique Ricardo ^[1]; Berg, John M. ^[1]; Birnbaum, Eva R. ^[1]; Cross, Justin Neil ^[1]; Engle, Jonathan Ward ^[1]; La Pierre, Henry S. ^[1]; Kozimor, Stosh Anthony ^[1]; Lezama Pacheco, Juan S. ^[2]; Stein, Benjamin W. ^[1]; Stieber, S. Chantal E. ^[3]; Wilson, Justin J. ^[4]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Stanford Univ., CA (United States)
California State Polytechnic Univ., Pomona, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Cornell Univ., Ithaca, NY (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

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, Ac^III 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_H₂O distances are measured to be 2.95(3) and 2.59(3) Å, respectively. The X-ray absorption spectroscopy comparisons between Ac^III and Am^III in HCl solutions indicate Ac^III coordinates more inner-sphere Cl^1– ligands (3.2±1.1) than Am^III (0.8±0.3). Finally, these results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique Ac^III chemical behaviour.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Nuclear Physics (NP); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Inst. of Health (NIH) (United States)

Contributing Organization:: Stanford Univ., CA (United States); California State Polytechnic Univ., Pomona, CA (United States); Cornell Univ., Ithaca, NY (United States)

Grant/Contract Number:: AC52-06NA25396; AC02-76SF00515

OSTI ID:: 1338756

Report Number(s):: LA-UR-16-20582

Journal Information:: Nature Communications, Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 61 works

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