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Title: Spectroscopic and computational investigation of actinium coordination chemistry

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.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [4]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Stanford Univ., CA (United States)
  3. California State Polytechnic Univ., Pomona, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Cornell Univ., Ithaca, NY (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Report Number(s):
LA-UR-16-20582
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC52-06NA25396; AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Nuclear Physics (NP) (SC-26); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Inst. of Health (NIH) (United States)
Contributing Orgs:
Stanford Univ., CA (United States); California State Polytechnic Univ., Pomona, CA (United States); Cornell Univ., Ithaca, NY (United States)
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; inorganic chemistry; nuclear chemistry
OSTI Identifier:
1338756

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., and Wilson, Justin J.. Spectroscopic and computational investigation of actinium coordination chemistry. United States: N. p., Web. doi:10.1038/ncomms12312.
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.. Spectroscopic and computational investigation of actinium coordination chemistry. United States. doi:10.1038/ncomms12312.
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., and Wilson, Justin J.. 2016. "Spectroscopic and computational investigation of actinium coordination chemistry". United States. doi:10.1038/ncomms12312. https://www.osti.gov/servlets/purl/1338756.
@article{osti_1338756,
title = {Spectroscopic and computational investigation of actinium coordination chemistry},
author = {Ferrier, Maryline Ghislaine and Batista, Enrique Ricardo and Berg, John M. and Birnbaum, Eva R. and Cross, Justin Neil and Engle, Jonathan Ward and La Pierre, Henry S. and Kozimor, Stosh Anthony and Lezama Pacheco, Juan S. and Stein, Benjamin W. and Stieber, S. Chantal E. and Wilson, Justin J.},
abstractNote = {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–OH2O 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). Finally, these results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique AcIII chemical behaviour.},
doi = {10.1038/ncomms12312},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {8}
}