Synthesis and Characterization of the Actinium Aquo Ion
Abstract
Metal aquo ions occupy central roles in all equilibria that define metal complexation in natural environments. These complexes are used to establish thermodynamic metrics (i.e., stability constants) for predicting metal binding, which are essential for defining critical parameters associated with aqueous speciation, metal chelation, in vivo transport, and so on. As such, establishing the fundamental chemistry of the actinium(III) aquo ion (Ac-aquo ion, Ac(H2O)x3+) is critical for current efforts to develop 225Ac [t1/2 = 10.0(1) d] as a targeted anticancer therapeutic agent. However, given the limited amount of actinium available for study and its high radioactivity, many aspects of actinium chemistry remain poorly defined. We overcame these challenges using the longer-lived 227Ac [t1/2 = 21.772(3) y] isotope and report the first characterization of this fundamentally important Ac-aquo coordination complex. Our X-ray absorption fine structure study revealed 10.9 ± 0.5 water molecules directly coordinated to the AcIII cation with an Ac–OH2O distance of 2.63(1) Å. This experimentally determined distance was consistent with molecular dynamics density functional theory results that showed (over the course of 8 ps) that AcIII was coordinated by 9 water molecules with Ac–OH2O distances ranging from 2.61 to 2.76 Å. Lastly, the data is presented in the contextmore »
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1344367
- Report Number(s):
- LA-UR-16-28891
Journal ID: ISSN 2374-7943; TRN: US1700898
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Central Science
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 3; Journal ID: ISSN 2374-7943
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Ferrier, Maryline G., Stein, Benjamin W., Batista, Enrique R., Berg, John M., Birnbaum, Eva R., Engle, Jonathan W., John, Kevin D., Kozimor, Stosh A., Lezama Pacheco, Juan S., and Redman, Lindsay N. Synthesis and Characterization of the Actinium Aquo Ion. United States: N. p., 2017.
Web. doi:10.1021/acscentsci.6b00356.
Ferrier, Maryline G., Stein, Benjamin W., Batista, Enrique R., Berg, John M., Birnbaum, Eva R., Engle, Jonathan W., John, Kevin D., Kozimor, Stosh A., Lezama Pacheco, Juan S., & Redman, Lindsay N. Synthesis and Characterization of the Actinium Aquo Ion. United States. https://doi.org/10.1021/acscentsci.6b00356
Ferrier, Maryline G., Stein, Benjamin W., Batista, Enrique R., Berg, John M., Birnbaum, Eva R., Engle, Jonathan W., John, Kevin D., Kozimor, Stosh A., Lezama Pacheco, Juan S., and Redman, Lindsay N. Wed .
"Synthesis and Characterization of the Actinium Aquo Ion". United States. https://doi.org/10.1021/acscentsci.6b00356. https://www.osti.gov/servlets/purl/1344367.
@article{osti_1344367,
title = {Synthesis and Characterization of the Actinium Aquo Ion},
author = {Ferrier, Maryline G. and Stein, Benjamin W. and Batista, Enrique R. and Berg, John M. and Birnbaum, Eva R. and Engle, Jonathan W. and John, Kevin D. and Kozimor, Stosh A. and Lezama Pacheco, Juan S. and Redman, Lindsay N.},
abstractNote = {Metal aquo ions occupy central roles in all equilibria that define metal complexation in natural environments. These complexes are used to establish thermodynamic metrics (i.e., stability constants) for predicting metal binding, which are essential for defining critical parameters associated with aqueous speciation, metal chelation, in vivo transport, and so on. As such, establishing the fundamental chemistry of the actinium(III) aquo ion (Ac-aquo ion, Ac(H2O)x3+) is critical for current efforts to develop 225Ac [t1/2 = 10.0(1) d] as a targeted anticancer therapeutic agent. However, given the limited amount of actinium available for study and its high radioactivity, many aspects of actinium chemistry remain poorly defined. We overcame these challenges using the longer-lived 227Ac [t1/2 = 21.772(3) y] isotope and report the first characterization of this fundamentally important Ac-aquo coordination complex. Our X-ray absorption fine structure study revealed 10.9 ± 0.5 water molecules directly coordinated to the AcIII cation with an Ac–OH2O distance of 2.63(1) Å. This experimentally determined distance was consistent with molecular dynamics density functional theory results that showed (over the course of 8 ps) that AcIII was coordinated by 9 water molecules with Ac–OH2O distances ranging from 2.61 to 2.76 Å. Lastly, the data is presented in the context of other actinide(III) and lanthanide(III) aquo ions characterized by XAFS and highlights the uniqueness of the large AcIII coordination numbers and long Ac–OH2O bond distances.},
doi = {10.1021/acscentsci.6b00356},
journal = {ACS Central Science},
number = 3,
volume = 3,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2017},
month = {Wed Feb 01 00:00:00 EST 2017}
}
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High-Energy X-ray Absorption Spectroscopy: A New Tool for Structural Investigations of Lanthanoids and Third-Row Transition Elements
journal, March 2008
- D'Angelo, Paola; De Panfilis, Simone; Filipponi, Adriano
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Extraction chromatographic behavior of actinium and REE on DGA, Ln and TRU resins in nitric acid solutions
journal, August 2015
- Ostapenko, V.; Vasiliev, A.; Lapshina, E.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 306, Issue 3
An overview of targeted alpha therapy
journal, December 2011
- Kim, Young-Seung; Brechbiel, Martin W.
- Tumor Biology, Vol. 33, Issue 3
Anion-exchange studies with actinium and lanthanides in nitrate solutions
journal, November 1958
- Danon, J.
- Journal of Inorganic and Nuclear Chemistry, Vol. 7, Issue 4
Chemical separations for super-heavy element searches in irradiated uranium targets
journal, February 1975
- Horwitz, E. P.; Bloomquist, C. A. A.
- Journal of Inorganic and Nuclear Chemistry, Vol. 37, Issue 2
Cleaning rare earth elements from actinium
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Production of actinium-225 for alpha particle mediated radioimmunotherapy
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Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes
journal, February 2015
- Radchenko, V.; Engle, J. W.; Wilson, J. J.
- Journal of Chromatography A, Vol. 1380, p. 55-63
Extraction chromatography of lanthanides using N,N,N′,N′-tetraoctyl diglycolamide (TODGA) as the stationary phase
journal, September 2008
- Husain, M.; Ansari, S. A.; Mohapatra, P. K.
- Desalination, Vol. 229, Issue 1-3
Evaluation of nitrogen-rich macrocyclic ligands for the chelation of therapeutic bismuth radioisotopes
journal, May 2015
- Wilson, Justin J.; Ferrier, Maryline; Radchenko, Valery
- Nuclear Medicine and Biology, Vol. 42, Issue 5
Synthesis, Conjugation, and Radiolabeling of a Novel Bifunctional Chelating Agent for 225 Ac Radioimmunotherapy Applications
journal, July 2000
- Chappell, Lara L.; Deal, Kim A.; Dadachova, Ekaterina
- Bioconjugate Chemistry, Vol. 11, Issue 4
Oxidation State and Local Structure of Plutonium Reacted with Magnetite, Mackinawite, and Chukanovite
journal, September 2011
- Kirsch, Regina; Fellhauer, David; Altmaier, Marcus
- Environmental Science & Technology, Vol. 45, Issue 17
The Curium Aqua Ion
journal, April 2007
- Skanthakumar, S.; Antonio, Mark R.; Wilson, Richard E.
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The Crystal Structure of Neodymium Bromate Enneahydrate, Nd(BrO 3 ) 3 ·9H 2 O
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- Journal of the American Chemical Society, Vol. 61, Issue 6
Improved in Vivo Stability of Actinium-225 Macrocyclic Complexes
journal, July 1999
- Deal, Kim A.; Davis, Ila A.; Mirzadeh, Saed
- Journal of Medicinal Chemistry, Vol. 42, Issue 15
Spectroscopic and computational investigation of actinium coordination chemistry
journal, August 2016
- Ferrier, Maryline G.; Batista, Enrique R.; Berg, John M.
- Nature Communications, Vol. 7, Issue 1
The coordination (hydration) of rare earth ions in aqueous chloride solutions from x‐ray diffraction. II. LaCl 3 , PrCl 3 , and NdCl 3 a)
journal, April 1979
- Habenschuss, Anton; Spedding, Frank H.
- The Journal of Chemical Physics, Vol. 70, Issue 8
The coordination (hydration) of rare earth ions in aqueous chloride solutions from x‐ray diffraction. III. SmCl 3 , EuCl 3 , and series behavior
journal, July 1980
- Habenschuss, Anton; Spedding, Frank H.
- The Journal of Chemical Physics, Vol. 73, Issue 1
An extended x‐ray absorption fine structure study of aqueous rare earth perchlorate solutions in liquid and glassy states
journal, October 1988
- Yamaguchi, Toshio; Nomura, Masaharu; Wakita, Hisanobu
- The Journal of Chemical Physics, Vol. 89, Issue 8
An Improved Method for the Production of Ac‐225/Bi‐213 from Th‐229 for Targeted Alpha Therapy
journal, April 2007
- Zielinska, B.; Apostolidis, C.; Bruchertseifer, F.
- Solvent Extraction and Ion Exchange, Vol. 25, Issue 3
Synergistic Enhancement of the Extraction of Trivalent Lanthanides and Actinides by Tetra‐( n ‐Octyl)Diglycolamide from Chloride Media
journal, January 2008
- Philip Horwitz, E.; McAlister, Daniel R.; Thakkar, Anil H.
- Solvent Extraction and Ion Exchange, Vol. 26, Issue 1
Extraction Behavior of Metal Ions by TODGA, DOODA, MIDOA, and NTAamide Extractants from HNO 3 to n -Dodecane
journal, July 2013
- Sasaki, Yuji; Tsubata, Yasuhiro; Kitatsuji, Yoshihiro
- Solvent Extraction and Ion Exchange, Vol. 31, Issue 4
The Actinide-Lanthanide Separation Concept
journal, May 2014
- Lumetta, Gregg J.; Gelis, Artem V.; Carter, Jennifer C.
- Solvent Extraction and Ion Exchange, Vol. 32, Issue 4
Isolation of Medicine-Applicable Actinium-225 from Thorium Targets Irradiated by Medium-Energy Protons
journal, June 2014
- Aliev, R. A.; Ermolaev, S. V.; Vasiliev, A. N.
- Solvent Extraction and Ion Exchange, Vol. 32, Issue 5
Behavior of Actinium, Alkaline, and Rare Earth Elements in Sr-Resin/Mineral Acid Systems
journal, March 2015
- Filosofov, Dmitry V.; Lebedev, Nikolai A.; Radchenko, Valery
- Solvent Extraction and Ion Exchange, Vol. 33, Issue 5
Tumor Therapy with Targeted Atomic Nanogenerators
journal, November 2001
- McDevitt, M. R.
- Science, Vol. 294, Issue 5546
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