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Title: Astatine partitioning between nitric acid and conventional solvents: indication of covalency in ketone complexation of AtO+

Abstract

Astatine-211 has been produced at Texas A&M University on the K150 cyclotron, with a yield of 890 ± 80 MBq through the 209Bi(α,2n)211At reaction via an 8 h bombardment with a beam current of 4–8 μA and an α-particle beam energy of 28.8 MeV. The target was then dissolved in HNO3 and the extraction of 211At was investigated into a variety of organic solvents in 1–3 M HNO3. Extraction of 211At with distribution ratios as high as 11.3 ± 0.6, 12.3 ± 0.8, 42.2 ± 2.2, 69 ± 4, and 95 ± 6 were observed for diisopropyl ether, 1-decanol, 1-octanol, 3-octanone, and methyl isobutyl ketone, respectively, while the distribution ratios for 207Bi were ≤0.05 in all cases. The extraction of 211At into both methyl isobutyl ketone and 3-octanone showed a strong, linear dependence on the HNO3 initial aqueous concentration and better extraction than other solvents. DFT calculations show stronger binding between the carbonyl oxygen of the ketone and the At metal center.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [2];  [2]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [3]
  1. Texas A & M Univ., College Station, TX (United States). Nuclear Engineering and Science Center
  2. Texas A & M Univ., College Station, TX (United States). Cyclotron Inst.
  3. Texas A & M Univ., College Station, TX (United States). Cyclotron Inst. Dept. of Chemistry
  4. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Texas A & M Univ., College Station, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Nuclear Physics (NP); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1800800
Alternate Identifier(s):
OSTI ID: 1637727
Grant/Contract Number:  
FG02-93ER40773; NA0003841
Resource Type:
Accepted Manuscript
Journal Name:
ChemComm
Additional Journal Information:
Journal Volume: 56; Journal Issue: 63; Journal ID: ISSN 1359-7345
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Burns, Jonathan D., Tereshatov, Evgeny E., McCarthy, Mallory A., McIntosh, Lauren A., Tabacaru, Gabriel C., Yang, Xin, Hall, Michael B., and Yennello, Sherry J. Astatine partitioning between nitric acid and conventional solvents: indication of covalency in ketone complexation of AtO+. United States: N. p., 2020. Web. doi:10.1039/d0cc03804k.
Burns, Jonathan D., Tereshatov, Evgeny E., McCarthy, Mallory A., McIntosh, Lauren A., Tabacaru, Gabriel C., Yang, Xin, Hall, Michael B., & Yennello, Sherry J. Astatine partitioning between nitric acid and conventional solvents: indication of covalency in ketone complexation of AtO+. United States. https://doi.org/10.1039/d0cc03804k
Burns, Jonathan D., Tereshatov, Evgeny E., McCarthy, Mallory A., McIntosh, Lauren A., Tabacaru, Gabriel C., Yang, Xin, Hall, Michael B., and Yennello, Sherry J. Mon . "Astatine partitioning between nitric acid and conventional solvents: indication of covalency in ketone complexation of AtO+". United States. https://doi.org/10.1039/d0cc03804k. https://www.osti.gov/servlets/purl/1800800.
@article{osti_1800800,
title = {Astatine partitioning between nitric acid and conventional solvents: indication of covalency in ketone complexation of AtO+},
author = {Burns, Jonathan D. and Tereshatov, Evgeny E. and McCarthy, Mallory A. and McIntosh, Lauren A. and Tabacaru, Gabriel C. and Yang, Xin and Hall, Michael B. and Yennello, Sherry J.},
abstractNote = {Astatine-211 has been produced at Texas A&M University on the K150 cyclotron, with a yield of 890 ± 80 MBq through the 209Bi(α,2n)211At reaction via an 8 h bombardment with a beam current of 4–8 μA and an α-particle beam energy of 28.8 MeV. The target was then dissolved in HNO3 and the extraction of 211At was investigated into a variety of organic solvents in 1–3 M HNO3. Extraction of 211At with distribution ratios as high as 11.3 ± 0.6, 12.3 ± 0.8, 42.2 ± 2.2, 69 ± 4, and 95 ± 6 were observed for diisopropyl ether, 1-decanol, 1-octanol, 3-octanone, and methyl isobutyl ketone, respectively, while the distribution ratios for 207Bi were ≤0.05 in all cases. The extraction of 211At into both methyl isobutyl ketone and 3-octanone showed a strong, linear dependence on the HNO3 initial aqueous concentration and better extraction than other solvents. DFT calculations show stronger binding between the carbonyl oxygen of the ketone and the At metal center.},
doi = {10.1039/d0cc03804k},
journal = {ChemComm},
number = 63,
volume = 56,
place = {United States},
year = {Mon Jun 29 00:00:00 EDT 2020},
month = {Mon Jun 29 00:00:00 EDT 2020}
}

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