Journal
INORGANIC CHEMISTRY
Volume 61, Issue 31, Pages 12087-12096Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c00085
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Funding
- U.S. Department of Energy Isotope Program [DE-SC0020958]
- Texas A&M University through the Bright Chair in Nuclear Science
- Texas A&M System National Laboratories Office
- Los Alamos National Laboratory
- U.S. Department of Energy [DE-SC0020958, DE-NA0003841, DE-FG02-93ER40773, NA0003841]
- College of Arts and Sciences and the O'Neal Comprehensive Cancer Center at the University of Alabama at Birmingham
- Welch Foundation [A-0648]
- National Science Foundation [CHE-1664866]
- U.S. Department of Energy (DOE) [DE-SC0020958] Funding Source: U.S. Department of Energy (DOE)
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Ketones have been proven effective in extracting astatine(III) from aqueous solvents. Co-extraction of NO3- as AtO(NO3).(O=CR1R2) species into the organic phase appears to be a key factor. Adjusting the electronic properties of ketones can enhance the bond strength between the ketone and AtO+ and increase the extraction of astatine into the organic phase. Extraction with diketones is dependent on the bridging distance between the two carbonyl moieties.
Ketones have been proven effective in extracting astatine(III) from aqueous solvents. Previous theoretical studies suggested a mechanism where the sp2 lone pair on the carbonyl oxygen donates electron density into the pi system of the AtO+ molecular cation to form a dative-type bond. In this study, co extraction of NO3- as AtO(NO3).(O=CR1R2) species into the organic phase appears to be a key factor. Adjusting the electronic properties of the ketone, by having an aryl group instead of an alkyl group in the alpha position of the ketone, increased the electron density on C=O, increased the bond strength between the ketone and AtO+, and in turn increased the extraction of 211At into the organic phase. Extraction with diketones shows dependence on the bridging distance between the two carbonyl moieties, where a C3 or longer bridge results in a 10-fold increase in extraction into the organic phase. DFT calculations show the longer bridge allows for the chelation of AtO(NO3) by either the second carbonyl or the phenyl ring.
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