Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling
Abstract
Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO2(NO3)2∙ 6H2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO2(NO3)2∙ 6H2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr, 95Nb, 137Cs, and 144Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Security and Isotope Technology Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
- OSTI Identifier:
- 1325476
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 55; Journal Issue: 17; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; americium; crystallization; minor actinides; nuclear fuel recycle; fission products
Citation Formats
Burns, Jonathan D., and Moyer, Bruce A. Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling. United States: N. p., 2016.
Web. doi:10.1021/acs.inorgchem.6b01430.
Burns, Jonathan D., & Moyer, Bruce A. Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling. United States. https://doi.org/10.1021/acs.inorgchem.6b01430
Burns, Jonathan D., and Moyer, Bruce A. 2016.
"Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling". United States. https://doi.org/10.1021/acs.inorgchem.6b01430. https://www.osti.gov/servlets/purl/1325476.
@article{osti_1325476,
title = {Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling},
author = {Burns, Jonathan D. and Moyer, Bruce A.},
abstractNote = {Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO2(NO3)2∙ 6H2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO2(NO3)2∙ 6H2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr, 95Nb, 137Cs, and 144Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.},
doi = {10.1021/acs.inorgchem.6b01430},
url = {https://www.osti.gov/biblio/1325476},
journal = {Inorganic Chemistry},
issn = {0020-1669},
number = 17,
volume = 55,
place = {United States},
year = {Wed Aug 17 00:00:00 EDT 2016},
month = {Wed Aug 17 00:00:00 EDT 2016}
}
Web of Science
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