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Title: 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 UO 2(NO 3) 2∙ 6H 2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO 2(NO 3) 2∙ 6H 2O 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:
 [1];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Security and Isotope Technology Division
  2. 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. doi:10.1021/acs.inorgchem.6b01430.
Burns, Jonathan D., and Moyer, Bruce A.. Wed . "Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling". United States. doi: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},
journal = {Inorganic Chemistry},
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}
}

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