Hexavalent Americium recovery using Copper(III) periodate
Abstract
Separation of americium from the lanthanides is considered one of the most difficult separation steps in closing the nuclear fuel cycle. One approach to this separation could involve oxidizing americium to the hexavalent state to form a linear dioxo cation while the lanthanides remain as trivalent ions. This work considers aqueous soluble Cu3+ periodate as an oxidant under molar nitric acid conditions to separate hexavalent Am with diamyl amylphosphonate (DAAP) in n-dodecane. Initial studies assessed the kinetics of Cu3+ periodate autoreduction in acidic media to aid in development of the solvent extraction system. Following characterization of the Cu3+ periodate oxidant, solvent extraction studies optimized the recovery of Am from varied nitric acid media and in the presence of other fission product, or fission product surrogate, species. Short aqueous/organic contact times encouraged successful recovery of Am (distribution values as high as 2) from nitric acid media in the absence of redox active fission products. In the presence of a post-plutonium uranium redox extraction (post-PUREX) simulant aqueous feed, precipitation of tetravalent species (Ce, Ru, Zr) occurred and the distribution values of 241Am were suppressed, suggesting some oxidizing capacity of the Cu3+ periodate is significantly consumed by other redox active metals in themore »
- Authors:
-
- Colorado School of Mines, Golden, CO (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
- OSTI Identifier:
- 1333664
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 55; Journal Issue: 22; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Citation Formats
McCann, Kevin, Brigham, Derek M., Morrison, Samuel, and Braley, Jenifer C. Hexavalent Americium recovery using Copper(III) periodate. United States: N. p., 2016.
Web. doi:10.1021/acs.inorgchem.6b02120.
McCann, Kevin, Brigham, Derek M., Morrison, Samuel, & Braley, Jenifer C. Hexavalent Americium recovery using Copper(III) periodate. United States. https://doi.org/10.1021/acs.inorgchem.6b02120
McCann, Kevin, Brigham, Derek M., Morrison, Samuel, and Braley, Jenifer C. Mon .
"Hexavalent Americium recovery using Copper(III) periodate". United States. https://doi.org/10.1021/acs.inorgchem.6b02120. https://www.osti.gov/servlets/purl/1333664.
@article{osti_1333664,
title = {Hexavalent Americium recovery using Copper(III) periodate},
author = {McCann, Kevin and Brigham, Derek M. and Morrison, Samuel and Braley, Jenifer C.},
abstractNote = {Separation of americium from the lanthanides is considered one of the most difficult separation steps in closing the nuclear fuel cycle. One approach to this separation could involve oxidizing americium to the hexavalent state to form a linear dioxo cation while the lanthanides remain as trivalent ions. This work considers aqueous soluble Cu3+ periodate as an oxidant under molar nitric acid conditions to separate hexavalent Am with diamyl amylphosphonate (DAAP) in n-dodecane. Initial studies assessed the kinetics of Cu3+ periodate autoreduction in acidic media to aid in development of the solvent extraction system. Following characterization of the Cu3+ periodate oxidant, solvent extraction studies optimized the recovery of Am from varied nitric acid media and in the presence of other fission product, or fission product surrogate, species. Short aqueous/organic contact times encouraged successful recovery of Am (distribution values as high as 2) from nitric acid media in the absence of redox active fission products. In the presence of a post-plutonium uranium redox extraction (post-PUREX) simulant aqueous feed, precipitation of tetravalent species (Ce, Ru, Zr) occurred and the distribution values of 241Am were suppressed, suggesting some oxidizing capacity of the Cu3+ periodate is significantly consumed by other redox active metals in the simulant. Furthermore, the manuscript demonstrates Cu3+ periodate as a potentially viable oxidant for Am oxidation and recovery and notes the consumption of oxidizing capacity observed in the presence of the post-PUREX simulant feed will need to be addressed for any approach seeking to oxidize Am for separations relevant to the nuclear fuel cycle.},
doi = {10.1021/acs.inorgchem.6b02120},
journal = {Inorganic Chemistry},
number = 22,
volume = 55,
place = {United States},
year = {Mon Oct 31 00:00:00 EDT 2016},
month = {Mon Oct 31 00:00:00 EDT 2016}
}
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