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Title: Hexavalent Americium recovery using Copper(III) periodate

Journal Article · · Inorganic Chemistry
 [1];  [2];  [3];  [1]
  1. Colorado School of Mines, Golden, CO (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
+ Show Author Affiliations

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1333664
Journal Information:
Inorganic Chemistry, Vol. 55, Issue 22; ISSN 0020-1669
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

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Cited By (2)

Relationship Between Structure and Coordination Strength of N and N,O -Hybrid Donor Ligands with Trivalent Lanthanides journal November 2018
Inner versus outer sphere metal-monoamide complexation: ramifications for tetravalent & hexavalent actinide selectivity journal January 2018

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS