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Title: Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning

Abstract

In response to the NEUP Program Supporting Fuel Cycle R&D Separations and Waste Forms call DEFOA- 0000799, this report describes the results of an R&D project focusing on streamlining separation processes for advanced fuel cycles. An example of such a process relevant to the U.S. DOE FCR&D program would be one combining the functions of the TRUEX process for partitioning of lanthanides and minor actinides from PUREX(UREX) raffinates with that of the TALSPEAK process for separating transplutonium actinides from fission product lanthanides. A fully-developed PUREX(UREX)/TRUEX/TALSPEAK suite would generate actinides as product(s) for reuse (or transmutation) and fission products as waste. As standalone, consecutive unit-operations, TRUEX and TALSPEAK employ different extractant solutions (solvating (CMPO, octyl(phenyl)-N,Ndiisobutylcarbamoylmethylphosphine oxide) vs. cation exchanging (HDEHP, di-2(ethyl)hexylphosphoric acid) extractants), and distinct aqueous phases (2-4 M HNO 3 vs. concentrated pH 3.5 carboxylic acid buffers containing actinide selective chelating agents). The separate processes may also operate with different phase transfer kinetic constraints. Experience teaches (and it has been demonstrated at the lab scale) that, with proper control, multiple process separation systems can operate successfully. However, it is also recognized that considerable economies of scale could be achieved if multiple operations could be merged into a single process basedmore » on a combined extractant solvent. The task of accountability of nuclear materials through the process(es) also becomes more robust with fewer steps, providing that the processes can be accurately modeled. Work is underway in the U.S. and Europe on developing several new options for combined processes (TRUSPEAK, ALSEP, SANEX, GANEX, ExAm are examples). There are unique challenges associated with the operation of such processes, some relating to organic phase chemistry, others arising from the variable composition of the aqueous medium. This project targets in particular two problematic issues in designing combined process systems: managing the chemistry of challenging aqueous species (like Zr 4+) and optimizing the composition and properties of combined extractant organic phases.« less

Authors:
 [1];  [1];  [1]
  1. Washington State Univ., Pullman, WA (United States)
Publication Date:
Research Org.:
Washington State Univ., Pullman, WA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1351946
Report Number(s):
13-5350
13-5350
DOE Contract Number:  
NE0000674
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wall, Nathalie, Nash, Ken, and Martin, Leigh. Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning. United States: N. p., 2017. Web. doi:10.2172/1351946.
Wall, Nathalie, Nash, Ken, & Martin, Leigh. Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning. United States. doi:10.2172/1351946.
Wall, Nathalie, Nash, Ken, and Martin, Leigh. Fri . "Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning". United States. doi:10.2172/1351946. https://www.osti.gov/servlets/purl/1351946.
@article{osti_1351946,
title = {Managing Zirconium Chemistry and Phase Compatibility in Combined Process Separations for Minor Actinide Partitioning},
author = {Wall, Nathalie and Nash, Ken and Martin, Leigh},
abstractNote = {In response to the NEUP Program Supporting Fuel Cycle R&D Separations and Waste Forms call DEFOA- 0000799, this report describes the results of an R&D project focusing on streamlining separation processes for advanced fuel cycles. An example of such a process relevant to the U.S. DOE FCR&D program would be one combining the functions of the TRUEX process for partitioning of lanthanides and minor actinides from PUREX(UREX) raffinates with that of the TALSPEAK process for separating transplutonium actinides from fission product lanthanides. A fully-developed PUREX(UREX)/TRUEX/TALSPEAK suite would generate actinides as product(s) for reuse (or transmutation) and fission products as waste. As standalone, consecutive unit-operations, TRUEX and TALSPEAK employ different extractant solutions (solvating (CMPO, octyl(phenyl)-N,Ndiisobutylcarbamoylmethylphosphine oxide) vs. cation exchanging (HDEHP, di-2(ethyl)hexylphosphoric acid) extractants), and distinct aqueous phases (2-4 M HNO3 vs. concentrated pH 3.5 carboxylic acid buffers containing actinide selective chelating agents). The separate processes may also operate with different phase transfer kinetic constraints. Experience teaches (and it has been demonstrated at the lab scale) that, with proper control, multiple process separation systems can operate successfully. However, it is also recognized that considerable economies of scale could be achieved if multiple operations could be merged into a single process based on a combined extractant solvent. The task of accountability of nuclear materials through the process(es) also becomes more robust with fewer steps, providing that the processes can be accurately modeled. Work is underway in the U.S. and Europe on developing several new options for combined processes (TRUSPEAK, ALSEP, SANEX, GANEX, ExAm are examples). There are unique challenges associated with the operation of such processes, some relating to organic phase chemistry, others arising from the variable composition of the aqueous medium. This project targets in particular two problematic issues in designing combined process systems: managing the chemistry of challenging aqueous species (like Zr4+) and optimizing the composition and properties of combined extractant organic phases.},
doi = {10.2172/1351946},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Mar 17 00:00:00 EDT 2017},
month = {Fri Mar 17 00:00:00 EDT 2017}
}

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