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Title: Evaluation of ALSEPO

Abstract

The level three milestone (M3FT-17IN030102013) "Evaluation of ALSEPO” has been completed. Researchers at INL are studying the impacts of gamma radiolysis on the Actinide Lanthanide Separation Process (ALSEP) flowsheet. The ALSEP process is being developed by the DOE-NE Material Recovery and Waste Form Development Campaign. The process solvent used a combination of the solvating extractant N,N,N’,N’-tetra(2-ethylhexyl)diglycolamide and the cation exchanging extractant 2-ethylhexylphosphonic acid mono-2-ethylehxyl ester dissolved in an aliphatic diluent. The actinides and lanthanides are co-extracted from nitric acid solution and the actinides are selectively stripped using a carboxylic acid buffered aminopolycarboxylic acid solution. The results irradiation studies previously performed at the INL on another diglycolamide-based solvent extraction system containing 1-octanol as a phase modifier suggested that the octanol may be serving to inhibit the radiolytic degradation of the ALSEP extractants. Although the mechanism of this radioprotection was not determined, the addition of octanol to the ALSEP solvent was proposed. The goal of this research program was to establish the mechanism responsible for the observed increase in the radiation hardiness of the ALSEP solvent upon the addition of 1-octanol. In addition, other possible enhancements of solvent behavior such as possible increased resistance to third phase formation and enhanced extraction/stripping kineticsmore » were examined. The addition of 1-octanol to the ALSEP formulation at either 1 % or 5 % (v/v) does reduce the rate of degradation of the solvent when exposed to gamma radiation. Unfortunately, the addition of the polar phase modifier essentially destroyed the An/Ln separation usually achievable with ALSEP chemistry. This loss of An/Ln separation ability is presumably do to the disruption of HEH[EHP] dimer formation due to the addition of the polar alcohol. The addition of octanol does not appear to have any significant impact upon the rate of removal of either americium or europium radiotracer from the loaded organic solvents. Based upon the distribution ratio data obtained for the 1% octanol and 5 % octanol ALSEPO solvent systems and the lack of any enhancement in the rate of stripping of the actinides and lanthanides from the loaded solvent, further efforts to reformulate the ALSEPO solvent were abandoned.« less

Authors:
 [1];  [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
Publication Date:
Research Org.:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1408742
Report Number(s):
INL/EXT-17-43040
DOE Contract Number:  
AC07-05ID14517
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Actinide; ALSEP; ALSEPO; Lanthanide; Separation

Citation Formats

Zalupski, Peter R., and Peterman, Dean R. Evaluation of ALSEPO. United States: N. p., 2017. Web. doi:10.2172/1408742.
Zalupski, Peter R., & Peterman, Dean R. Evaluation of ALSEPO. United States. doi:10.2172/1408742.
Zalupski, Peter R., and Peterman, Dean R. Fri . "Evaluation of ALSEPO". United States. doi:10.2172/1408742. https://www.osti.gov/servlets/purl/1408742.
@article{osti_1408742,
title = {Evaluation of ALSEPO},
author = {Zalupski, Peter R. and Peterman, Dean R.},
abstractNote = {The level three milestone (M3FT-17IN030102013) "Evaluation of ALSEPO” has been completed. Researchers at INL are studying the impacts of gamma radiolysis on the Actinide Lanthanide Separation Process (ALSEP) flowsheet. The ALSEP process is being developed by the DOE-NE Material Recovery and Waste Form Development Campaign. The process solvent used a combination of the solvating extractant N,N,N’,N’-tetra(2-ethylhexyl)diglycolamide and the cation exchanging extractant 2-ethylhexylphosphonic acid mono-2-ethylehxyl ester dissolved in an aliphatic diluent. The actinides and lanthanides are co-extracted from nitric acid solution and the actinides are selectively stripped using a carboxylic acid buffered aminopolycarboxylic acid solution. The results irradiation studies previously performed at the INL on another diglycolamide-based solvent extraction system containing 1-octanol as a phase modifier suggested that the octanol may be serving to inhibit the radiolytic degradation of the ALSEP extractants. Although the mechanism of this radioprotection was not determined, the addition of octanol to the ALSEP solvent was proposed. The goal of this research program was to establish the mechanism responsible for the observed increase in the radiation hardiness of the ALSEP solvent upon the addition of 1-octanol. In addition, other possible enhancements of solvent behavior such as possible increased resistance to third phase formation and enhanced extraction/stripping kinetics were examined. The addition of 1-octanol to the ALSEP formulation at either 1 % or 5 % (v/v) does reduce the rate of degradation of the solvent when exposed to gamma radiation. Unfortunately, the addition of the polar phase modifier essentially destroyed the An/Ln separation usually achievable with ALSEP chemistry. This loss of An/Ln separation ability is presumably do to the disruption of HEH[EHP] dimer formation due to the addition of the polar alcohol. The addition of octanol does not appear to have any significant impact upon the rate of removal of either americium or europium radiotracer from the loaded organic solvents. Based upon the distribution ratio data obtained for the 1% octanol and 5 % octanol ALSEPO solvent systems and the lack of any enhancement in the rate of stripping of the actinides and lanthanides from the loaded solvent, further efforts to reformulate the ALSEPO solvent were abandoned.},
doi = {10.2172/1408742},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2017},
month = {8}
}