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Title: Summary of TRUEX Radiolysis Testing Using the INL Radiolysis Test Loop

Abstract

The INL radiolysis and hydrolysis test loop has been used to evaluate the effects of hydrolytic and radiolytic degradation upon the efficacy of the TRUEX flowsheet for the recovery of trivalent actinides and lanthanides from acidic solution. Repeated irradiation and subsequent re-conditioning cycles did result in a significant decrease in the concentration of the TBP and CMPO extractants in the TRUEX solvent and a corresponding decrease in americium and europium extraction distributions. However, the build-up of solvent degradation products upon {gamma}-irradiation, had little impact upon the efficiency of the stripping section of the TRUEX flowsheet. Operation of the TRUEX flowsheet would require careful monitoring to ensure extraction distributions are maintained at acceptable levels.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Idaho National Laboratory (INL)
Sponsoring Org.:
DOE - NE
OSTI Identifier:
1046071
Report Number(s):
INL/EXT-12-25311
TRN: US1203744
DOE Contract Number:
DE-AC07-05ID14517
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; ACTINIDES; AMERICIUM; EFFICIENCY; EUROPIUM; FLOWSHEETS; HYDROLYSIS; IRRADIATION; MONITORING; RADIOLYSIS; RARE EARTHS; SOLVENTS; TESTING; CMPO; Degradation; Radiolysis; TBP; Test Loop; TRUEX

Citation Formats

Dean R. Peterman, Lonnie G. Olson, Rocklan G. McDowell, Gracy Elias, and Jack D. Law. Summary of TRUEX Radiolysis Testing Using the INL Radiolysis Test Loop. United States: N. p., 2012. Web. doi:10.2172/1046071.
Dean R. Peterman, Lonnie G. Olson, Rocklan G. McDowell, Gracy Elias, & Jack D. Law. Summary of TRUEX Radiolysis Testing Using the INL Radiolysis Test Loop. United States. doi:10.2172/1046071.
Dean R. Peterman, Lonnie G. Olson, Rocklan G. McDowell, Gracy Elias, and Jack D. Law. Thu . "Summary of TRUEX Radiolysis Testing Using the INL Radiolysis Test Loop". United States. doi:10.2172/1046071. https://www.osti.gov/servlets/purl/1046071.
@article{osti_1046071,
title = {Summary of TRUEX Radiolysis Testing Using the INL Radiolysis Test Loop},
author = {Dean R. Peterman and Lonnie G. Olson and Rocklan G. McDowell and Gracy Elias and Jack D. Law},
abstractNote = {The INL radiolysis and hydrolysis test loop has been used to evaluate the effects of hydrolytic and radiolytic degradation upon the efficacy of the TRUEX flowsheet for the recovery of trivalent actinides and lanthanides from acidic solution. Repeated irradiation and subsequent re-conditioning cycles did result in a significant decrease in the concentration of the TBP and CMPO extractants in the TRUEX solvent and a corresponding decrease in americium and europium extraction distributions. However, the build-up of solvent degradation products upon {gamma}-irradiation, had little impact upon the efficiency of the stripping section of the TRUEX flowsheet. Operation of the TRUEX flowsheet would require careful monitoring to ensure extraction distributions are maintained at acceptable levels.},
doi = {10.2172/1046071},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Mar 01 00:00:00 EST 2012},
month = {Thu Mar 01 00:00:00 EST 2012}
}

Technical Report:

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  • The INL radiolysis test loop has been used to evaluate the affect of radiolytic degradation upon the efficacy of the strip section of the TRUEX flowsheet for the recovery of trivalent actinides and lanthanides from acidic solution. The nominal composition of the TRUEX solvent used in this study is 0.2 M CMPO and 1.4 M TBP dissolved in n-dodecane and the nominal composition of the TRUEX strip solution is 1.5 M lactic acid and 0.050 M diethylenetriaminepentaacetic acid. Gamma irradiation of a mixture of TRUEX process solvent and stripping solution in the test loop does not adversely impact flowsheet performancemore » as measured by stripping americium ratios. The observed increase in americium stripping distribution ratios with increasing absorbed dose indicates the radiolytic production of organic soluble degradation compounds.« less
  • Design and installation has been completed for a state-of-the-art radiolysis/hydrolysis test loop system. The system is used to evaluate the effects of gamma radiolysis and acid hydrolysis on the stability and performance of solvent extraction process solvents. The test loop is comprised of two main sections; the solvent irradiation and hydrolysis loop and the solvent reconditioning loop. In the solvent irradiation and hydrolysis loop, aqueous and organic phases are mixed and circulated through a gamma irradiator until the desired absorbed dose is achieved. Irradiation of the mixed phases is more representative of actual conditions in a solvent extraction process. Additionally,more » the contact of the organic phase with the aqueous phase will subject the solvent components to hydrolysis. This hydrolysis can be accelerated by controlling the system at an elevated temperature. At defined intervals, the organic from the irradiation/hydrolysis loop will be transferred to the solvent reconditioning loop where the solvent is contacted with scrub, strip, and solvent wash solutions which simulate process flowsheet conditions. These two processes are repeated until the total desired dose is achieved. Since all viable solvent extraction components in an advanced fuel cycle must exhibit high radiolytic and hydrolytic stability, this test loop is not limited to any one solvent system but is applicable to all systems of interest. Also, the test loop is not limited to testing of process flowsheets. It is also a valuable tool in support of fundamental research on newly identified extractants/modifiers and the impact of gamma radiation on their stability in a dynamic environment. The investigation of the radiolysis of a TBP/n-dodecane process solvent in contact with aqueous nitric acid has been performed. These studies were intended to confirm/optimize the operability of the test loop system. Additionally, these data are directly applicable to numerous other solvent extraction processes containing TBP that are being developed to support advanced aqueous separations processes. Initial experimental results are consistent with existing literature reports regarding TBP/n-dodecane radiolysis. Additionally, the gamma dose rate has been characterized within the test loop and analytical methods have been developed for the characterization and quantification of radiolytic degradation products.« less
  • Separating the minor actinide elements (americium and curium) from the fission product lanthanides is an important step in closing the nuclear fuel cycle. Isolating the minor actinides will allow transmuting them to short lived or stable isotopes in fast reactors, thereby reducing the long-term hazard associated with these elements. The Actinide Lanthanide Separation Process (ALSEP) is being developed by the DOE-NE Material Recovery and Waste Form Development Campaign to accomplish this separation with a single process. To develop a fundamental understanding of the solvent degradation mechanisms for the ALSEP Process, testing was performed in the INL Radiolysis/Hydrolysis Test Loop formore » the extraction section of the ALSEP flowsheet. This work culminated in the completion of the level two milestone (M2FT-16IN030102021) "Complete ALSEP test loop solvent irradiation test.” This report summarizes the testing performed and the impact of radiation on the ALSEP Process performance as a function of dose.« less