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Title: Performance of an i-SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop

Here, the i-SANEX solvent formulation consisting of nominally 0.2 M TODGA/5% 1-octanol/dodecane was γ-irradiated under realistic conditions in the Idaho National Laboratory radiolysis test loop, in contact with both extraction and stripping aqueous phases. The extraction aqueous phase was 4.5 M HNO 3, and the stripping aqueous phase was 0.018 M SO 3–Ph–BTP/0.35 M HNO 3. When irradiated in contact with only the 4.5 M HNO 3 phase, the TODGA solvent maintained excellent extraction performance for americium, cerium, europium, and neodymium to a maximum absorbed dose of nearly 0.9 MGy. The results for preliminary static, batch irradiations were consistent with test loop findings. When the aqueous phase was changed to that containing the aqueous soluble BTP, the irradiated aqueous phase showed a dramatic color change, but this does not appear to have had adverse effect on solvent extraction performance. The distribution ratios for both the lanthanides and actinides were invariant with absorbed dose, and the separation factors were essentially unchanged to a maximum absorbed dose of 174 kGy. The results of inductively coupled plasma mass spectrometry analysis of the aqueous and organic phases showed that ruthenium and strontium were not extracted in the presence of the irradiated BTP-aqueous phase. Molybdenummore » was extracted under both conditions. Further, the buildup of corrosion products of stainless steel in the presence of the BTP was not dramatically greater than in the nitric acid-only system. Phase separation times were not adversely affected by irradiation for either system. The results presented here indicate that the performance of the TODGA/SO 3–Ph–BTP, i-SANEX process under test loop radiolysis is much better than expected based on a literature report using single-phase batch irradiation experiments, and better than might be predicted based on diglycolamide radiolysis studies alone.« less
Authors:
ORCiD logo [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [1] ; ORCiD logo [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Karlsruhe Institute of Technology (KIT), Karlsruhe (Germany)
  3. Forschungszentrum Jülich GmbH (FZJ), Jülich (Germany)
  4. Centro de Investigaciones Energeticas Medioambientales y Tecnologicas (CIEMAT), Madrid (Spain)
Publication Date:
Report Number(s):
INL/JOU-16-39376-Rev000
Journal ID: ISSN 0888-5885
Grant/Contract Number:
AC07-05ID14517
Type:
Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 55; Journal Issue: 39; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Research Org:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org:
USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Radiolysis; i-Sanex
OSTI Identifier:
1469199

Peterman, Dean R., Geist, Andreas, Mincher, Bruce, Modolo, Giuseppe, Galán, Maria Hitos, Olson, Lonnie, and McDowell, Rocklan G.. Performance of an i-SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop. United States: N. p., Web. doi:10.1021/acs.iecr.6b02862.
Peterman, Dean R., Geist, Andreas, Mincher, Bruce, Modolo, Giuseppe, Galán, Maria Hitos, Olson, Lonnie, & McDowell, Rocklan G.. Performance of an i-SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop. United States. doi:10.1021/acs.iecr.6b02862.
Peterman, Dean R., Geist, Andreas, Mincher, Bruce, Modolo, Giuseppe, Galán, Maria Hitos, Olson, Lonnie, and McDowell, Rocklan G.. 2016. "Performance of an i-SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop". United States. doi:10.1021/acs.iecr.6b02862. https://www.osti.gov/servlets/purl/1469199.
@article{osti_1469199,
title = {Performance of an i-SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop},
author = {Peterman, Dean R. and Geist, Andreas and Mincher, Bruce and Modolo, Giuseppe and Galán, Maria Hitos and Olson, Lonnie and McDowell, Rocklan G.},
abstractNote = {Here, the i-SANEX solvent formulation consisting of nominally 0.2 M TODGA/5% 1-octanol/dodecane was γ-irradiated under realistic conditions in the Idaho National Laboratory radiolysis test loop, in contact with both extraction and stripping aqueous phases. The extraction aqueous phase was 4.5 M HNO3, and the stripping aqueous phase was 0.018 M SO3–Ph–BTP/0.35 M HNO3. When irradiated in contact with only the 4.5 M HNO3 phase, the TODGA solvent maintained excellent extraction performance for americium, cerium, europium, and neodymium to a maximum absorbed dose of nearly 0.9 MGy. The results for preliminary static, batch irradiations were consistent with test loop findings. When the aqueous phase was changed to that containing the aqueous soluble BTP, the irradiated aqueous phase showed a dramatic color change, but this does not appear to have had adverse effect on solvent extraction performance. The distribution ratios for both the lanthanides and actinides were invariant with absorbed dose, and the separation factors were essentially unchanged to a maximum absorbed dose of 174 kGy. The results of inductively coupled plasma mass spectrometry analysis of the aqueous and organic phases showed that ruthenium and strontium were not extracted in the presence of the irradiated BTP-aqueous phase. Molybdenum was extracted under both conditions. Further, the buildup of corrosion products of stainless steel in the presence of the BTP was not dramatically greater than in the nitric acid-only system. Phase separation times were not adversely affected by irradiation for either system. The results presented here indicate that the performance of the TODGA/SO3–Ph–BTP, i-SANEX process under test loop radiolysis is much better than expected based on a literature report using single-phase batch irradiation experiments, and better than might be predicted based on diglycolamide radiolysis studies alone.},
doi = {10.1021/acs.iecr.6b02862},
journal = {Industrial and Engineering Chemistry Research},
number = 39,
volume = 55,
place = {United States},
year = {2016},
month = {9}
}