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Title: An Advanced TALSPEAK Concept for Separating Minor Actinides. Part 2. Flowsheet Test with Actinide-spiked Simulant

Abstract

A solvent extraction system has been developed for separating trivalent actinides from lanthanides. This “Advanced TALSPEAK” system uses 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester to extract the lanthanides into a n-dodecane-based solvent phase, while the actinides are retained in a citrate-buffered aqueous phase by complexation to N-(2-hydroxyethyl)ethylenediamine-N,N',N'-triacetic acid. Batch distribution measurements indicate that the separation of americium from the light lanthanides decreases as the pH decreases. For example, the separation factor between La and Am increases from 2.5 at pH 2.0 to 19.3 at pH 3.0. However, previous investigations indicated that the extraction rates for the heavier lanthanides decrease with increasing pH. So, a balance between these two competing effects is required. An aqueous phase in which the pH was set at 2.6 was chosen for further process development because this offered optimal separation, with a minimum separation factor of ~8.4, based on the separation between La and Am. Centrifugal contactor single-stage efficiencies were measured to characterize the performance of the system under flow conditions.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1]; ORCiD logo [1];  [1];  [1];  [3];  [4];  [1]; ORCiD logo [1]
  1. Forschungszentrum Jülich GmbH, Institut für Energie – und Klimaforschung – Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich, Germany
  2. Nuclear Science and Engineering Group, Pacific Northwest National Laboratory, Richland, DC, USA
  3. Aqueous Separations and Radiochemistry Department, Idaho National Laboratory, Idaho Falls, ID, USA
  4. Karlsruhe Institute of Technology (KIT), Institute for Nuclear Waste Disposal (INE), Karlsruhe, Germany
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1406777
Report Number(s):
PNNL-SA-122678
Journal ID: ISSN 0736-6299; AF5805010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Solvent Extraction and Ion Exchange; Journal Volume: 35; Journal Issue: 6
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; actinide extraction; actinide separation; Advanced TALSPEAK; lanthanide separation; HEH[EHP]

Citation Formats

Wilden, Andreas, Lumetta, Gregg J., Sadowski, Fabian, Schmidt, Holger, Schneider, Dimitri, Gerdes, Markus, Law, Jack D., Geist, Andreas, Bosbach, Dirk, and Modolo, Giuseppe. An Advanced TALSPEAK Concept for Separating Minor Actinides. Part 2. Flowsheet Test with Actinide-spiked Simulant. United States: N. p., 2017. Web. doi:10.1080/07366299.2017.1368945.
Wilden, Andreas, Lumetta, Gregg J., Sadowski, Fabian, Schmidt, Holger, Schneider, Dimitri, Gerdes, Markus, Law, Jack D., Geist, Andreas, Bosbach, Dirk, & Modolo, Giuseppe. An Advanced TALSPEAK Concept for Separating Minor Actinides. Part 2. Flowsheet Test with Actinide-spiked Simulant. United States. doi:10.1080/07366299.2017.1368945.
Wilden, Andreas, Lumetta, Gregg J., Sadowski, Fabian, Schmidt, Holger, Schneider, Dimitri, Gerdes, Markus, Law, Jack D., Geist, Andreas, Bosbach, Dirk, and Modolo, Giuseppe. Thu . "An Advanced TALSPEAK Concept for Separating Minor Actinides. Part 2. Flowsheet Test with Actinide-spiked Simulant". United States. doi:10.1080/07366299.2017.1368945.
@article{osti_1406777,
title = {An Advanced TALSPEAK Concept for Separating Minor Actinides. Part 2. Flowsheet Test with Actinide-spiked Simulant},
author = {Wilden, Andreas and Lumetta, Gregg J. and Sadowski, Fabian and Schmidt, Holger and Schneider, Dimitri and Gerdes, Markus and Law, Jack D. and Geist, Andreas and Bosbach, Dirk and Modolo, Giuseppe},
abstractNote = {A solvent extraction system has been developed for separating trivalent actinides from lanthanides. This “Advanced TALSPEAK” system uses 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester to extract the lanthanides into a n-dodecane-based solvent phase, while the actinides are retained in a citrate-buffered aqueous phase by complexation to N-(2-hydroxyethyl)ethylenediamine-N,N',N'-triacetic acid. Batch distribution measurements indicate that the separation of americium from the light lanthanides decreases as the pH decreases. For example, the separation factor between La and Am increases from 2.5 at pH 2.0 to 19.3 at pH 3.0. However, previous investigations indicated that the extraction rates for the heavier lanthanides decrease with increasing pH. So, a balance between these two competing effects is required. An aqueous phase in which the pH was set at 2.6 was chosen for further process development because this offered optimal separation, with a minimum separation factor of ~8.4, based on the separation between La and Am. Centrifugal contactor single-stage efficiencies were measured to characterize the performance of the system under flow conditions.},
doi = {10.1080/07366299.2017.1368945},
journal = {Solvent Extraction and Ion Exchange},
number = 6,
volume = 35,
place = {United States},
year = {Thu Aug 17 00:00:00 EDT 2017},
month = {Thu Aug 17 00:00:00 EDT 2017}
}