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Title: Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

Abstract

The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in a single process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).

Authors:
 [1];  [1]
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  1. Washington State Univ., Pullman, WA (United States)
Publication Date:
Research Org.:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1245822
Report Number(s):
INL/JOU-15-34089
Journal ID: ISSN 0736-6299
Grant/Contract Number:  
AC07-05ID14517
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Solvent Extraction and Ion Exchange
Additional Journal Information:
Journal Volume: 33; Journal Issue: 7; Journal ID: ISSN 0736-6299
Publisher:
Taylor and Francis
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; ALSPEAK; lanthanide; actinide; solvent extraction; Cyanex 923; HEH[EHP]

Citation Formats

Johnson, Aaron T., and Nash, Kenneth L. Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME. United States: N. p., 2015. Web. doi:10.1080/07366299.2015.1085225.
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Johnson, Aaron T., & Nash, Kenneth L. Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME. United States. https://doi.org/10.1080/07366299.2015.1085225
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Johnson, Aaron T., and Nash, Kenneth L. 2015. "Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME". United States. https://doi.org/10.1080/07366299.2015.1085225. https://www.osti.gov/servlets/purl/1245822.
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@article{osti_1245822,
title = {Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME},
author = {Johnson, Aaron T. and Nash, Kenneth L.},
abstractNote = {The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in a single process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).},
doi = {10.1080/07366299.2015.1085225},
url = {https://www.osti.gov/biblio/1245822}, journal = {Solvent Extraction and Ion Exchange},
issn = {0736-6299},
number = 7,
volume = 33,
place = {United States},
year = {Thu Aug 20 00:00:00 EDT 2015},
month = {Thu Aug 20 00:00:00 EDT 2015}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1080/07366299.2015.1085225
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Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

Figures / Tables:

Table 1 Table 1: pH dependence of Nd(III)/Am(III) separation factors (S.F.) for the HEDTA and TTHA systems. 0.2 M Cyanex-923 + 0.2 M HEH[EHP], 0.1 M Glycine with 20 mM HEDTA or 10 mM TTHA.
All figures and tables (9 total)
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Works referenced in this record:

Nuclear fuels – Present and future
journal, May 2009

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EXTRACTION BY N,N,N',N'-TETRAALKYL -2 ALKYL PROPANE -1,3 DIAMIDES. H. U(VI) and Pu(IV)
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Review Article: A Review of the Development and Operational Characteristics of the TALSPEAK Process
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Trivalent f -Element Intra-group Separation by Solvent Extraction with CMPO-complexant System
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A Counter Current Experiment for the Separation of Trivalent Actinides and Lanthanides by the Setfics Process
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Review: Solvent Systems Combining Neutral and Acidic Extractants for Separating Trivalent Lanthanides from the Transuranic Elements
journal, April 2010

Studies on the Partitioning of Actinides from high Level Waste Using a Mixture of Hdehp and cmpo as Extractant
journal, December 2001

Extraction of Lanthanides(III) and Am(III) by Mixtures of Malonamide and Dialkylphosphoric Acid
journal, April 2007

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journal, July 2008

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journal, May 2013

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journal, January 2014

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journal, May 2014

Futuristic back-end of the nuclear fuel cycle with the partitioning of minor actinides
journal, October 2007

Lipophilic ternary complexes in liquid–liquid extraction of trivalent lanthanides
journal, February 2012

Study of the Interaction between HDEHP and CMPO and Its Effect on the Extraction of Selected Lanthanides
journal, July 2012

Cyanex 923 as an Extractant for Trivalent Lanthanides and Yttrium
journal, May 1998

Solvent extraction of uranium(VI) and thorium(IV) from nitrate media by Cyanex 923
journal, January 2000

Simplified Chinese TRPO Process to Extract and Recover Transuranium Elements from High‐Level Liquid Waste
journal, December 2004

Radioactive Tracer Tests of Two Improved TRPO Processes for High-Level Liquid Waste Using Annular Centrifugal Contactors
journal, October 2014

Alternatives to HDEHP and DTPA for Simplified TALSPEAK Separations
journal, June 2011

The role of carboxylic acids in TALSQuEAK separations
journal, August 2012

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journal, December 1958

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Trivalent Lanthanide/Actinide Separation Using Aqueous-Modified TALSPEAK Chemistry
journal, May 2014

Trans‐Lanthanide Extraction Studies in the TALSPEAK System: Investigating the Effect of Acidity and Temperature
journal, April 2009

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    Works referencing / citing this record:

    Ligands for f-element extraction used in the nuclear fuel cycle
    journal, January 2017

    Coordination of rare earth element cations on the surface of silica-derived nanoadsorbents
    journal, January 2018

    Unfolding the complexation and extraction of Am 3+ and Eu 3+ using N-heterocyclic aromatic diphosphonic acids: a combined experimental and DFT study
    journal, January 2019

    Interactions between Extractant Molecules: Organic-Phase Thermodynamics of TALSPEAK–MME
    journal, January 2017

    Interactions between Extractant Molecules: Organic-Phase Thermodynamics of TALSPEAK–MME
    text, January 2017

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      Figures / Tables found in this record:

      Table 1(p. 16)table
      Figure 1(p. 22)figure
      Figure 2(p. 23)figure
      Figure 3(p. 24)figure
      Figure 4(p. 25)figure
      Figure 5(p. 26)figure
      Figure 6(p. 27)figure
      Figure 7(p. 28)figure
      Figure 8(p. 29)figure
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