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Title: Extraction Behavior of Ln(III) ions by T2EHDGA/n-dodecane from Nitric acid and Sodium Nitrate Solutions

Abstract

The diglycolamide extractant, T2EHDGA, has proven promising for the separation of lanthanides and minor actinides in high-level nuclear waste reprocessing. This neutral extractant has shown significant extraction capacity for HNO3 into the non-polar organic phase, along with hyper-stoichiometric nitrate dependence on extraction of trivalent f-elements. The transport behavior of T2EHDGA/n-dodecane toward trivalent lanthanides is not well understood. This work found a significant increase in distribution measurements for Eu(III) extracted from aqueous HNO3 media as compared to NaNO3. The extraction of Eu(III) from HNO3 results in a different thermodynamic product than predicted by classic solvent extraction of 3:1 ligand-metal complex as observed with NaNO3 in FTIR and UV-vis spectroscopy. Experimental distribution measurements in conjunction with the solvent extraction modeling program, SXLSQI, suggest participation of 1- to 2 HNO3 molecules in the Eu(III)/T2EHDGA complex when extracted from HNO3 media, indicative of a mechanism change responsible for the enhanced extraction behavior toward lanthanides in the presence of HNO3.

Authors:
 [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. BATTELLE (PACIFIC NW LAB)
  2. VISITORS
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1556901
Report Number(s):
PNNL-SA-128106
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Solvent Extraction and Ion Exchange
Additional Journal Information:
Journal Volume: 36; Journal Issue: 4
Country of Publication:
United States
Language:
English

Citation Formats

Campbell, Emily L., Holfeltz, Vanessa E., Hall, Gabriel B., Nash, Kenneth L., Lumetta, Gregg J., and Levitskaia, Tatiana G. Extraction Behavior of Ln(III) ions by T2EHDGA/n-dodecane from Nitric acid and Sodium Nitrate Solutions. United States: N. p., 2018. Web. doi:10.1080/07366299.2018.1447261.
Campbell, Emily L., Holfeltz, Vanessa E., Hall, Gabriel B., Nash, Kenneth L., Lumetta, Gregg J., & Levitskaia, Tatiana G. Extraction Behavior of Ln(III) ions by T2EHDGA/n-dodecane from Nitric acid and Sodium Nitrate Solutions. United States. doi:10.1080/07366299.2018.1447261.
Campbell, Emily L., Holfeltz, Vanessa E., Hall, Gabriel B., Nash, Kenneth L., Lumetta, Gregg J., and Levitskaia, Tatiana G. Wed . "Extraction Behavior of Ln(III) ions by T2EHDGA/n-dodecane from Nitric acid and Sodium Nitrate Solutions". United States. doi:10.1080/07366299.2018.1447261.
@article{osti_1556901,
title = {Extraction Behavior of Ln(III) ions by T2EHDGA/n-dodecane from Nitric acid and Sodium Nitrate Solutions},
author = {Campbell, Emily L. and Holfeltz, Vanessa E. and Hall, Gabriel B. and Nash, Kenneth L. and Lumetta, Gregg J. and Levitskaia, Tatiana G.},
abstractNote = {The diglycolamide extractant, T2EHDGA, has proven promising for the separation of lanthanides and minor actinides in high-level nuclear waste reprocessing. This neutral extractant has shown significant extraction capacity for HNO3 into the non-polar organic phase, along with hyper-stoichiometric nitrate dependence on extraction of trivalent f-elements. The transport behavior of T2EHDGA/n-dodecane toward trivalent lanthanides is not well understood. This work found a significant increase in distribution measurements for Eu(III) extracted from aqueous HNO3 media as compared to NaNO3. The extraction of Eu(III) from HNO3 results in a different thermodynamic product than predicted by classic solvent extraction of 3:1 ligand-metal complex as observed with NaNO3 in FTIR and UV-vis spectroscopy. Experimental distribution measurements in conjunction with the solvent extraction modeling program, SXLSQI, suggest participation of 1- to 2 HNO3 molecules in the Eu(III)/T2EHDGA complex when extracted from HNO3 media, indicative of a mechanism change responsible for the enhanced extraction behavior toward lanthanides in the presence of HNO3.},
doi = {10.1080/07366299.2018.1447261},
journal = {Solvent Extraction and Ion Exchange},
number = 4,
volume = 36,
place = {United States},
year = {2018},
month = {10}
}