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Title: Organic Speciation and Interactions in ALSEP -One Step Partitioning Process of MinorActinides, Lanthanides, and Fission Products

Abstract

Research conducted in this project focused on speciation characterization of the ALSEP extraction system (similar to the TALSPEAK-like application) which addresses recovery of minor actinides and lanthanides from PUREX raffinate. The ALSEP (Actinide-Lanthanide Separation) system proposes a trivalent minor actinide/lanthanide group extraction followed by a selective actinide strip to effectively partition minor actinides, lanthanides, and other fission products. The group extraction is achieved by a mixed organic solvent, combining acidic and neutral extracting ligands. The objective of this work is investigation the interactions of the acidic and neutral ligands with each other in the extraction organic solvent and with desired metals. Four combinations of a cation-exchange ligand (either HDEHP or HEH[EHP]) and a neutral solvating ligand (either TODGA or T2EHDGA) in n-dodecane were studied. Interligand dimers in these combinations were investigated with NMR and FTIR, the strongest interaction was observed for HDEHP+TODGA and weakest for T2EHDGA+HEH[EHP]. Complexes of the trivalent Am and lanthanides Nd, Eu, Ho, Pr in these binary ligand mixtures were probed with spectroscopic (UV–vis, time-resolved fluorescence, XAFS and SAXS-spectroscopies) and extraction (Job’s plot, slope analysis) methods; co-extracted water and nitric acid were analyzed by titration methods. Comparison of the collected spectra showed significant shifting for both DGAmore » ligands with HDEHP, while both combinations of HEH[EHP]+DGA displayed much smaller spectral changes. Data were modeled with HypSpec program, and stability constants for extracted complexes were calculated. Aggregation in these systems were studied by SAXS (small-angle X-ray scattering) spectroscopy and interfacial tension, size of aggregates were measured. Two PhD students graduated (2017, 2018) and one student continues her PhD study.« less

Authors:
 [1]
  1. Oregon State Univ., Corvallis, OR (United States). School of Nuclear Science and Engineering
Publication Date:
Research Org.:
Oregon State Univ., Corvallis, OR (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
Contributing Org.:
Argonne National Laboratory
OSTI Identifier:
1463115
Report Number(s):
13-5124
13-5124
DOE Contract Number:  
NE0000720
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English

Citation Formats

Paulenova, Alena. Organic Speciation and Interactions in ALSEP -One Step Partitioning Process of MinorActinides, Lanthanides, and Fission Products. United States: N. p., 2018. Web. doi:10.2172/1463115.
Paulenova, Alena. Organic Speciation and Interactions in ALSEP -One Step Partitioning Process of MinorActinides, Lanthanides, and Fission Products. United States. doi:10.2172/1463115.
Paulenova, Alena. Sun . "Organic Speciation and Interactions in ALSEP -One Step Partitioning Process of MinorActinides, Lanthanides, and Fission Products". United States. doi:10.2172/1463115. https://www.osti.gov/servlets/purl/1463115.
@article{osti_1463115,
title = {Organic Speciation and Interactions in ALSEP -One Step Partitioning Process of MinorActinides, Lanthanides, and Fission Products},
author = {Paulenova, Alena},
abstractNote = {Research conducted in this project focused on speciation characterization of the ALSEP extraction system (similar to the TALSPEAK-like application) which addresses recovery of minor actinides and lanthanides from PUREX raffinate. The ALSEP (Actinide-Lanthanide Separation) system proposes a trivalent minor actinide/lanthanide group extraction followed by a selective actinide strip to effectively partition minor actinides, lanthanides, and other fission products. The group extraction is achieved by a mixed organic solvent, combining acidic and neutral extracting ligands. The objective of this work is investigation the interactions of the acidic and neutral ligands with each other in the extraction organic solvent and with desired metals. Four combinations of a cation-exchange ligand (either HDEHP or HEH[EHP]) and a neutral solvating ligand (either TODGA or T2EHDGA) in n-dodecane were studied. Interligand dimers in these combinations were investigated with NMR and FTIR, the strongest interaction was observed for HDEHP+TODGA and weakest for T2EHDGA+HEH[EHP]. Complexes of the trivalent Am and lanthanides Nd, Eu, Ho, Pr in these binary ligand mixtures were probed with spectroscopic (UV–vis, time-resolved fluorescence, XAFS and SAXS-spectroscopies) and extraction (Job’s plot, slope analysis) methods; co-extracted water and nitric acid were analyzed by titration methods. Comparison of the collected spectra showed significant shifting for both DGA ligands with HDEHP, while both combinations of HEH[EHP]+DGA displayed much smaller spectral changes. Data were modeled with HypSpec program, and stability constants for extracted complexes were calculated. Aggregation in these systems were studied by SAXS (small-angle X-ray scattering) spectroscopy and interfacial tension, size of aggregates were measured. Two PhD students graduated (2017, 2018) and one student continues her PhD study.},
doi = {10.2172/1463115},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {3}
}