Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation

Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.

doi:10.1080/07366299.2015.1064296

Title: Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation

Full Record
Other Related Research

Abstract

The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquid system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.

Authors:

Zalupski, Peter R. ^[1]; Klaehn, John R. ^[1]; Peterman, Dean R. ^[1]

Idaho National Lab. (INL), Idaho Falls, ID (United States)

Publication Date:: Thu Jul 30 00:00:00 EDT 2015

Research Org.:: Idaho National Lab. (INL), Idaho Falls, ID (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1259499

Report Number(s):: INL/JOU-15-34616
Journal ID: ISSN 0736-6299

Grant/Contract Number:: AC07-05ID14517

Resource Type:: Accepted Manuscript

Journal Name:: Solvent Extraction and Ion Exchange

Additional Journal Information:: Journal Volume: 33; Journal Issue: 6; Journal ID: ISSN 0736-6299

Publisher:: Taylor and Francis

Country of Publication:: United States

Language:: English

Subject:: 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; dithiophosphinic acid; diaryldithiophosphinic acid; trioctylphosphine oxide; synergic extraction; actinide; lanthanide; separation factor; neptunium optical spectroscopy

Citation Formats


                    Zalupski, Peter R., Klaehn, John R., and Peterman, Dean R. Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation.  United States: N. p., 2015. 
Web.  doi:10.1080/07366299.2015.1064296.

Copy to clipboard


                    Zalupski, Peter R., Klaehn, John R., & Peterman, Dean R. Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation.  United States.  https://doi.org/10.1080/07366299.2015.1064296

Copy to clipboard


                    Zalupski, Peter R., Klaehn, John R., and Peterman, Dean R. Thu .  
"Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation".  United States.  https://doi.org/10.1080/07366299.2015.1064296.  https://www.osti.gov/servlets/purl/1259499.

Copy to clipboard


                    
@article{osti_1259499,

  title        = {Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation},

  author       = {Zalupski, Peter R. and Klaehn, John R. and Peterman, Dean R.},

  abstractNote = {The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquid system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.},

  doi          = {10.1080/07366299.2015.1064296},

  journal      = {Solvent Extraction and Ion Exchange},

  number       = 6,

  volume       = 33,

  place        = {United States},

  year         = {Thu Jul 30 00:00:00 EDT 2015},

  month        = {Thu Jul 30 00:00:00 EDT 2015}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1080/07366299.2015.1064296

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 1 work

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Similar Records in DOE PAGES and OSTI.GOV collections:

Feasibility of actinide separation from UREX-like raffinates using a combination of sulfur- and oxygen-donor extractants

Conference Zalupski, P. R. ; Peterman, D. R. ; Riddle, C. L.

A synergistic combination of bis(o-trifluoromethylphenyl)dithios-phosphinic acid and trioctylphosphine oxide has been recently shown to selectively remove uranium, neptunium, plutonium and americium from aqueous environment containing up to 0.5 M nitric acid and 5.5 g/l fission products. Here the feasibility of performing this complete actinide recovery from aqueous mixtures is forecasted for a new organic formulation containing sulfur donor extractant of modified structure based on Am(III) and Eu(III) extraction data. A mixture of bis(bis-m,m-trifluoromethyl)phenyl)-dithios-phosphinic acid and TOPO in toluene enhances the extraction performance, accomplishing Am/Eu differentiation in aqueous mixtures up to 1 M nitric acid. The new organic recipe is alsomore »« less
Feasibility of actinide separation from UREX-like raffinates using a combination of sulfur- and oxygen-donor extractants

Conference Zalupski, Peter R. ; Peterman, Dean R. ; Riddle, Catherine L.

A synergistic combination of bis(o-trifluoromethylphenyl)dithiosphosphinic acid and trioctylphosphine oxide has been recently shown to selectively remove uranium, neptunium, plutonium and americium from aqueous environment containing up to 0.5 M nitric acid and 5.5 g/L fission products. Here the feasibility of performing this complete actinide recovery from aqueous mixtures is forecasted for a new organic formulation containing sulfur donor extractant of modified structure based on Am(III) and Eu(III) extraction data. A mixture of bis(bis-m,m-trifluoromethyl)phenyl)-dithiosphosphinic acid and TOPO in toluene enhances the extraction performance, accomplishing Am/Eu differentiation in aqueous mixtures up to 1 M nitric acid. The new organic recipe is alsomore »« less
Full Text Available
INL DPAH STAAR 2015 Annual Report

Technical Report Peterman, Dean Richard

Research conducted at the INL has demonstrated the synergistic extraction of americium using solvents comprised of bis(o,o-(trifluoromethyl)phenyl) dithiophosphinic acid (DPAH “1”) and trioctylphosphine oxide (TOPO), butyl bis(2,4,4-trimethylpentyl) phosphinate (BuCy272), or dibutyl butylphosphonate (DBBP). One potential drawback of this separations scheme is that soft metals such as silver, cadmium, or palladium and fission products such as zirconium are well extracted by these solvents. Several potential scrubbing reagents were examined. Of the scrubbing reagents studied, cysteine and methione exhibited some ability to scrub soft metals from the loaded solvent. More conventional scrub reagents such as ammonium fluoride or oxalic acid were notmore »« less
https://doi.org/10.2172/1260884

Full Text Available
Synergistic selective extraction of actinides(III) over lanthanides from nitric acid using new aromatic diorganyldithiophosphinic acids and neutral organophosphorus compounds

Journal Article Modolo, G ; Odoj, R - Solvent Extraction and Ion Exchange

New aromatic dithiophosphinic acids (R{sub 2}PSSH) with R = C{sub 6}H{sub 5{sup {minus}}}, ClC{sub 6}H{sub 4{sup {minus}}}, FC{sub 6}H{sub 4{sup {minus}}} and CH{sub 3}C{sub 6}H{sub 4{sup {minus}}} were synthesized, characterized and tested as potential separating agents for trivalent actinides over lanthanides. The extraction of Am(III), Eu(III) and other lanthanides was carried out from nitric acid medium with mixtures of R{sub 2}PSSHs and neutral organophosphorus compounds. There was no detectable extraction when R{sub 2}PSSHs were used alone as extractants for either Am(III) or Eu(III) (D{sub Am,Eu} < 10{sup {minus}3}) under the experimental conditions used in this study. High separation factors (D{submore »« less
https://doi.org/10.1080/07360299908934599
The Effects of Radiation Chemistry on Solvent Extraction 4. Separation of the Trivalent Actinides and Considerations for Radiation-Resistant Solvent Systems

Journal Article Mincher, Bruce J ; Modolo, Giuseppe ; Mezyk, Stephen P - Solvent Extraction and Ion Exchange

The separation of the minor actinides from dissolved nuclear fuel is one of the more formidable challenges associated with the design of the advanced fuel cycle. The partitioning of americium and its transmutation in fast reactor fuel would reduce high-level-waste long-term storage requirements by as much as two orders of magnitude. However, the lanthanides have very similar chemistry. They also have large neutron capture cross sections and poor metal alloy properties and thus they can not be incorporated into fast reactor fuel. A separation amenable to currently existing aqueous solvent extraction processes is therefore desired, and research is underway inmore »« less
https://doi.org/10.1080/07366299.2010.485548

Similar Records