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Title: Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides

Abstract

As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O 3PC 6H 4PO 3) 1-x/2(APO 4)x·nH 2O: where M=Zr 4+, Sn 4+, A=H, Na, or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.

Authors:
 [1]
+ Show Author Affiliations
  1. Texas A & M Univ., College Station, TX (United States)
Publication Date:
Research Org.:
Texas A & M Univ., College Station, TX (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1407693
Report Number(s):
DOE/NEUP-13-4758
13-4758; TRN: US1800020
DOE Contract Number:
NE0000746
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; RARE EARTHS; NUCLEAR FUELS; FUEL CYCLE; WASTES; ACTINIDES

Citation Formats

Clearfield, Abraham. Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides. United States: N. p., 2017. Web. doi:10.2172/1407693.
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Clearfield, Abraham. Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides. United States. doi:10.2172/1407693.
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Clearfield, Abraham. Tue . "Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides". United States. doi:10.2172/1407693. https://www.osti.gov/servlets/purl/1407693.
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@article{osti_1407693,
title = {Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides},
author = {Clearfield, Abraham},
abstractNote = {As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O3PC6H4PO3)1-x/2(APO4)x·nH2O: where M=Zr4+, Sn4+, A=H, Na, or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.},
doi = {10.2172/1407693},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Oct 24 00:00:00 EDT 2017},
month = {Tue Oct 24 00:00:00 EDT 2017}
}
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Technical Report:
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DOI:  10.2172/1407693
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  • Implementation of a closed loop nuclear fuel cycle requires the utilization of Pu-containing MOX fuels with the important side effect of increased production of the transplutonium actinides, most importantly isotopes of Am and Cm. Because the presence of these isotopes significantly impacts the long-term radiotoxicity of high level waste, it is important that effective methods for their isolation and/or transmutation be developed. Furthermore, since transmutation is most efficiently done in the absence of lanthanide fission products (high yield species with large thermal neutron absorption cross sections) it is important to have efficient procedures for the mutual separation of Am andmore » Cm from the lanthanides. The chemistries of these elements are nearly identical, differing only in the slightly stronger strength of interaction of trivalent actinides with ligand donor atoms softer than O (N, Cl-, S). Research being conducted around the world has led to the development of new reagents and processes with considerable potential for this task. However, pilot scale testing of these reagents and processes has demonstrated the susceptibility of the new classes of reagents to radiolytic and hydrolytic degradation. In this project, separations of trivalent actinides from fission product lanthanides have been investigated in studies of 1) the extraction and chemical stability properties of a class of soft-donor extractants that are adapted from water-soluble analogs, 2) the application of water soluble soft-donor complexing agents in tandem with conventional extractant molecules emphasizing fundamental studies of the TALSPEAK Process. This research was conducted principally in radiochemistry laboratories at Washington State University. Collaborators at the Radiological Processing Laboratory (RPL) at the Pacific Northwest National Laboratory (PNNL) have contributed their unique facilities and capabilities, and have supported student internships at PNNL to broaden their academic experience. New information has been developed to qualify the extraction potential of a class of pyridine-functionalized tetraaza complexants indicating potential single contact Am-Nd separation factors of about 40. The methodology developed for characterization will find further application in our continuing efforts to synthesize and characterize new reagents for this separation. Significant new insights into the performance envelope and supporting information on the TALSPEAK process has also been developed.« less

  • ; ;
    With increased application of MOX fuels and longer burnup times for conventional fuels, higher concentrations of the transplutonium actinides Am and Cm (and even heavier species like Bk and Cf) will be produced. The half-lives of the Am isotopes are significantly longer than those of the most important long-lived, high specific activity lanthanides or the most common Cm, Bk and Cf isotopes, thus the greatest concern as regards long-term radiotoxicity. With the removal and transmutation of Am isotopes, radiation levels of high level wastes are reduced to near uranium mineral levels within less than 1000 years as opposed to themore » time-fram if they remain in the wastes.« less

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  • ;
    A process for separating americium and curium from rare earths by anion exchange based on selective chloride complexing was developed and tested on a laboratory scale. The separation is accomplished by sorption of americium, curium, and rare earths on Dowex 1-10X resin from a solution of 8 M LiNO/dub 3/ followed by selective elution of rare earths with 10 M LiCl and americium-curium elution with 1 M LiCl. In a laboratory demonstration of this process, greater than 99.5% of americium tracer containing no detectable amounts of rare earths was recovered. (auth)