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Title: Recovery of minor actinides from spent fuel using TPEN-immobilized gels

Abstract

A series of separation experiments was performed in order to study the recovery process for minor actinides (MAs), such as americium (Am) and curium (Cm), from the actual spent fuel by using an extraction chromatographic technique. N,N,N',N'-tetrakis-(4-propenyloxy-2-pyridylmethyl) ethylenediamine (TPPEN) is an N,N,N',N'-tetrakis (2-pyridylmethyl) ethylenediamine (TPEN) analogue consisting of an incorporated pyridine ring that acts as not only a ligand but also as a site for polymerization and crosslinking of the gel. The TPPEN and N-isopropylacrylamide (NIPA) were dissolved into dimethylformamide (DMF, Wako Co., Ltd.) and a silica beads polymer, and then TTPEN was immobilized chemically in a polymer gel (so called TPEN-gel). Mixed oxide (MOX) fuel, which was highly irradiated up to 119 GWD/MTM in the experimental fast reactor Joyo, was used as a reference spent fuel. First, uranium (U) and plutonium (Pu) were separated from the irradiated fuel using an ion-exchange method, and then, the platinum group elements were removed by CMPO to leave a mixed solution of MAs and lanthanides. The 3 mol% TPPEN-gel was packed with as an extraction column (CV: 1 ml) and then rinsed by 0.1 M NaNO{sub 3}(pH 4.0) for pH adjustment. After washing the column by 0.01 M NaNO{sub 3} (pH 4.0), Eumore » was detected and the recovery rate reached 93%. The MAs were then recovered by changing the eluent to 0.01 M NaNO{sub 3} (pH 2.0), and the recovery rate of Am was 48 %. The 10 mol% TPPEN-gel was used to improve adsorption coefficient of Am and a condition of eluent temperature was changed in order to confirm the temperature swing effect on TPEN-gel for MA. More than 90% Eu was detected in the eluent after washing with 0.01 M NaNO{sub 3} (pH 3.5) at 5 Celsius degrees. Americium was backwardly detected and eluted continuously during the same condition. After removal of Eu, the eluent temperature was changed to 32 Celsius degrees, then Am was detected (pH 3.0). Finally remained Am could be stripped from TPPEN-gel by changing the pH of the eluent to 2.0. These results These results prove that the proposed recovery process for MAs is a potential candidate for future reprocessing methods based on the extraction chromatographic technique. (authors)« less

Authors:
; ;  [1];  [2];  [3]
  1. Oarai Research and Development Center, Japan Atomic Energy Agency, Oarai (Japan)
  2. Solutions Research Organization, Tokyo Institute of Technology, Tokyo (Japan)
  3. Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, Tokyo (Japan)
Publication Date:
Research Org.:
American Nuclear Society, 555 North Kensington Avenue, La Grange Park, IL 60526 (United States)
OSTI Identifier:
22257907
Resource Type:
Conference
Resource Relation:
Conference: GLOBAL 2013: International Nuclear Fuel Cycle Conference - Nuclear Energy at a Crossroads, Salt Lake City, UT (United States), 29 Sep - 3 Oct 2013; Other Information: Country of input: France; 11 refs.; Related Information: In: Proceedings of GLOBAL 2013: International Nuclear Fuel Cycle Conference - Nuclear Energy at a Crossroads| 1633 p.
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; AMERICIUM; CHROMATOGRAPHY; CROSS-LINKING; CURIUM; EXTRACTION; EXTRACTION COLUMNS; GELS; JOYO REACTOR; MATERIALS RECOVERY; MIXED OXIDE FUELS; PH VALUE; PLATINUM; PLUTONIUM; PYRIDINE; RARE EARTHS; SILICA; SODIUM NITRATES; SPENT FUELS; URANIUM; WASHING

Citation Formats

Koyama, S., Suto, M., Ohbayashi, H., Oaki, H., and Takeshita, K. Recovery of minor actinides from spent fuel using TPEN-immobilized gels. United States: N. p., 2013. Web.
Koyama, S., Suto, M., Ohbayashi, H., Oaki, H., & Takeshita, K. Recovery of minor actinides from spent fuel using TPEN-immobilized gels. United States.
Koyama, S., Suto, M., Ohbayashi, H., Oaki, H., and Takeshita, K. Mon . "Recovery of minor actinides from spent fuel using TPEN-immobilized gels". United States.
@article{osti_22257907,
title = {Recovery of minor actinides from spent fuel using TPEN-immobilized gels},
author = {Koyama, S. and Suto, M. and Ohbayashi, H. and Oaki, H. and Takeshita, K.},
abstractNote = {A series of separation experiments was performed in order to study the recovery process for minor actinides (MAs), such as americium (Am) and curium (Cm), from the actual spent fuel by using an extraction chromatographic technique. N,N,N',N'-tetrakis-(4-propenyloxy-2-pyridylmethyl) ethylenediamine (TPPEN) is an N,N,N',N'-tetrakis (2-pyridylmethyl) ethylenediamine (TPEN) analogue consisting of an incorporated pyridine ring that acts as not only a ligand but also as a site for polymerization and crosslinking of the gel. The TPPEN and N-isopropylacrylamide (NIPA) were dissolved into dimethylformamide (DMF, Wako Co., Ltd.) and a silica beads polymer, and then TTPEN was immobilized chemically in a polymer gel (so called TPEN-gel). Mixed oxide (MOX) fuel, which was highly irradiated up to 119 GWD/MTM in the experimental fast reactor Joyo, was used as a reference spent fuel. First, uranium (U) and plutonium (Pu) were separated from the irradiated fuel using an ion-exchange method, and then, the platinum group elements were removed by CMPO to leave a mixed solution of MAs and lanthanides. The 3 mol% TPPEN-gel was packed with as an extraction column (CV: 1 ml) and then rinsed by 0.1 M NaNO{sub 3}(pH 4.0) for pH adjustment. After washing the column by 0.01 M NaNO{sub 3} (pH 4.0), Eu was detected and the recovery rate reached 93%. The MAs were then recovered by changing the eluent to 0.01 M NaNO{sub 3} (pH 2.0), and the recovery rate of Am was 48 %. The 10 mol% TPPEN-gel was used to improve adsorption coefficient of Am and a condition of eluent temperature was changed in order to confirm the temperature swing effect on TPEN-gel for MA. More than 90% Eu was detected in the eluent after washing with 0.01 M NaNO{sub 3} (pH 3.5) at 5 Celsius degrees. Americium was backwardly detected and eluted continuously during the same condition. After removal of Eu, the eluent temperature was changed to 32 Celsius degrees, then Am was detected (pH 3.0). Finally remained Am could be stripped from TPPEN-gel by changing the pH of the eluent to 2.0. These results These results prove that the proposed recovery process for MAs is a potential candidate for future reprocessing methods based on the extraction chromatographic technique. (authors)},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2013},
month = {7}
}

Conference:
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