Study on selective separation of uranium(VI) by new N,N-dialkyl carboxy-amides
- Japan Atomic Energy Agency: 2-4 Shirakata-shirane, Tokai-mura, Naka-gun, Ibaraki 319-1195 (Japan)
The Feasibility study (FS) on commercialized FR cycle systems has been carried out in Japan. In this Feasibility study, 'Advanced Aqueous' reprocessing was designed as a new reprocessing concept to enhance nuclear non-proliferation by recycling U, Pu and minor actinides (MA) with some fission products (FP). The crystallization and U(VI)/TRU(transuranics) co-extraction technique have been selected as candidate technique in the 'Advanced Aqueous' reprocessing. In JAEA, the result of Feasibility study was received and Fast Reactor Cycle Technology Development Project (FaCT) was started. In the nuclear spent fuel reprocessing, FBR spent fuels will coexist with LWR spent fuels for several decades until FBR cycle begins to operate. For the treatment of LWR spent fuels, high decontamination factor for FP was required for U(VI) storage, and solvent extraction technique was selected in the nuclear fuel treatment. In our laboratory, N,N-di-alkyl carboxy-amides have been developed as extractant based on solvent extraction technique for one of a back-up technology of 'Advanced Aqueous' reprocessing in FBR spent fuel treatments. N,N-di-alkyl carboxy-amides were noted as one of the alternative extractant of tri-butylphosphate (TBP) in the field of nuclear fuel reprocessing. Extraction behavior of U(VI) and Pu(IV) with N,N-di-alkyl carboxy-amides was almost similar to those with TBP. N,N-di-alkyl carboxy-amides have some advantages, namely, their complete incinerability (CHON principle) and high stability for hydrolysis and radiolysis. Their main degradation products are carboxylic acids and secondary amines which hardly affect the separation of U(VI) and Pu(IV) from fission products. Further, the synthesis of N,N-di-alkyl carboxy-amides was relatively easy with reaction of carboxylic chloride and secondary amine. The main purpose of this solvent extraction technique using N,N-di-alkyl carboxy-amides is selective separation of Uranium(VI) with branched N,N-di-alkyl carboxy-amides and group separation of Pu-Np linear alkyl type N,N-di-alkyl carboxy-amide for FBR and LWR spent fuel treatment. Since the branched alkyl type N,N-di-alkyl carboxy-amides have the steric hindrance on the complexation with metal cations, branched alkyl type N,N-di-alkyl carboxy-amides can be used to separate An(VI) from An(IV). On the other hand, linear type N,N-di-alkyl carboxy-amides have potential for alternative extractant for tri-butyl phosphate(TBP) because linear type N,N-di-alkyl-amide can extract An(VI) and An(IV). In our previous research work, we have proposed N,N-di-(2- ethyl)hexyl-(2,2-dimethyl)-propanamide (D2EHDMPA) as a candidate extractant for uranium selective separation in FBR spent fuel treatments. However D2EHDMPA was able to separate uranium(VI) from plutonium(IV) and neptunium(VI), D2EHDMPA showed poor U(VI) loading capacity in organic phase. For the purpose of improvement of U(VI) loading capacity in organic phase, nineteenth kinds of New N,N-di-alkyl-amides: N,N-di-hexyl-(3,3-dimethyl)butanamide (DHDMBA), N,N-di-oxyl-(3,3-dimethyl)butanamide (DODMBA), N,N-di-hexyl-(2,2-dimethyl)propanamide (DHDMPA) N,N-di-octyl-(2,2-dimethyl)propanamide (DODMPA), N,N-di-octyl-(2-ethyl)butanamide (DO2EBA), N,N-di-hexyl-(2-ethyl)butanamide (DH2EBA), N-benzyl-N-R{sub 1}-(2-ethyl)hexanamide (R{sub 1}:- C{sub 4}H{sub 9}, -C{sub 6} H{sub 13}, -C{sub 8} H{sub 17}, N-cyclohexyl-N-R{sub 1}-(2- ethyl)hexanamide (R{sub 1}:-C{sub 4}H{sub 9}, -C{sub 6} H{sub 13}, -C{sub 8} H{sub 17}), N-phenyl- N-R{sub 1}-(2-ethyl)hexanamide (R{sub 1}:-C{sub 3}H{sub 9}, -C{sub 4} H{sub 9}, -C{sub 5} H{sub 11}, - C{sub 6}H{sub 13}, -C{sub 8}H{sub 17}, N-(2-ethyl)hexyl-N-Phenyl-octanamide, N-Benzyl- N-Phenyl-(2-ethyl)hexanamide are synthesized. In this paper, our experimental results of new N,N-dialkyl carboxy-amides extraction property of U(VI)/Pu(IV), extraction of macro amount of U(VI), and gamma-ray radiolysis will be summarized. Solvent extraction of U(VI) and Pu (IV) by nineteenth kinds of new N,N-di-alkyl carboxy-amides, macro amount of U(VI) extraction and radiolysis of four compounds were carried out and the following results were obtained: Cyclohexyl group and branched alkyl group combined N,N-di-alk yl carboxy-amides show good separation factors for U/Pu. DH2EBA and DO2EBA show an enough extraction ability for the macro amount of U(VI). The radiation stability of N,N-di-alkyl carboxy-amides (DOHA, DHDMBA and D2EH2EHA) was equal for that of TBP. For adoption of N,N-di-alkyl carboxy-amides for FBR cycle, more information of degradation, extraction of fission products and accurate of the third phase formation boundary are necessary. (authors)
- Research Organization:
- American Nuclear Society, 555 North Kensington Avenue, La Grange Park, IL 60526 (United States)
- OSTI ID:
- 20979676
- Resource Relation:
- Conference: Advanced nuclear fuel cycles and systems (GLOBAL 2007), Boise - Idaho (United States), 9-13 Sep 2007; Other Information: Country of input: France; 14 refs; Related Information: In: Proceedings of GLOBAL 2007 conference on advanced nuclear fuel cycles and systems, 1873 pages.
- Country of Publication:
- United States
- Language:
- English
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