Radiation Stability of Benzyl Tributyl Ammonium Chloride towards Technetium-99 Extraction - 13016
- Idaho National Laboratory, 2525 Fremont Street, Idaho Falls, ID 83402 (United States)
- University of Nevada - Las Vegas, Harry Reid Center, 4505 S. Maryland Pkwy, Box 4009, Las Vegas, NV 89154-4009 (United States)
- CIEMAT, Avda Complutense, 40, 28040- Madrid (Spain)
A closed nuclear fuel cycle combining new separation technologies along with generation III and generation IV reactors is a promising way to achieve a sustainable energy supply. But it is important to keep in mind that future recycling processes of used nuclear fuel (UNF) must minimize wastes, improve partitioning processes, and integrate waste considerations into processes. New separation processes are being developed worldwide to complement the actual industrialized PUREX process which selectively separates U(VI) and Pu(IV) from the raffinate. As an example, the UREX process has been developed in the United States to co-extract hexavalent uranium (U) and hepta-valent technetium (Tc) by tri-n-butyl phosphate (TBP). Tc-99 is recognized to be one of the most abundant, long-lived radio-toxic isotopes in UNF (half-life, t{sub 1/2} = 2.13 x 10{sup 5} years), and as such, is targeted in UNF separation strategies for isolation and encapsulation in solid waste-forms for final disposal in a nuclear waste repository. Immobilization of Tc-99 by a durable solid waste-form is a challenge, and its fate in new advanced technology processes is of importance. It is essential to be able to quantify and locate 1) its occurrence in any new developed flowsheets, 2) its chemical form in the individual phases of a process, 3) its potential quantitative transfer in any waste streams, and consequently, 4) its quantitative separation for either potential transmutation to Ru-100 or isolation and encapsulation in solid waste-forms for ultimate disposal. In addition, as a result of an U(VI)-Tc(VII) co-extraction in a UREX-based process, Tc(VII) could be found in low level waste (LLW) streams. There is a need for the development of new extraction systems that would selectively extract Tc-99 from LLW streams and concentrate it for feed into high level waste (HLW) for either Tc-99 immobilization in metallic waste-forms (Tc-Zr alloys), and/or borosilicate-based waste glass. Studies have been launched to investigate the suitability of new macro-compounds such as crown-ethers, aza-crown ethers, quaternary ammonium salts, and resorcin-arenes for the selective extraction of Tc-99 from nitric acid solutions. The selectivity of the ligand is important in evaluating potential separation processes and also the radiation stability of the molecule is essential for minimization of waste and radiolysis products. In this paper, we are reporting the extraction of TcO{sub 4}{sup -} by benzyl tributyl ammonium chloride (BTBA). Experimental efforts were focused on determining the best extraction conditions by varying the ligand's matrix conditions and concentration, as well as varying the organic phase composition (i.e. diluent variation). Furthermore, the ligand has been investigated for radiation stability. The ?-irradiation was performed on the neat organic phases containing the ligand at different absorbed doses to a maximum of 200 kGy using an external Co-60 source. Post-irradiation solvent extraction measurements will be discussed. (authors)
- Research Organization:
- WM Symposia, 1628 E. Southern Avenue, Suite 9-332, Tempe, AZ 85282 (United States)
- OSTI ID:
- 22224826
- Report Number(s):
- INIS-US-13-WM-13016; TRN: US14V0259045781
- Resource Relation:
- Conference: WM2013: Waste Management Conference: International collaboration and continuous improvement, Phoenix, AZ (United States), 24-28 Feb 2013; Other Information: Country of input: France; 17 refs.
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
ABSORBED RADIATION DOSES
AMMONIUM CHLORIDES
BORON SILICATES
COBALT 60
CROWN ETHERS
HIGH-LEVEL RADIOACTIVE WASTES
LIGANDS
LOW-LEVEL RADIOACTIVE WASTES
NUCLEAR FUELS
PUREX PROCESS
RESORCINOL
RUTHENIUM 100
SOLID WASTES
SOLVENT EXTRACTION
STABILITY
TBP
TECHNETIUM
TECHNETIUM 99
URANIUM
WASTE FORMS