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Title: Development of Alternative Technetium Waste Forms

Abstract

The UREX+1 process is under consideration for the separation of transuranic elements from spent nuclear fuel. The first steps of this process extract the fission product technicium-99 ({sup 99}Tc) into an organic phase containing tributylphosphate together with uranium. Treatment of this stream requires the separation of Tc from U and placement into a suitable waste storage form. A potential candidate waste form involves immobilizing the Tc as an alloy with either excess metallic zirconium or stainless steel. Although Tc-Zr alloys seem to be promising waste forms, alternative materials must be investigated. Innovative studies related to the synthesis and behavior of a different class of Tc materials will increase the scientific knowledge related to development of Tc waste forms. These studies will also provide a better understanding of the behavior of {sup 99}Tc in repository conditions. A literature survey has selected promising alternative waste forms for further study: technetium metallic alloys, nitrides, oxides, sulfides, and pertechnetate salts. The goals of this project are to 1) synthesize and structurally characterize relevant technetium materials that may be considered as waste forms, 2) investigate material behavior in solution under different conditions of temperature, electrochemical potential, and radiation, and 3) predict the long-term behavior ofmore » these materials.« less

Authors:
Publication Date:
Research Org.:
Battelle Energy Alliance, LLC
Sponsoring Org.:
USDOE
OSTI Identifier:
1116528
Report Number(s):
09-821
DOE Contract Number:
AC07-05ID14517
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES

Citation Formats

Czerwinski, Kenneth. Development of Alternative Technetium Waste Forms. United States: N. p., 2013. Web. doi:10.2172/1116528.
Czerwinski, Kenneth. Development of Alternative Technetium Waste Forms. United States. doi:10.2172/1116528.
Czerwinski, Kenneth. Fri . "Development of Alternative Technetium Waste Forms". United States. doi:10.2172/1116528. https://www.osti.gov/servlets/purl/1116528.
@article{osti_1116528,
title = {Development of Alternative Technetium Waste Forms},
author = {Czerwinski, Kenneth},
abstractNote = {The UREX+1 process is under consideration for the separation of transuranic elements from spent nuclear fuel. The first steps of this process extract the fission product technicium-99 ({sup 99}Tc) into an organic phase containing tributylphosphate together with uranium. Treatment of this stream requires the separation of Tc from U and placement into a suitable waste storage form. A potential candidate waste form involves immobilizing the Tc as an alloy with either excess metallic zirconium or stainless steel. Although Tc-Zr alloys seem to be promising waste forms, alternative materials must be investigated. Innovative studies related to the synthesis and behavior of a different class of Tc materials will increase the scientific knowledge related to development of Tc waste forms. These studies will also provide a better understanding of the behavior of {sup 99}Tc in repository conditions. A literature survey has selected promising alternative waste forms for further study: technetium metallic alloys, nitrides, oxides, sulfides, and pertechnetate salts. The goals of this project are to 1) synthesize and structurally characterize relevant technetium materials that may be considered as waste forms, 2) investigate material behavior in solution under different conditions of temperature, electrochemical potential, and radiation, and 3) predict the long-term behavior of these materials.},
doi = {10.2172/1116528},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Sep 13 00:00:00 EDT 2013},
month = {Fri Sep 13 00:00:00 EDT 2013}
}

Technical Report:

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  • An evaluation of available information on eleven alternative solid forms for immobilization of SRP high-level waste has been completed. Based on the assessment of both product and process characteristics, four forms were selected for more detailed evaluation: (1) borosilicate glass made in the reference process, (2) a high-silica glass made from a porous glass matrix, (3) crystalline ceramics such as supercalcine or SYNROC, and (4) ceramics coated with an impervious barrier. The assessment includes a discussion of product and process characteristics for each of the eleven forms, a cross comparison of these characteristics for the forms, and the bases formore » selecting the most promising forms for further study.« less
  • Alternative treatment and disposition options may exist for technetium-99 (99Tc) in secondary liquid waste from the Hanford Direct-Feed Low-Activity Waste (DFLAW) process. One approach includes development of an alternate glass waste form that is suitable for on-site disposition of technetium, including salts and other species recovered by ion exchange or precipitation from the EMF evaporator concentrate. By recovering the Tc content from the stream, and not recycling the treated concentrate, the DFLAW process can potentially be operated in a more efficient manner that lowers the cost to the Department of Energy. This report provides a survey of candidate glass formulationsmore » and glass-making processes that can potentially incorporate technetium at temperatures <700 °C to avoid volatilization. Three candidate technetium feed streams are considered: (1) dilute sodium pertechnetate loaded on a non-elutable ion exchange resin; (2) dilute sodium-bearing aqueous eluent from ion exchange recovery of pertechnetate, or (3) technetium(IV) oxide precipitate containing Sn and Cr solids in an aqueous slurry. From the technical literature, promising candidate glasses are identified based on their processing temperatures and chemical durability data. The suitability and technical risk of three low-temperature glass processing routes (vitrification, encapsulation by sintering into a glass composite material, and sol-gel chemical condensation) for the three waste streams was assessed, based on available low-temperature glass data. For a subset of candidate glasses, their long-term thermodynamic behavior with exposure to water and oxygen was modeled using Geochemist’s Workbench, with and without addition of reducing stannous ion. For further evaluation and development, encapsulation of precipitated TcO2/Sn/Cr in a glass composite material based on lead-free sealing glasses is recommended as a high priority. Vitrification of pertechnetate in aqueous anion exchange eluent solution using a high lead content borate glass, or other low melting glass is also recommended for further evaluation and development. Additional laboratory studies of phase behavior and chemical durability of low-temperature glasses is also recommended to provide risk mitigation if one of the primary development paths proves infeasible. This report is a deliverable for the task “Candidate Low-T Glass Waste Forms for EMF Bottoms On-Site Disposition Alternative Option.”« less
  • This study was undertaken to examine alternate crystalline (ceramic/mineral) and glass waste forms for immobilizing spent salt from the Advanced Fuel Cycle Initiative (AFCI) electrochemical separations process. The AFCI is a program sponsored by U.S. Department of Energy (DOE) to develop and demonstrate a process for recycling spent nuclear fuel (SNF). The electrochemical process is a molten salt process for the reprocessing of spent nuclear fuel in an electrorefiner and generates spent salt that is contaminated with alkali, alkaline earths, and lanthanide fission products (FP) that must either be cleaned of fission products or eventually replaced with new salt tomore » maintain separations efficiency. Currently, these spent salts are mixed with zeolite to form sodalite in a glass-bonded waste form. The focus of this study was to investigate alternate waste forms to immobilize spent salt. On a mole basis, the spent salt is dominated by alkali and Cl with minor amounts of alkaline earth and lanthanides. In the study reported here, we made an effort to explore glass systems that are more compatible with Cl and have not been previously considered for use as waste forms. In addition, alternate methods were explored with the hope of finding a way to produce a sodalite that is more accepting of as many FP present in the spent salt as possible. This study was done to investigate two different options: (1) alternate glass families that incorporate increased concentrations of Cl; and (2) alternate methods to produce a mineral waste form.« less
  • An evaluation panel was organized to aid in the selection of an appropriate solid form for the high level wastes generated by chemical processing of fuels at the Idaho Chemical Processing Plant. This report is a summary of the panel's findings. The panel agrees that the best choice is borosilicate glass because its performance is acceptable, it represents a well developed process and hence it can be implemented expeditiously. In-can melt appears to be the best process at this time, however, development may result in the continuous melt process proving to be better. Stabilized calcine in a matrix, based onmore » the data presently available, may be acceptable. The ratings are based on performance predicted from scanty experimental evidence. If these preliminary observations stand up, the performance of stabilized calcine in fuetap should be satisfactory and the more attractive processing characteristics of this form would prevail. The glass-crystalline and the other crystalline forms have not been developed to a point demonstrating superior performances that would justify their replacing borosilicate glass. System performance improvements great enough to justify more R and D, and probable higher cost, must be also shown. An objective basis to conclude that increased leach resistance will decrease risk to humans does not now exist.« less