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Title: Candidate Low-Temperature Glass Waste Forms for Technetium-99 Recovered from Hanford Effluent Management Facility Evaporator Concentrate

Abstract

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 formulations 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)more » 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

Authors:
 [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM)
OSTI Identifier:
1372804
Report Number(s):
LA-UR-17-25579
DOE Contract Number:
AC52-06NA25396
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; technetium; glass; composite material; vitrification; durability; melting

Citation Formats

Ding, Mei, Tang, Ming, Rim, Jung Ho, and Chamberlin, Rebecca M. Candidate Low-Temperature Glass Waste Forms for Technetium-99 Recovered from Hanford Effluent Management Facility Evaporator Concentrate. United States: N. p., 2017. Web. doi:10.2172/1372804.
Ding, Mei, Tang, Ming, Rim, Jung Ho, & Chamberlin, Rebecca M. Candidate Low-Temperature Glass Waste Forms for Technetium-99 Recovered from Hanford Effluent Management Facility Evaporator Concentrate. United States. doi:10.2172/1372804.
Ding, Mei, Tang, Ming, Rim, Jung Ho, and Chamberlin, Rebecca M. 2017. "Candidate Low-Temperature Glass Waste Forms for Technetium-99 Recovered from Hanford Effluent Management Facility Evaporator Concentrate". United States. doi:10.2172/1372804. https://www.osti.gov/servlets/purl/1372804.
@article{osti_1372804,
title = {Candidate Low-Temperature Glass Waste Forms for Technetium-99 Recovered from Hanford Effluent Management Facility Evaporator Concentrate},
author = {Ding, Mei and Tang, Ming and Rim, Jung Ho and Chamberlin, Rebecca M.},
abstractNote = {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 formulations 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.”},
doi = {10.2172/1372804},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2017,
month = 7
}

Technical Report:

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  • During October 1997, the ETF Evaporator Waste Concentrate Tank No. 2 was discovered to contain a significant accumulation of solid deposits. SRTC performed destructive and nondestructive examination of solid samples from the tank. The results of these tests indicate that the solids contain mixtures of sodium oxalate (65 percent), the sulfide enclathrated sodium aluminosilicate (30 percent), and iron oxide (5 percent).
  • This report describes the results from grout formulation and cementitious waste form qualification testing performed by Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions, LLC (WRPS). These results are part of a screening test that investigates three grout formulations proposed for wide-range treatment of different waste stream compositions expected for the Hanford Effluent Management Facility (EMF) evaporator bottom waste. This work supports the technical development need for alternative disposition paths for the EMF evaporator bottom wastes and future direct feed low-activity waste (DFLAW) operations at the Hanford Site. High-priority activities included simulant production, grout formulation, and cementitious wastemore » form qualification testing. The work contained within this report relates to waste form development and testing, and does not directly support the 2017 Integrated Disposal Facility (IDF) performance assessment (PA). However, this work contains valuable information for use in PA maintenance past FY 2017 and future waste form development efforts. The provided results and data should be used by (1) cementitious waste form scientists to further the understanding of cementitious leach behavior of contaminants of concern (COCs), (2) decision makers interested in off-site waste form disposal, and (3) the U.S. Department of Energy, their Hanford Site contractors and stakeholders as they assess the IDF PA program at the Hanford Site. The results reported help fill existing data gaps, support final selection of a cementitious waste form for the EMF evaporator bottom waste, and improve the technical defensibility of long-term waste form risk estimates.« less
  • The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Melter Off-Gas Condensate, LMOGC) from the off-gas system. The baseline plan for disposition of this stream during full WTP operations is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation and recycled to the LAW vitrification facility. However, during the Direct Feed LAW (DFLAW) scenario, planned disposition of this stream is to evaporate it in a new evaporator in the Effluent Management Facility (EMF) and then return it tomore » the LAW melter. It is important to understand the composition of the effluents from the melter and new evaporator so that the disposition of these streams can be accurately planned and accommodated. Furthermore, alternate disposition of the LMOGC stream would eliminate recycling of problematic components, and would enable less integrated operation of the LAW melter and the Pretreatment Facilities. Alternate disposition would also eliminate this stream from recycling within WTP when it begins operations and would decrease the LAW vitrification mission duration and quantity of glass waste, amongst the other problems such a recycle stream present. This LAW Melter Off-Gas Condensate stream will contain components that are volatile at melter temperatures and are problematic for the glass waste form, such as halides and sulfate. Because this stream will recycle within WTP, these components accumulate in the Melter Condensate stream, exacerbating their impact on the number of LAW glass containers that must be produced. Diverting the stream reduces the halides and sulfate in the recycled Condensate and is a key outcome of this work. This overall program examines the potential treatment and immobilization of this stream to enable alternative disposal. The objective of this task was to formulate and prepare a simulant of the LAW Melter Off-gas Condensate expected during DFLAW operations. That simulant can be used in evaporator testing to predict the composition of the effluents from the Effluent Management Facility (EMF) evaporator to aid in planning for their disposition. This document describes the method used to formulate a simulant of this LAW Melter Off-Gas Condensate stream, which, after pH adjustment, is the feed to the evaporator in the EMF.« less
  • The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Melter Off-Gas Condensate, LMOGC) from the off-gas system. The baseline plan for disposition of this stream during full WTP operations is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation, and recycled to the LAW vitrification facility. However, during the Direct Feed LAW (DFLAW) scenario, planned disposition of this stream is to evaporate it in a new evaporator, in the Effluent Management Facility (EMF), and then return it tomore » the LAW melter. It is important to understand the composition of the effluents from the melter and new evaporator, so that the disposition of these streams can be accurately planned and accommodated. Furthermore, alternate disposition of the LMOGC stream would eliminate recycling of problematic components, and would reduce the need for closely integrated operation of the LAW melter and the Pretreatment Facilities. Long-term implementation of this option after WTP start-up would decrease the LAW vitrification mission duration and quantity of glass waste, amongst the other operational complexities such a recycle stream presents. In order to accurately plan for the disposition path, it is key to experimentally determine the fate of contaminants. To do this, testing is needed to accurately account for the buffering chemistry of the components, determine the achievable evaporation end point, identify insoluble solids that form, and determine the distribution of key regulatory-impacting constituents. The LAW Melter Off-Gas Condensate stream will contain components that are volatile at melter temperatures, have limited solubility in the glass waste form, and represent a materials corrosion concern, such as halides and sulfate. Because this stream will recycle within WTP, these components will accumulate in the Melter Condensate stream, exacerbating their impact on the number of LAW glass containers that must be produced. Diverting the stream reduces the halides and sulfates in the recycled Condensate and is a key outcome of this work. This overall program examines the potential treatment and immobilization of this stream to enable alternative disposal. The objective of this task was to demonstrate evaporation of a simulant of the LAW Melter Off-gas Condensate expected during DFLAW operations, in order to predict the composition of the effluents from the EMF evaporator to aid in planning for their disposition. This document describes the results of that test using the core simulant. This simulant formulation is designated as the “core simulant”; other additives will be included for specific testing, such as volatiles for evaporation or hazardous metals for measuring leaching properties of waste forms. The results indicate that the simulant can easily be concentrated via evaporation. During that the pH adjustment step in simulant preparation, ammonium is quickly converted to ammonia, and most of the ammonia was stripped from the simulated waste and partitioned to the condensate. Additionally, it was found that after concentrating (>12x) and cooling that a small amount of LiF and Na 3(SO 4)F precipitate out of solution. With the exception of ammonia, analysis of the condensate indicated very low to below detectable levels of many of the constituents in the simulant, yielding very high decontamination factors (DF).« less
  • The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Melter Off-Gas Condensate, LMOGC) from the off-gas system. The baseline plan for disposition of this stream during full WTP operations is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation, and recycled to the LAW vitrification facility. However, during the Direct Feed LAW (DFLAW) scenario, planned disposition of this stream involves concentrating the condensate in a new evaporator at the Effluent Management Facility (EMF) and returning it to themore » LAW melter. The LMOGC stream will contain components, e.g. halides and sulfates, that are volatile at melter temperatures, have limited solubility in glass waste forms, and present a material corrosion concern. Because this stream will recycle within WTP, these components are expected to accumulate in the LMOGC stream, exacerbating their impact on the number of LAW glass containers that must be produced. Diverting the stream reduces the halides and sulfates in the glass and is a key objective of this program. In order to determine the disposition path, it is key to experimentally determine the fate of contaminants. To do this, testing is needed to account for the buffering chemistry of the components, determine the achievable evaporation end point, identify insoluble solids that form, determine the formation and distribution of key regulatoryimpacting constituents, and generate an aqueous stream that can be used in testing of the subsequent immobilization step. This overall program examines the potential treatment and immobilization of the LMOGC stream to enable alternative disposal. The objective of this task was to (1) prepare a simulant of the LAW Melter Off-gas Condensate expected during DFLAW operations, (2) demonstrate evaporation in order to predict the final composition of the effluents from the EMF evaporator to aid in planning for their disposition, and (3) generate concentrated evaporator bottoms for use in immobilization testing.« less