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Title: Bench scale experiments for the remediation of Hanford Waste Treatment Plant low activity waste melter off-gas condensate

Abstract

The Low Activity Waste (LAW) vitrification facility at the Hanford Waste Treatment and Immobilization Plant (WTP) will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The plan for disposition of this stream during baseline 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 again. The primary reason to recycle this stream is so that the semi-volatile 99Tc isotope eventually becomes incorporated into the glass. This stream also contains non-radioactive salt components that are problematic in the melter, so diversion of this stream to another process would eliminate recycling of these salts and would enable simplified operation of the LAW melter and the Pretreatment Facilities. This diversion from recycling this stream within WTP would have the effect of decreasing the LAW vitrification mission duration and quantity of glass waste. The concept being tested here involves removing the 99Tc so that the decontaminated aqueous stream, with the problematic salts, can be disposed elsewhere.

Authors:
 [1];  [1];  [1]
+ Show Author Affiliations
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1377029
Report Number(s):
SRNL-STI-2017-00322
TRN: US1801139
DOE Contract Number:
AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; GAS CONDENSATES; WASTE PROCESSING; WASTES; VITRIFICATION; OFF-GAS SYSTEMS; decontamination; technetium; stannous chloride; chromium

Citation Formats

Taylor-Pashow, Kathryn M.L., Poirier, Michael, and McCabe, Daniel J. Bench scale experiments for the remediation of Hanford Waste Treatment Plant low activity waste melter off-gas condensate. United States: N. p., 2017. Web. doi:10.2172/1377029.
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Taylor-Pashow, Kathryn M.L., Poirier, Michael, & McCabe, Daniel J. Bench scale experiments for the remediation of Hanford Waste Treatment Plant low activity waste melter off-gas condensate. United States. doi:10.2172/1377029.
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Taylor-Pashow, Kathryn M.L., Poirier, Michael, and McCabe, Daniel J. Fri . "Bench scale experiments for the remediation of Hanford Waste Treatment Plant low activity waste melter off-gas condensate". United States. doi:10.2172/1377029. https://www.osti.gov/servlets/purl/1377029.
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@article{osti_1377029,
title = {Bench scale experiments for the remediation of Hanford Waste Treatment Plant low activity waste melter off-gas condensate},
author = {Taylor-Pashow, Kathryn M.L. and Poirier, Michael and McCabe, Daniel J.},
abstractNote = {The Low Activity Waste (LAW) vitrification facility at the Hanford Waste Treatment and Immobilization Plant (WTP) will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The plan for disposition of this stream during baseline 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 again. The primary reason to recycle this stream is so that the semi-volatile 99Tc isotope eventually becomes incorporated into the glass. This stream also contains non-radioactive salt components that are problematic in the melter, so diversion of this stream to another process would eliminate recycling of these salts and would enable simplified operation of the LAW melter and the Pretreatment Facilities. This diversion from recycling this stream within WTP would have the effect of decreasing the LAW vitrification mission duration and quantity of glass waste. The concept being tested here involves removing the 99Tc so that the decontaminated aqueous stream, with the problematic salts, can be disposed elsewhere.},
doi = {10.2172/1377029},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Aug 11 00:00:00 EDT 2017},
month = {Fri Aug 11 00:00:00 EDT 2017}
}
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DOI:  10.2172/1377029
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  • ;
    The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The baseline plan for disposition of this stream 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 again. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable simplified operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also decrease the LAW vitrificationmore » mission duration and quantity of glass waste.« less

  • ;
    The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The baseline plan for disposition of this stream 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. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable less integrated operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also decrease the LAW vitrificationmore » mission duration and quantity of glass waste.« less

  • ; ;
    The Low Activity Waste (LAW) vitrification facility at the Hanford Waste Treatment and Immobilization Plant (WTP) will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the offgas system. The plan for disposition of this stream during baseline 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 again. The primary reason to recycle this stream is so that the semi-volatile 99Tc isotope eventually becomes incorporated into the glass. This stream also contains non-radioactive salt components that are problematic in the melter,more » so diversion of this stream to another process would eliminate recycling of these salts and would enable simplified operation of the LAW melter and the Pretreatment Facilities. This diversion from recycling this stream within WTP would have the effect of decreasing the LAW vitrification mission duration and quantity of glass waste. The concept being tested here involves removing the 99Tc so that the decontaminated aqueous stream, with the problematic salts, can be disposed elsewhere.« less

  • ; ; ; ...
    The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The baseline plan for disposition of this stream 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 again. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable de-coupled operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also decrease the LAW vitrificationmore » mission duration and quantity of glass waste. This LAW Off-Gas Condensate stream contains components that are volatile at melter temperatures and are problematic for the glass waste form. Because this stream recycles within WTP, these components accumulate in the Condensate stream, exacerbating their impact on the number of LAW glass containers that must be produced. Approximately 32% of the sodium in Supplemental LAW comes from glass formers used to make the extra glass to dilute the halides to acceptable concentrations in the LAW glass, and diverting the stream reduces the halides in the recycled Condensate and is a key outcome of this work. Additionally, under possible scenarios where the LAW vitrification facility commences operation prior to the WTP Pretreatment facility, identifying a disposition path becomes vitally important. This task seeks to examine the potential treatment of this stream to remove radionuclides and subsequently disposition the decontaminated stream elsewhere, such as the Effluent Treatment Facility (ETF), for example. The treatment process envisioned is very similar to that used for the Actinide Removal Process (ARP) that has been operating for years at the Savannah River Site (SRS), and focuses on using mature radionuclide removal technologies that are also compatible with longterm tank storage and immobilization methods. For this new application, testing is needed to demonstrate acceptable treatment sorbents and precipitating agents and measure decontamination factors for additional radionuclides in this unique waste stream. The origin of this LAW Off-Gas Condensate stream will be the liquids from the Submerged Bed Scrubber (SBS) and the Wet Electrostatic Precipitator (WESP) from the LAW melter off-gas system. The stream is expected to be a dilute salt solution with near neutral pH, and will likely contain some insoluble solids from melter carryover. The soluble components are expected to be mostly sodium and ammonium salts of nitrate, chloride, and fluoride. This stream has not been generated yet and will not be available until the WTP begins operation, but a simulant has been produced based on models, calculations, and comparison with pilot-scale tests. One of the radionuclides that is volatile and expected to be in high concentration in this LAW Off-Gas Condensate stream is Technetium-99 ( 99Tc). Technetium will not be removed from the aqueous waste in the Hanford WTP, and will primarily end up immobilized in the LAW glass by repeated recycle of the off-gas condensate into the LAW melter. Other radionuclides that are also expected to be in appreciable concentration in the LAW Off-Gas Condensate are 129I, 90Sr, 137Cs, and {sup 241}Am. This report discusses results of preliminary radionuclide decontamination testing of the simulant. Testing examined use of Monosodium Titanate (MST) to remove 90Sr and actinides, inorganic reducing agents for 99Tc, and zeolites for 137Cs. Test results indicate that excellent removal of 99Tc was achieved using Sn(II)Cl 2 as a reductant, coupled with sorption onto hydroxyapatite, even in the presence of air and at room temperature. This process was very effective at neutral pH, with a Decontamination Factor (DF) >577 in two hours. It was less effective at alkaline pH. Conversely, removal of the cesium was more effective at alkaline pH, with a DF of 17.9. As anticipated, ammonium ion probably interfered with the Ionsiv®a IE-95 zeolite uptake of 137Cs. Although this DF of 137Cs was moderate, additional testing is expected to identify more effective conditions. Similarly, Monosodium Titanate (MST) was more effective at alkaline pH at removing Sr, Pu, and U, with a DF of 319, 11.6, and 10.5, respectively, within 24 hours. Actually, the Ionsiv® IE-95, which was targeting removal of Cs, was also moderately effective for Sr, and highly effective for Pu and U at alkaline pH. The only deleterious effect observed was that the chromium co-precipitates with the {sup 99}Tc during the SnCl 2 reduction. This effect was anticipated, and would have to be considered when managing disposition paths of this stream. Results of this separation testing indicate that sorption/precipitation was a viable concept and has the potential to decontaminate the stream. All radionuclides were at least partially removed by one or more of the materials tested. Based on the results, a possible treatment scenario could involve the use of a reductive precipitation agent (SnCl 2) and sorbent at neutral pH to remove the Tc, followed by pH adjustment and the addition of zeolite (Ionsiv® IE-95) to remove the Cs, Sr, and actinides. Addition of MST to remove Sr and actinides may not be needed. Since this was an initial phase of testing, additional tasks to improve separation methods were expected to be identified. Primarily, further testing is needed to identify the conditions for the decontamination process. Once these conditions are established, follow-on tasks likely include evaluation and testing of applicable solid-liquid separation technologies, slurry rheology measurements, composition variability testing and evaluations, corrosion and erosion testing, slurry storage and immobilization investigations, and decontaminated LAW Off-Gas Condensate evaporation and solidification.« less

  • ; ; ; ...
    The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream, LAW Off-Gas Condensate, from the off-gas system. The baseline plan for disposition of this stream 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 again. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable de-coupled operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also decrease the LAW vitrificationmore » mission duration and quantity of canistered glass waste forms. This LAW Off-Gas Condensate stream contains components that are volatile at melter temperatures and are problematic for the glass waste form. Because this stream recycles within WTP, these components accumulate in the Condensate stream, exacerbating their impact on the number of LAW glass containers that must be produced. Approximately 32% of the sodium in Supplemental LAW comes from glass formers used to make the extra glass to dilute the halides to be within acceptable concentration ranges in the LAW glass. Diverting the stream reduces the halides in the recycled Condensate and is a key outcome of this work. Additionally, under possible scenarios where the LAW vitrification facility commences operation prior to the WTP Pretreatment facility, identifying a disposition path becomes vitally important. This task examines the impact of potential future disposition of this stream in the Hanford tank farms, and investigates auxiliary evaporation to enable another disposition path. Unless an auxiliary evaporator is used, returning the stream to the tank farms would require evaporation in the 242-A evaporator. This stream is expected to be unusual because it will be very high in corrosive species that are volatile in the melter (chloride, fluoride, sulfur), will have high ammonia, and will contain carryover particulates of glass-former chemicals. These species have potential to cause corrosion of tanks and equipment, precipitation of solids, release of ammonia gas vapors, and scale in the tank farm evaporator. Routing this stream to the tank farms does not permanently divert it from recycling into the WTP, only temporarily stores it prior to reprocessing. Testing is normally performed to demonstrate acceptable conditions and limits for these compounds in wastes sent to the tank farms. The primary parameter of this phase of the test program was measuring the formation of solids during evaporation in order to assess the compatibility of the stream with the evaporator and transfer and storage equipment. The origin of this LAW Off-Gas Condensate stream will be the liquids from the Submerged Bed Scrubber (SBS) and the Wet Electrostatic Precipitator (WESP) from the LAW facility melter offgas system. The stream is expected to be a dilute salt solution with near neutral pH, and will likely contain some insoluble solids from melter carryover. The soluble components are expected to be mostly sodium and ammonium salts of nitrate, chloride, and fluoride. This stream has not been generated yet, and, thus, the composition will not be available until the WTP begins operation, but a simulant has been produced based on models, calculations, and comparison with pilot-scale tests. This report discusses results of evaporation testing of the simulant. Two conditions were tested, one with the simulant at near neutral pH, and a second at alkaline pH. The neutral pH test is comparable to the conditions in the Hanford Effluent Treatment Facility (ETF) evaporator, although that evaporator operates at near atmospheric pressure and tests were done under vacuum. For the alkaline test, the target pH was based on the tank farm corrosion control program requirements, and the test protocol and equipment was comparable to that used for routine evaluation of feed compatibility studies for the 242-A evaporator. One of the radionuclides that is volatile in the melter and expected to be in high concentration in this LAW Off-Gas Condensate stream is Technetium-99 (99Tc). Technetium will not be removed from the aqueous waste in the Hanford WTP, and will primarily end up immobilized in the LAW glass by repeated recycle of the off-gas condensate into the LAW melter. Other radionuclides that are also expected to be in appreciable concentrations in the LAW Off-Gas Condensate are 129I, 90Sr, 137Cs, and 241Am. The concentrations of these radionuclides in this stream will be much lower than in the LAW, but they will still be higher than limits for some of the other disposition pathways currently available. At this time, these scoping tests did not evaluate the partitioning of the radionuclides to the evaporator condensate, since ample data are available separately from other experience in the DOE complex. Results from the evaporation testing show that the neutral SBS simulant first forms turbidity at ~7.5X concentration, while the alkaline-adjusted simulant became turbid at ~3X concentration. The major solid in both cases was Kogarkoite, Na3FSO4. Sodium and lithium fluorides were also detected. Minimal solids were formed in the evaporator bottoms until a substantial fraction of liquid was removed, indicating that evaporation could minimize storage volume issues. Achievable concentration factors without significant insoluble solids were 17X at alkaline pH, and 23X at neutral pH. In both runs, significant ammonia carried over and was captured in the condenser with the water condensate. Results also indicate that with low insoluble solids formation in the initial testing at neutral pH, the use of Reverse Osmosis is a potential alternate method for concentrating the solution, although an evaluation is needed to identify equipment that can tolerate insoluble solids. Most of the ammonia remains in the evaporator bottoms during the neutral pH evaporation, but partitions to the condensate during alkaline evaporation. Disposition of both streams needs to consider the management of ammonia vapor and its release. Since this is an initial phase of testing, additional tasks related to evaporation methods are expected to be identified for development. These tasks likely include evaluation and testing of composition variability testing and evaluations, corrosion and erosion testing, slurry storage and immobilization investigations, and evaporator condensate disposition.« less