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DOE OSTI2022

Preliminary Enhanced LAW Glass Formulation Algorithm

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DOE OSTI2023

Product Consistency Test Results for the LAW HPVR Glasses

This report summarizes the chemical analysis of Product Consistency Test (PCT) leachates received from Pacific Northwest National Laboratory (PNNL). The leachates are from a series of simulated nuclear waste glasses designated Low-Activity Waste High PCT and VHT Response (LAW HPVR) glasses that were designed and fabricated at PNNL. The glasses included both quenched and canister centerline cooled glasses. The reported data will be used in the development, validation, and implementation of enhanced property/composition models for waste glass vitrification at Hanford. The elemental release for the study glasses is reported as normalized concentration (NC i ). NC i of several elements was computed for both the target and measured glass compositions, which were similar, resulting in no significant differences when computing the NC i values. The majority of the glasses exhibited NC B , NC Na , and NC Si values that were greater than the Hanford Tank Waste Treatment Plant (WTP) low-activity waste constraint of 4 g/L. Several blank solutions included with the study glasses had K, Na, and Si concentrations above the analytical detection limit. Additionally, several of the reference glasses that were included with the study glasses had Na concentrations that were higher than expected. The unexpected analyte concentrations in the reference glass and blank solutions were insignificant with respect to the reported NC i values, and are noted for completeness and their experimental relevance.

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DOE OSTI2023

Low Activity Waste Tuning Feed Material Testing VSL-18R4350-1 (Final Report)

High level waste (HLW) from the Hanford tank farms will be retrieved and transferred to the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The waste will be pretreated to separate the soluble chemical salts (mostly sodium nitrate/nitrite and sodium hydroxide) from the bulk of the radioactive materials. This decontaminated salt solution is the low activity waste (LAW) stream which constitutes most of the total waste volume. The remaining HLW contains most of the radioactive materials but a fraction of the volume. Each of these waste streams is directed to an independent processing facility where the waste is mixed with glass forming chemicals (mostly silica and borax or boric acid) and fed into the melters for stabilization by conversion into glass. The molten glass is poured into stainless steel containers to produce packages for disposal: local shallow burial for the LAW containers and a future geologic repository for the HLW containers. The LAW facility melters produce significant quantities of NOx-laden off-gas that require abatement in accordance with 10 CFR 830 and air emission requirements. The NOx emissions also pose a safety risk. The LAW facility commissioning sequence requires that the melters be operated and process control loops tuned prior to introducing waste or waste feed materials that produce NOx. Therefore, a temporary or permanent system architecture is needed that provides a feed supply to the melters for the purpose of melter testing and off-gas tuning that does not result in the production of significantly hazardous off-gas products.

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DOE OSTI2023

Product Consistency Test Results for the LAW ML1 Glasses

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DOE OSTI2023

Preliminary Enhanced LAW Glass Formulation Algorithm

This report summarizes the Preliminary Enhanced Low-Activity Waste Glass Formulation Algorithm (GFA), its background information, and the calculations it performs. The Preliminary Enhanced Low-Activity Waste GFA is a tool developed in MATLAB to formulate glass for a given waste composition while attempting to maximize waste loading. It is intended for use at the Waste Treatment and Immobilization Plant, where nuclear waste will be vitrified into glass. The formulated glass is required to satisfy several processing and product quality constraints. In addition, calculations must account for associated uncertainties in constraint prediction and measurement. The GFA adheres to Pacific Northwest National Laboratory nuclear quality assurance procedures and has been validated and verified. In this second revision to the report, two constraints: the lithium and zirconia target constraints were amended to Table 3.1 and programmed into the algorithm. Additionally, three sections were added. Section 3.2.1 includes the Enhanced LAW Correlation Rules, an addition to the glass optimality criteria. Section 4.0 discusses a stepped process approach taken to ensure the algorithm can adequately react to differences between its recommended output and the actual measurements and transfers made during plant operation, and calculation of specific radionuclide concentrations. Section 5.2 describes changes to the user interaction with the algorithm program including the addition of a graphical user interface and compilation of the software.

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DOE OSTI2023

Cesium Removal from SY-101 Tank Waste Using Crystalline Silicotitanate

The newly operational Tank Side Cesium Removal (TSCR) system removes radioactive cesium-137 ( 137 Cs) and solids from tank waste supernate in the 200 east area of the Hanford site. Efforts to expand the removal capabilities to the 200 west area are underway by a system anticipated to be called the West Area Risk Management (WARM) system. Laboratory-scale ion exchange processing using expected WARM unit operations were conducted to contribute toward Washington River Protection Solutions (WRPS) establishing accurate process flowsheets for the individual feed campaigns planned for the west area supernate pretreatment. This report describes the small-scale ion exchange testing with 8.0 L of filtered supernate from tank 241-SY-101 (referred to as SY-101) at 16 °C (62 °F) to demonstrate processing conditions that would be prototypic of what the WARM system may experience. One of the waste acceptance criteria (WAC) for the Waste Treatment Plant (WTP) Low-Activity Waste Facility is that the waste must contain less than 3.18×10 -5 Ci 137 Cs per mole of Na. For the SY-101 tank waste to meet this criterion, only 0.44% of the influent 137 Cs concentration may be delivered to the WTP; this requires a Cs decontamination factor of 227. Testing with SY-101 matched current TSCR prototypic operations where a lead-lag configuration is used until the lag column reached the WAC limit. Neither the lead nor lag columns reached the WAC, so a polish column was never utilized during this test. Feed was processed at 1.9 bed volumes (BVs) per hour; the flowrate, in terms of contact time with the crystalline silicotitate (CST) bed, matched the current flowrate at TSCR (an expected flowrate to be used at WARM). The lead column only reached 0.09% Cs breakthrough after processing ~1363 BVs of feed. Cesium breakthrough from the lag column was not observed during the entire processing. Table S.1 and Figure S.1 summarize the observed column performance and relevant Cs loading characteristics. Table S.1 and Figure S.1 also summarize the measured SY-101 Cs load performance.

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DOE OSTI2020

DOE Hanford Tank Side Cesium Removal System (TSCR) Update: Fabrication and Factory Acceptance Testing - 20300

The Tank Side Cesium Removal (TSCR) System is a modular, quickly-deployable, and passively safe system for efficiently removing solids and cesium from alkaline liquid waste raffinate created by fuel processing on the Hanford site. This paper provides an overview of the project with particular emphasis on completion of fabrication and factory acceptance testing (FAT). All TSCR System components are inside three enclosures known as the Process Enclosure, Ancillary Enclosure, and Control Enclosure. The Process Enclosure is seismic design category II (SDC-II) and built to withstand the rigors of transportation and lifting, high winds, volcanic ash fall, and heavy precipitation (snow) over a temperature range of -25 to 115 deg. F. The Process Enclosure and Control Enclosure were fabricated in AVANTech's Columbia, SC facility, while the Ancillary Enclosure was fabricated in AVANTech's Richland, WA facility. The design and preliminary documented safety analysis were completed in December 2019, with all work being performed in accordance with ASME NQA-1 quality assurance requirements. The Process Enclosure, Ion Exchange Columns (IXCs), and several other TSCR components have a nuclear safety function and are designated as safety significant structures, systems, and components (SS-SSCs). The NQA-1 Commercial Grade Dedication (CGD) process was used to identify critical characteristics in order to accept materials and items used for fabrication of several safety significant TSCR components. This paper also addresses unique aspects and challenges of implementing CGD in DOE facilities and systems. After fabrication and preliminary testing, the Process and Control Enclosures were shipped to AVANTech's Richland facility where the complete TSCR System was setup and connected in a represented layout and configuration that will be used on the Hanford site. Test tanks and pumps were put in place and connected to the TSCR Process Enclosure in a manner that mimicked interfacing Double Shell Tanks in the 241-AP Tank Farm. The TSCR System was then tested/operated under conditions equivalent to those planned for onsite operation. Testing was separated into five separate phases as defined below: - Phase 1: Confirmation of TSCR System readiness for the FAT; - Phase 2: Verification of TSCR System operation under standard conditions; - Phase 3: Demonstration of TSCR System operation under non-standard conditions; - Phase 4: Demonstration of ion exchange media removal from an IXC; and - Phase 5: Completion of TSCR System lift plans and site mobilization. The Hanford Tank Operations Contractor, Washington River Protection Solutions (WRPS), participated in all phases of testing. Testing at AVANTech's Richland Facility allowed WRPS personnel to familiarize themselves with TSCR operations in a radiologically clean facility prior to onsite mobilization. Engineering and operations personnel gained valuable experience that allowed them to better refine onsite operational protocols and procedures - including handling and movement of IXCs with a forklift. This paper describes the technologies used by the TSCR System as well as how these technologies are deployed and operated to advance the Hanford mission of safely, efficiently, and effectively treating tank waste. It also provides detailed information on fabrication and FAT, including operational data from simulated tank waste runs. A project schedule for WRPS' planned construction acceptance testing, operational acceptance testing, and actual tank waste treatment is provided. This presentation should be of great interest to parties responsible for the design, testing, and mobilization of modular NQA-1 technologies for the treatment of raffinate and similar liquid wastes containing high concentrations of radioactive cesium. (authors)

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DOE OSTI2022

The Effects of Mixing Multi-Component HLW Glasses on Spinel Crystal Size

The Hanford Waste Treatment and Immobilization Plant will vitrify radioactive waste into borosilicate glass. The high-level waste (HLW) glass formulations are constrained by processing and property requirements, including restrictions aimed at avoiding detrimental impacts of spinel crystallization in the melter. To understand the impact of glass chemistry on crystallization, two HLW glasses precipitating small (?5 µm) spinel crystals were individually mixed with a glass that precipitated large (?45 µm) spinel crystals in ratios of 25, 50, and 75 wt%. The size of spinel crystals in the mixed glasses varied from 5 to 20 µm. Small crystal size was attributed to: (1) high concentrations of nuclei due to the presence of ruthenium oxide and (2) chromium oxide aiding high rates of nucleation. Results indicate that the spinel crystal size can be controlled using chromium oxide and/or noble metal concentrations in the melt, even in complex mixtures like HLW glasses. Small crystals tend to settle slowly, so they are acceptable in the melter without a risk of failure. Allowing higher concentrations of spinel-forming waste components in the waste glass enables glass compositions with higher waste loading, thus increasing plant operational flexibility. An additional benefit to the presence of chromium oxide in the glass composition is the potential for the oxide to protect melter walls against corrosion.

Lonergan, Charmayne E.↗

DOE OSTI2022

Product Consistency Test Results for the Environmental Management Headquarters (EMHQ) Low-Activity Waste (LAW) Glasses

This report provides the results of the Product Consistency Test leachates from the Environmental Management Headquarters Low-Activity Waste glasses, a series of simulated nuclear waste glasses designed and fabricated at the Pacific Northwest National Laboratory. The series included quenched versions of the glasses. These data will be used in the development, validation, and implementation of enhanced property/composition models for waste glass vitrification at Hanford. The measured concentrations of the analytes in the test blank samples were below detection limits. The measured concentrations of B, Li, Na, and Si in the Approved Reference Material-1 samples included with the Product Consistency Tests fell within control chart values indicating proper test performance. The measured glass compositions for the study glasses were close to target values: therefore, little difference was seen when evaluating the normalized values using the targeted or measured glass compositions. The $NC_B$, $NC_{Na}$, and $NC_{Si}$ values were less than the Hanford Tank Waste Treatment and Immobilization Plant low-activity waste constraint of 4 g/L for all glasses.

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DOE OSTI2020

Mercury Speciation During Vitrification of LAW

n this work, laboratory and engineering-scale tests were conducted that mimic the reactive environment of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) low activity waste (LAW) melter and off-gas system in order to assess the speciation of mercury at select points in the processing system. The experimental protocols, test equipment, feed materials used, and rationale for testing are detailed in the Test Plan for this work. Particular attention was paid to the amount and speciation of mercury in submerged bed scrubber (SBS) solutions, which are intended to be recycled back to the melter feed at the WTP. Results are presented from detailed mercury analysis of these solutions using Environmental Protection Agency (EPA) Method 1630 and modifications to this method for dimethyl mercury and methyl mercury as well as EPA Method 1631 and modifications to this method for total, dissolved, elemental, suspended, and ionic mercury. Testing was conducted in two separate sets of experiments: (1) One set of tests (crucible-scale furnace tests) that involved heating small batches of mercury-spiked melter feed in crucibles to determine the amount of mercury retained in the glass and the species of mercury in the exhaust gases; (2) A second set of tests (DM10 melter tests) was planned that involved creating LAW melter plenum gas compositions using the DM10 melter system, injecting mercury into the off-gas stream, and passing that stream though a reactor that simulates various plenum gas conditions. Operational issues led to the need to use one of the VSL DM100 melters in place of the planned DM10 melter for these tests. The speciation of mercury after exposure to those conditions was monitored. In both sets of tests, the exhaust gases were run through a scrubber that was intended to mimic the LAW SBS in order to determine how much of the mercury exiting the melter would be retained in the primary off-gas system fluids and in what form. After passing through the SBS, the exhaust stream was analyzed to determine particulate, ionic, elemental, and total mercury passing downstream of the SBS. In tests employing gases derived from the DM100 melter that were spiked with elemental mercury, the processing system provided gas temperatures and residence times that are representative of the WTP LAW vitrification system in order to assess the effect of those conditions on mercury speciation. The Decontamination Factor (DF) across the system in the tests with mercury-spiked DM100 melter exhaust was determined using the analytical data from EPA Method 30B (Fluegas Adsorption Mercury Speciation (FAMS TM )) exhaust samples and the amount of mercury detected in the SBS solutions. Mercury species used in melter feed crucible scale tests were divalent (chloride and iodide), monovalent (chloride and fluoride), and elemental mercury. Individual tests included only a single form of mercury in the feed. The results for total mercury mass balances in the crucible tests are also presented.

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DOE OSTI2025

Summary of DM1200 WESP History and Performance

The principal objective of this report was to summarize the testing experience on the DM1200 WESP. Further objectives were to provide descriptions of the history of all modifications and maintenance, methods of operation, problems and unit failures, and performance while processing a variety of feeds, and while employing a variety of operating methods, and to provide comparisons to the Hanford Tank Waste Treatment and Immobilization Plant (WTP) high level waste (HLW) and low activity waste (LAW) WESP designs.

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DOE OSTI2025

Summary of DM1200 SBS history and performance

The principal objective of this report is to summarize the testing experience on the DM1200 SBS. Further objectives are to provide descriptions of the history of all modifications and maintenance, methods of operation, problems and unit failures, and performance while processing a variety of feeds, and while employing a variety of operating methods, and to provide comparisons to the Hanford Tank Waste Treatment and Immobilization Plant (WTP) High Level Waste (HLW) and Low Activity Waste (LAW) Submerged Bed Scrubber (SBS) designs.

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DOE OSTI2020

Product Consistency Test Results for the High-Chromium Matrix Glasses

This report provides chemical analysis of a series of Product Consistency Test (PCT) leachates from simulated nuclear waste glasses. The resulting data will be used in the development of improved property/composition models. For some of the glass leachates, minor scatter among the triplicate values of some analytes was observed. For other leachates, there were more significant differences among the triplicate values. A review of the PCT data noted that there was little difference between the normalized values on the basis of targeted or measured glass composition. Several of the study glasses, both quenched and canister centerline cooled, have NC i values that are greater than the Hanford Tank Waste Treatment and Immobilization Plant immobilized low-activity waste constraint of 4 g/L for B, Na, and Si. For many of the study glasses, heat treatment had only a marginal impact on the NC i values. The samples of the Environmental Assessment (EA) reference glass included with each PCT set had inconsistent NC i values, although some degree of variation in NC i values for the EA glass is typical. The release rates for boron and sodium were highly correlated for the study glasses, while for the other analytes, less correlation was observed.

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DOE OSTI2024

Off-line Tests of the DM1200 Thermal Catalytic Oxidation (TCO) Unit (Final Report)

The River Protection Project-Waste Treatment Plant (RPP-WTP) Low-Activity Waste (LAW) and High-Level Waste (HLW) feed streams are listed for a variety of hazardous organic compounds. The permitting basis for the WTP systems may necessitate the demonstration of minimum Destruction/Removal Efficiencies (DREs) of such species from any released emissions of up to 99.99%. Results from a previous study on the fate of hazardous organics in the melter itself indicated, not only that DREs for selected test compounds approached 99.99% only at extreme melter conditions, but also that organic compounds not originally present in the feed were actually produced in the melter, In order to ensure that the required DREs for hazardous organics are met, Thermal Catalytic Oxidation (TCO) units were therefore added to both the HLW and LAW off-gas treatment systems, The extent to which these species can be destroyed or removed in the TCO units is therefore an important issue in the design and permitting of the LAW and HLW off-gas treatment systems. A further consideration is that it would be desirable, if possible, to be able to achieve all of the required DRE across the TCO alone. If that is not the case, the DRE would be distributed across several unit operations, which may then become subject to additional operational constraints that may reduce process flexibility. Compliance with the DRE requirements on the basis of the TCO unit alone is also an approach that lends itself to periodic confirmation during operations, since the TCO is located at the back-end of the off-gas treatment system where radioactivity levels are lowest.

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DOE OSTI2020

Product consistency test results for the LAW Phase 4 gases

In this report, the Savannah River National Laboratory provides chemical analysis of Product Consistency Test (PCT) leachates from a series of simulated nuclear waste glasses fabricated at the Pacific Northwest National Laboratory (PNNL). The series included quenched and canister-centerline cooled (CCC) versions of the glasses. The resulting data will be used in the development of enhanced property/composition models for waste vitrification at Hanford. For some of the glass leachates, minor scatter among the triplicate values of some analytes were observed. For other leachates, there were more significant differences among the triplicate values. A review of the PCT data noted that there was little difference between the normalized values based on targeted or measured glass composition. Several of the study glasses have normalized concentration of element “i” (NCi) values that are greater than the Hanford Tank Waste Treatment and Immobilization Plant immobilized low-activity waste constraint of 4 g/L for boron (B), sodium (Na), and silicon (Si). The results of these glasses will help ensure the ability of advanced glass performance models to appropriately predict acceptable compositions. For the study glasses with NCi values exceeding 4 g/L, the CCC heat treatment samples had generally lower NCi values than quenched samples. The samples of the Environmental Assessment (EA) reference glass included with each PCT set had generally consistent NCi values. The release rates for boron (B), potassium (K), lithium (Li), sodium (Na), and silicon (Si) were highly correlated for the study glasses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Spent Crystalline Silicotitanate Storage Study—Post AP-105DF Processing

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DOE OSTI2020

Product Consistency Test Results for the LXC-Series Glasses

This report provides chemical analysis of a series of Product Consistency Test (PCT) leachates from simulated nuclear waste glasses. The resulting data will be used in the development of improved property/composition models. For some of the glass leachates, minor scatter among the triplicate values of some analytes was observed. For other leachates, there were more significant differences among the triplicate values. A review of the PCT data noted that there was little difference between the normalized values on the basis of targeted or measured glass composition. Several of the canister centerline cooled study glasses have NC i values that are greater than the Hanford Tank Waste Treatment and Immobilization Plant immobilized low-activity waste constraint of 4 g/L for B and Na. The results of these glasses will help ensure the ability of advanced glass performance models to appropriately predict acceptable compositions. For many of the study glasses, heat treatment had only a marginal impact on the NC i values. The samples of the Environmental Assessment (EA) reference glass included with each PCT set had generally consistent NC i values. The release rates for boron and sodium, and for sodium and silicon were highly correlated for the study glasses, while for the other analytes, less correlation was observed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Spent Crystalline Silicotitanate Storage Study—Post AP-105DF Processing

A Tank-Side Cesium Removal (TSCR) system is under development by Washington River Protection Solutions to support initial production of immobilized low-activity waste (LAW) by feeding Hanford tank supernate from tank farms to the Hanford Waste Treatment and Immobilization Plant (WTP) LAW Facility. Tank waste supernate will be filtered to remove suspended solids and then Cs will be removed by processing it through crystalline silicotitanate (CST) ion exchange media manufactured by Honeywell UOP, LLC. The Cs-loaded CST columns will be stored indefinitely, with a goal of eventual CST removal and treatment. Thus, the spent CST needs to be recoverable after undetermined storage time. Previous testing with AP-105 simulant showed that rinsing the CST bed with 3 bed volumes (1.4 apparatus volumes [AVs]) of 0.1 M NaOH resulted in a dried bed that maintained flow characteristics indicative of ease of recovery. This study explored the intermediate conditions (between feed dried in place and the 1.4 AVs of 0.1 M NaOH rinse) to evaluate CST bed properties after: 1) stoppage with feed in place; 2) stoppage after draining feed; 3) stoppage after 0.7 AV of 0.1 M NaOH rinse through column; 4) stoppage after 1.5 AVs of 0.1 M NaOH rinse through column. Post processing, each column was heated at 50 °C for 19 days under pseudo-storage conditions to simulate the expected dried and stored CST bed conditions. Testing was conducted at the small scale (12-mL bed volume); actual, Cs-depleted, AP-105 tank waste was used as the feed. Post-dried CST bed physical properties (angle of repose and penetration depth) were measured to evaluate how CST moved and flowed. All process stop-conditions resulted in a solidified CST bed except for the final condition, 1.5 AVs of 0.1 M NaOH rinse. At this small scale, the three CST beds presented an issue for retrievability after the short storage period (19 days at 50 °C). The latter case confirmed the results from simulant testing. The testing was intended to provide a preliminary assessment of issues that may arise from desiccation of CST during storage with the indicated salt solutions in place. Since these were small-scale tests, the processing system did not scale to full scale conditions exactly; however, the tests did provide insight into the impact on the dried and stored CST bed after stopping processing at an earlier step (upset condition) than normal. These results indicate that if an upset condition occurs at TSCR, a dilute hydroxide rinse should be considered before the CST dries from internal heating.

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