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DOE OSTI2020

Analysis of Air-Purifying Respirator (APR) and Powered Air-Purifying Respirator (PAPR) Cartridge Performance Testing on a Hanford AX Tank Farm Exhauster Slipstream Volume 2: Raw Analytical Data

As the Tank Operations Contractor for U.S. Department of Energy operations at the Hanford site in Washington State, Washington River Protection Solutions (WRPS) is responsible for managing highly radioactive wastes stored in tanks at Hanford. To protect workers at Hanford Tank Farms, WRPS tests air-purifying respirator (APR) and powered air-purifying respirator (PAPR) chemical cartridges commonly used at the tank farms. The tests were conducted to determine the period of time the cartridges would provide adequate performance for APRs and PAPRs when workers are exposed to a mixture of Chemicals of Potential Concern (COPC) from any vapors exiting headspaces in the storage tanks. Occupational Safety and Health Administration (OSHA) Standard 29 Code of the Federal Regulations (CFR) 1910.134(d)(3)(iii)(b)(2) specifies that for protection against gases and vapors, employers shall implement a schedule for cartridges to ensure that change-outs occur before the end of service life. The change schedule can be based on objective information or data that ensures cartridge change-outs occur before the end of their service life. The primary function of the WRPS Cartridge Test Program is to obtain objective data to determine service lives for the APR and PAPR cartridges used at Hanford Tank Farms. WRPS contracted with Pacific Northwest National Laboratory to analyze the test data and offer an independent analysis and any recommendations. This report summarizes data analysis of APR and PAPR cartridge testing on a vapor slipstream from the Hanford AX tank farm exhauster. Volume 1 of this report documents the testing, data analysis, results, conclusions, and recommendations resulting from the cartridge testing on AX exhauster slipstream vapors. Volume 2 provides an introduction to the raw data, including analytical laboratory analysis results that supported the analysis and conclusions documented in Volume 1.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Analysis of Powered Air-Purifying Respirator (PAPR) Cartridge Performance Testing on Hanford Tanks SX-101 and SX-104: Volume 2 Raw Analytical Data

As the Tank Operations Contractor for U.S. Department of Energy operations at the Hanford site in Washington State, Washington River Protection Solutions (WRPS) is responsible for managing highly radioactive wastes stored in tanks at Hanford. WRPS tests of cartridges used in air-purifying respirators (APR) and powered air-purifying respirators (PAPR) commonly used at Hanford Tank Farms. The tests are conducted to determine the period of time the cartridges would provide adequate performance for APRs and PAPRs used to protect workers when exposed to a mixture of Chemicals of Potential Concern (COPC) from any vapors exiting headspaces in the storage tanks. Occupational Safety and Health Administration (OSHA) Standard 29 Code of the Federal Regulations (CFR) 1910.134(d)(3)(iii)(b)(2) specifies that for protection against gases and vapors, employers shall implement a schedule for cartridges to ensure that change-outs occur before the end of service life. The change schedule can be based on objective information or data that ensures cartridge change-outs occur before the end of their service life. The primary function of the WRPS Cartridge Test Program is to obtain objective data to determine service lives for the APR and PAPR cartridges used at Hanford Tank Farms. WRPS contracted with Pacific Northwest National Laboratory to analyze the test data and offer an independent analysis and any recommendations. This report summarizes data analysis of PAPR cartridge testing on headspace vapors from Hanford SX-101 and SX-104 single-shell tanks. Two different PAPR cartridges—one from MSA Safety Inc. (Pittsburgh, Pennsylvania) and another from 3M (Maplewood, Minnesota)—were assessed on each tank headspace source on separate days. These data represent the first PAPR cartridge testing under the recent WRPS program, as testing to date had been focused on APR cartridges. Volume 1 of this report documents the testing, data analysis, results, conclusions, and recommendations resulting from the PAPR testing on SX-101 and SX-104 headspace vapors. Volume 2 provides an introduction to the raw data, including analytical laboratory analysis results that supported the analysis and conclusions documented in Volume 1.

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DOE OSTI2024

Organic Evaporation, Oxidation, and Hydrolysis Testing in Support of Hanford Sample-and-Send

The Hanford site has approximately 54 to 56 million gallons of radioactive mixed waste stored in 156 unretrieved underground storage tanks. The Hanford Waste Treatment and Immobilization Plant (WTP) is being built to treat and immobilize the tank waste. The baseline method for immobilization of Low Activity Waste (LAW) through the WTP is vitrification, but additional immobilization capacity is needed to supplement the initial LAW melters. An alternative cementitious waste form is being investigated for that future immobilization method. However, one impediment to a cementitious waste form is the presence of Land Disposal Restricted (LDR) organic chemicals in tank waste, which are regulated on a concentration based standard in the final waste form. Hence, if the quantity of organics in LAW is high enough, they must be destroyed or removed to make a waste form compatible with disposal in a mixed low level waste landfill. This work evaluates potential avenues for treatment of LDR organics to eliminate the impediment and permit possible use of a cementitious waste form. Vacuum evaporation testing to remove LDR organics consisted of preparing a non-radioactive LAW simulant, spiking that simulant with organic chemicals, and evaporating the mixture via differential distillation. The apparatus was a laboratory-scale vacuum evaporator operated at 60 ±5 torr absolute (vacuum evaporation). The LAW simulant represented the liquid expected to be retrieved from the Hanford tank farms at approximately 4.0 M [Na+] total sodium ion concentration. The concentration of the organic chemicals added was significantly higher than typically found in the tank waste samples since the higher levels were necessary to assist in analytical measurement and tracking of the spiked species.

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DOE OSTI2020

Enhanced Hanford Low-Activity Waste Glass Property Data Development (Phase 3)

This work was performed for the U.S. Department of Energy (DOE) Office of River Protection (ORP) to provide expert evaluation and experimental work in support of the River Protection Project vitrification technology development1. The long-term objective of this work is to expand the property-composition database for Hanford site low-activity waste (LAW) glasses and property-composition models to cover the balance of the mission for the Hanford Waste Treatment and Immobilization Plant (WTP). When this effort is complete, enhanced LAW glass property-composition models will be developed.

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DOE OSTI2021

Advancements of On-Line Monitoring and Real-Time Characterization of Actual Low-Level Hanford Tank-Waste Samples

Waste and process stream characterization is essential to the safe, efficient, and cost-effective processing of Hanford Site materials. The demand for materials characterization including chemical, radionuclide, and physical attributes during waste management, transfer, and staging operations in the Hanford tank farms is expected to significantly increase as the U.S. Department of Energy River Protection Project progresses toward Hanford waste treatment and immobilization. Our past work has applied Raman on-line monitoring and chemometric modeling to the supernate of Hanford tank 241-AP-105 and has demonstrated the quantitative measurement of nine analytes within this waste. To demonstrate broader applicability, this method has now been expanded to waste from two additional Hanford tanks, AW-102 and AP-107, and the offgas condensate from lab-scale melter runs of actual-tank waste feeds. To enhance the performance of the Raman method, instruments with various excitation wavelengths were compared, since it is known that the Raman response is enhanced by shorter wavelength excitation. The laser excitations for the three systems tested were 404 nm, 532 nm, and 671 nm. In addition to laser wavelength selection, the laser power, measurement integration times, and signal averaging techniques were also investigated to determine their effect on detection limits for oxy-anion analytes within tank wastes. These advancements in Raman capability are compared with past standards and will be presented.

Bryan, Samuel A.↗

DOE OSTI2024

Effect of Drying on Corrosion Mitigation of Hanford Transfer Lines

Radioactive waste is stored in underground, carbon-steel double-shell tanks at the Department of Energy Hanford site. The waste is transferred between the tanks and other assets using the transfer lines spanning throughout the various tank farms at Hanford. The transfer lines consist of a pipe-in-pipe design, small diameter pipes, and are not piggable. Recent inspection data of the transfer lines have shown areas with corrosion on both interior of the encasements and exterior of the primary pipes, with nearly 50 percent wall loss on the primary pipes and nearly 25% wall loss on the encasement pipes due to pitting corrosion. The visual inspections of the transfer lines have shown presence of corrosion products near the pipeline risers and beyond. It has been hypothesized that the corrosion is predominantly due to the high humidity conditions and in some cases is driven by the presence of residual hydrotest water in the encasement and the associated contact with the safety significant primary pipe. Therefore, drying of the transfer lines could lead to corrosion mitigation. Experimental studies are being conducted to understand the effect of environmental conditions, especially, relative humidity and temperature, on transfer line grade carbon steel corrosion and on mitigating corrosion. The experimental conditions are selected based on the seasonal temperature changes, and relative humidity conditions ranging from 30 to 100 percent. The experimental data will be used as guidance for maintaining a dry environment that will help mitigate the transfer-line corrosion caused by the high humidity conditions.

Shukla, Pavan K.↗

DOE OSTI2020

Ion Exchange of Selected Group II Metals and Lead by Crystalline Silicotitanate and Competition for Cs Exchange Sites

A series of batch contact tests were conducted to evaluate the exchange behavior of Ba, Ca, Pb, and Sr onto crystalline silicotitanate (CST) in support of an expedited Cs removal and pretreatment system at the Hanford site. Binary Na/M 2+ and ternary Na/Cs/M 2+ isotherms were generated to understand selectivity, capacity, and competitive impact of each analyte on Cs uptake from a simple 1 M NaOH/4.6 M NaNO 3 simulant. Analyte loading from a 0.1 M NaOH/5.5 M NaNO 3 simulant was assessed to determine the effect of hydroxide concentration on binary Na/M 2+ isotherms. Finally, results from binary and ternary isotherms indicated that group II metals, and Pb do not impact CST performance toward CST at concentrations expected in Hanford tank waste supernate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Determining Unabated Airborne Radionuclide Emissions Monitoring Requirements Using Inventory-Based Methods

Compliance with the airborne radionuclide emission monitoring requirements in the National Emission Standards for Hazardous Air Pollutants (NESHAP; 40 CFR Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247 and 173-480 were evaluated for Pacific Northwest National Laboratory (PNNL) operations. Additional guidance may be found in the U.S. Department of Energy Handbook, Environmental Radiological Effluent Monitoring and Environmental Surveillance. To meet regulatory requirements, reviews of planned or proposed projects and activities provide the basis for implementing necessary monitoring adjustments or for implementing changes to projects and activities in a timely manner. Potential unabated off-site doses were evaluated for emission locations managed by PNNL and licensed to the Department of Energy. These locations were at facilities in Richland, Washington (i.e., the Hanford Site and PNNL-Richland Campus) and in Sequim, Washington, (PNNL-Sequim Campus, which formerly was known as the Marine Sciences Laboratory). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2021 for calendar year ending 2020.

40 CFR 61 Subpart H↗

DOE OSTI2024

Determining Unabated Airborne Radionuclide Emissions Monitoring Requirements Using Inventory-Based Methods

Compliance with the airborne radionuclide emission monitoring requirements in the National Emission Standards for Hazardous Air Pollutants (NESHAP; Title 40 of the U.S. Code of Federal Regulations Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247: Radiation Protection – Air Emissions and 173-480: Ambient Air Quality Standards and Emission Limits for Radionuclides were evaluated for Pacific Northwest National Laboratory (PNNL) operations. Additional guidance may be found in the U.S. Department of Energy Handbook, Environmental Radiological Effluent Monitoring and Environmental Surveillance. To meet regulatory requirements, reviews of planned or proposed projects and activities provide the basis for implementing necessary monitoring adjustments or for implementing changes to projects and activities in a timely manner. Potential unabated off-site doses were evaluated for emission locations managed by PNNL and licensed to the Department of Energy. These locations were at facilities in Richland, Washington (i.e., the Hanford Site and PNNL–Richland campus) and in Sequim, Washington, (PNNL–Sequim campus). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2024 for calendar year ending 2023.

40 CFR 61 Subpart H↗

DOE OSTI2025

Evaluation of Hanford 200 West Area Tank Farms (241-S/241-SX-/241-U tank farms) Physical Properties Data for Use in Development of West Area Tank Treatment (WATT) Processing

With the recent acceptance of West Area Tank Treatment disposition alternative for 200 West Area tanks at the Hanford Site by the State of Washington and the U.S. Department of Energy, a review was initiated to identify the physical properties data available in the literature for the Hanford 241-S, 241-SX, and 241-U tank farms. The literature reviewed indicated that there is a relatively small set of useful data on physical properties of 200 West Area tanks, and the data that do exist are biased around a narrow range of tank samples. Much of the testing between the 1990s and mid-2010s was intended to support either enhanced sludge washing or feed delivery to the Pretreatment Facility at the Hanford Waste Treatment and Immobilization Plant. As such, some physical properties of 200 West Area samples were measured under conditions that are no longer relevant. Because of the distinctly different nature of many past processes at the 200 West Area compared to the 200 East Area, insight from waste testing in the 200 East Area waste should be used with caution, as there may be significantly different qualities in the physical properties data between these two areas (both in situ and as measured in laboratory analyses). Based on this assessment, there is a need to collect additional physical property data to support planning for 200 West Area retrievals.

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DOE OSTI2021

Influences on Subsurface Plutonium and Americium Migration

Plutonium (Pu) has been released to the environment worldwide, including approximately 1.85 × 1015 Bq (200 kg) of Pu from process waste solutions to unconfined soil structures at the Hanford Site in Washington State. The subsurface mobility of Pu is influenced by complex interactions with sediments, groundwater, and any co-contaminants within the waste stream. Previous investigations at Hanford have shown that Pu exists as discrete PuO 2 particles forming before or after disposal, as secondary solid phases formed from waste interactions with sediments as adsorbed/incorporated species, and/or as dissolved species. In this research, new evidence is presented for the existence of PuO 2 , PuO 2 -Bi 2 O 3 composites, and particles from burnt Pu metal in near-surface sediments where Pu-laden acidic process waste was disposed to sediments. Pu and americium (Am) L3 X-ray absorption spectroscopy and density functional theory suggest that, in larger, more crystalline PuO 2 particles, Am formed from radioactive decay is retained in the Pu IV O 2 structure as Am IV . The Pu and Am that were disposed of in an acidic waste stream have since migrated deeper into the subsurface with detection to at least 37 meters below ground surface. In contrast, Pu deposited near the ground surface from neutral pH waste is found to be homogeneously distributed and relatively immobile. Groundwater extractions performed on contaminated sediments indicate that both Pu and Am are recalcitrant, with Am being fractionally less extractable than Pu on a molar basis. These results suggest that the more mobile fraction of Am has migrated from the near-surface and may be present in the deeper sediments as a different phase than Pu. From these results, it is suggested that Pu and Am deposited from acidic wastes were initially mobile and became significantly less mobile as wastes were neutralized within the soil profile.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2020

FY 2020 Radionuclide Migration Project Status

The Waste Management Project provides safe, compliant, and cost-effective waste management services for the Hanford Site and the U.S. Department of Energy (DOE) complex. Part of these services includes safe disposal of low-level waste and mixed low-level waste at the Hanford Low-Level Waste Burial Grounds in accordance with the requirements of DOE Order 435.1, Radioactive Waste Management. To partially satisfy these requirements, performance assessment analyses were completed and approved. DOE Order 435.1 also requires continuing data collection to increase confidence in the critical assumptions used in these analyses to characterize the operational features of the disposal facility that are relied on to satisfy the performance objectives identified in the order.

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DOE OSTI2021

Geophysical Characterization of 200 TEDF to Support Discharge Permit Renewal

The Treated Effluent Disposal Facility (TEDF) is a site where treated non-hazardous and non-radioactive liquid wastes are collected and disposed of in two state-permitted disposal basins near the 200 East Area at the Hanford Site. In 2016, a renewal application was submitted for TEDF that requested mass loading effluent limits instead of concentration-based effluent limits. The Washington State Department of Ecology denied this request due to a lack of groundwater monitoring wells that can be used to identify and characterize the impact of TEDF discharges on the underlying groundwater. Current TEDF monitoring wells are screened in the confined aquifer below the Ringold Lower Mud (RLM) unit and are not representative of TEDF discharges that can potentially mound above the RLM unit.

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DOE OSTI2024

Ion Exchange Processing of AN-107 Hanford Tank Waste through Crystalline Silicotitanate in a Staged 2- then 3-Column System

The Hanford Site stores an estimated 56 million gallons of mixed radioactive and chemically hazardous waste in large underground tanks. In support of the Direct Feed Low-Activity Waste (DFLAW) Program for expediting Hanford tank waste supernate treatment, laboratory-scale ion exchange processing using prototypic unit operations was conducted on AN-107 tank waste at the Pacific Northwest National Laboratory Radiochemical Processing Laboratory. This report describes the small-scale ion exchange testing with 13.7 L of diluted and filtered supernate from Tank 241-AN-107 (hereafter referred to as AN-107) at 16 °C (62 °F). 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 AN-107 tank waste to meet this criterion, only 0.147% of the influent 137 Cs concentration may be delivered to the WTP; this requires a Cs decontamination factor of 678. Testing with AN-107 matched current Tank Side Cesium Removal (TSCR) facility prototypic operations where a lead-lag configuration was used until the lag column reached the WAC limit, then a polish column was brought online for continued processing in a lead-lag-polish column configuration. Feed was processed at 1.9 bed volumes (BVs) per hour; the flowrate, in terms of contact time with the crystalline silicotitanate (CST) bed, matched the expected flowrate at TSCR. The Cs-decontaminated product was retained for vitrification testing (to be reported separately). The lead column reached 40% Cs breakthrough after processing ~1700 BVs of feed; the 50% Cs breakthrough was extrapolated from the breakthrough data to occur at 1873 BVs. Testing compared to previous AP-101 and AP-107 testing at 16 °C showed ~300 BV increases in volume processed to reach the WAC limit for both lead and lag columns. The increase in capacity was determined to be due to the significantly lower K concentration in the AN-107 compared to the other tank waste matrices. A comparison in breakthrough curves for the three tests indicated slightly slower kinetic behavior in the AN-107, with variations in feed matrices (high organic complexants) likely responsible for the deviation. The Cs effluent from the lag column reached the WAC limit after processing 1097 BVs. Anticipating this breakthrough point, the polish column was preemptively installed around 900 BVs. Cs breakthrough from the lag column began at 500 BVs, reaching 3.06×10 0 µCi/mL, or 2.6 % Cs breakthrough, after processing all 1700 BVs of feed. Table S.1 and Figure S.1 summarize the observed column performance and relevant Cs loading characteristics.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Ion Exchange Processing of AW-105 Hanford Tank Waste through Crystalline Silicotitanate in a Staged 2- then 3-Column System

The Hanford Site stores an estimated 56 million gallons of mixed radioactive and chemically hazardous waste in large underground tanks. In support of the Direct Feed Low-Activity Waste (DFLAW) Program for expediting Hanford tank waste supernate treatment, laboratory-scale ion exchange processing using prototypic unit operations was conducted on AW-105 tank waste at the Pacific Northwest National Laboratory Radiochemical Processing Laboratory. This report describes the small-scale ion exchange testing with 9.2 L of diluted and filtered supernate from Tank 241-AW-105 (hereafter referred to as AW-105) at 16 °C (62 °F). 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 AW-105 tank waste to meet this criterion, only 0.225% of the influent 137 Cs concentration may be delivered to the WTP; this requires a Cs decontamination factor of 445. Testing with AW-105 matched current Tank Side Cesium Removal (TSCR) facility prototypic operations where a lead-lag configuration was used until the lag column reached the WAC limit, then a polish column was brought online for continued processing in a lead-lag-polish column configuration. Feed was processed at 1.9 bed volumes (BVs) per hour; the flowrate, in terms of contact time with the crystalline silicotitanate (CST) bed, matched the expected flowrate at TSCR. The Cs-decontaminated product was retained for vitrification testing (to be reported separately). The lead column reached 83% Cs breakthrough after processing ~1500 BVs of feed; the 50% Cs breakthrough was interpolated from the breakthrough data and occurred at 1041 BVs. Despite the AW-105 having a significantly higher K concentration (0.55 M compared to 0.10 M), testing compared to previous AP-107 ion exchange column testing at 16 °C showed no difference in BVs processed to reach the WAC on the lead column and only an approximate ~20 BV decrease in volume processed to reach the WAC limit on the lag column. The negligible differences in capacity despite the 5x concentration differences in K was determined to be due to the significantly lower NO3 concentration in the AW-105 supernate compared to the AP-107 tank waste matrix. A comparison in breakthrough curves for the two tests also indicated slightly faster kinetic behavior in the AW-105, with the variations in feed matrices (lower NO3 concentration) likely responsible for the deviation. The Cs effluent from the lag column reached the WAC limit after processing 772 BVs. Anticipating this breakthrough point, the polish column was preemptively installed around 675 BVs. Cs breakthrough from the lag column began at 300 BVs, reaching 1.10×10 1 µCi/mL, or 14.13 % Cs breakthrough, after processing all 1500 BVs of feed. The polish column processed nominally 830 BVs and reached 2.10×10 -1 µCi/mL, or 0.27 % Cs breakthrough at the conclusion of the test. Table S.1 and Figure S.1 summarize the observed column performance and relevant Cs loading characteristics.

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DOE OSTI2025

FY25 Task 5: Small-Scale Mixing

The U.S. Department of Energy (DOE) Hanford Site has 177 underground storage tanks that contain a complex and diverse mix of chemical and radioactive wastes from past nuclear fuel reprocessing and waste management operations. The strategy of the DOE Hanford Field Office is to retrieve this waste, ~20 vol% of which is in the form of insoluble undissolved solids (UDS) or sludge, and treat it via immobilization at the Hanford Waste Treatment and Immobilization Plant (WTP). The diverse properties and characteristics of Hanford tank waste lead to major challenges related to its transport from the underground tanks to the WTP. These challenges, however, can be addressed by investigating the behavior of tank waste samples and simulant materials and evaluating their behavior against the capabilities of mixing and transport system designs that may be incorporated to retrieve and treat the waste.

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DOE OSTI2025

Batch contact testing with variable Na AN-107 and AP-105

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Refining the Approach to Process Flowsheet Development and Maturation at Hanford - 20049

Rigorous process flowsheet management strategies form the basis of an enduring approach to refining the River Protection Project Integrated Process Flowsheet. Incorporation of lessons learned, recognizing upstream and downstream impacts and understanding barriers to implementation of process flowsheets from the outset of the decision-making process will help future revisions to the River Protection Project Integrated Process Flowsheet be more robust, technically defensible, cost effective, and time efficient, ultimately leading to an improved environmental stewardship of the Hanford site. (authors)

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