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DOE OSTI2025

Tank 48H Phase 1 Initial Testing Using Sodium Permanganate to Decompose Tetraphenylborate: Simulant Studies with Shaker Oven and 2-L Vessel

Tank 48H currently holds legacy material including organic tetraphenylborate (TPB) compounds from the operation of the In-Tank Precipitation process. The large quantity of TPB is not compatible with the waste treatment facilities at SRS and must be removed or undergo treatment to oxidize the organic compounds before the tank can be returned to routine Tank Farm service. Tank 48H currently holds approximately 270,000 gallons of legacy material comprised of decontaminated salt solution, approximately 20,000 kilograms of TPB solids, 3,400 kilograms of sludge solids, and 1,800 kilograms of monosodium titanate (MST).

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DOE OSTI2023

Temperature Rise on Liner Surfaces of Fuel Cell Electric Vehicle Tanks during Fueling Process

Herein, the temperature of the inner tank walls, or plastic liners, of composite pressure tanks in fuel cell electric vehicles during fueling using three‐dimensional computational fluid dynamics (CFD) models is evaluated. The liner materials are limited to 85.0 °C to prevent thermal stress causing material failure that would result in a hydrogen leak. Therefore, the temperature of hydrogen gas must be limited to below 85.0 °C during the fueling process as dictated by the current fueling protocol. However, there are limited experimental or simulation data confirming that the temperature changes do not exceed the threshold. Herein, the liner temperatures with CFD tank models for two sizes of type IV tanks representative of the upper and lower system bounds that are close to the SAE J2601 fueling protocol (36.0 and 244.0 L) are evaluated. First, each model's reliability is validated with experimental data and then analyzed, and the data are used to evaluate the maximum hydrogen and liner temperatures under real‐world fueling conditions. The evaluation shows that the maximum liner surface temperature of each tank model is at least 7 °C lower than that of the hydrogen. Additionally, there is at least 12 °C difference found between the upper limit and actual liner temperatures.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2024

Concrete Testing Case for Closure of Handford’s 241-C Underground Storage Tanks

Sixty percent of the nation's highly toxic and radioactive mixed wastes are stored at Hanford in 177 deteriorating underground storage tanks. To close or remove these storage tanks from service and place them in a condition that is protective of human health and the environment, the tanks must be physically stabilized to prevent subsidence once wastes have been retrieved. Remaining residual liquid waste in the tanks that cannot be removed must be solidified and the solid wastes encapsulated to meet the Nuclear Regulatory Commission, Department of Energy, Environmental Protection Agency, and the State of Washington requirements. The Department of Energy has developed cementitious flowable concretes to restrict access and provide chemical stabilization for radionuclides. Formulation, laboratory, and field testing for application at Hanford began with flowable, self-leveling structural and non-structural fills. A slump flow equal to or greater than 610 mm, 0% bleed water, and 0.1% (by volume) shrinkage measurements were key parameters guiding reformulation efforts that resulted in highly flowable, self-consolidating concretes that met Hanford 241-C Tank closure short- and long-term regulatory and engineering performance requirements.

formula development↗

DOE OSTI2020

Modified Isotherm Modeling to Predict Cs Exchange with Crystalline Silicotitanate in Tank Waste Simulants

The U.S. Department of Energy is working to expedite processing of Hanford tank waste supernate at the Hanford Waste Treatment and Immobilization Plant. To support this goal, Washington River Protection Solutions is designing a Tank Side Cesium Removal (TSCR) system for suspended solids and cesium (Cs/ 137 Cs) removal from Hanford tank waste supernate. The ion exchange media selected for Cs removal at TSCR is crystalline silicotitanate (CST) that is manufactured in a nearly spherical form by Honeywell UOP LLC (UOP; Des Plaines, IL) as product IONSIV® R9140-B (Na form). The Zheng Anthony Miller (ZAM) isotherm model (Zheng et al. 1997) is a multicomponent ion exchange model used to predict the exchange of Group I metals onto CST. The ZAM isotherm has historically been used to predict Cs distribution values from Hanford and Savannah River Site (SRS) tank waste simulants. Figure S.1 summarizes model predictions from the ZAM isotherm that indicate poor prediction of Cs distribution values for simple and complex simulants with the engineered form of CST, IONSIV® R9140-B, and IONSIV® R9120-B where the solid line indicates a perfect fit by the model. The dotted lines indicate ±20% error. Batch contact testing with Hanford tank waste complex and simple simulants was used in conjunction with SRS simulants to experimentally determine Cs distribution values using a modification to the original isotherm model. The experimentally determined maximum Cs capacity for IONSIV® R9140-B CST in both the simple and complex matrices was found to be 0.53±0.3 mmoles Cs/g of CST. This value is not drastically different from the maximum Cs capacity of 0.58 mmoles Cs/g TAM-5 reported by Zheng et al. (1997). However, it is important to note that TAM-5 (commercially IONSIV® IE-910) is a powder. Hamm et al. (2002) determined that a dilution factor was needed to account for the Zr(OH)2 binder in the engineered form of CST. Hamm et al. determined that a dilution factor of 0.68 was appropriate to account for binder contribution and correct overprediction of Cs exchange on the engineered form of CST in ZAM calculations. This reduced the total capacity from 0.58 mmol/g with TAM-5 to 0.39 mmol/g for the engineered form of CST (Hamm et al. 2002). Despite substituting the experimentally determined maximum Cs capacity of 0.55 mmoles Cs/g for the literature-reported capacity of 0.39 mmoles Cs/g, it was determined that additional modifications to the model’s equilibrium rate constants were necessary in refining the isotherm model. The modified model overpredicted K+ uptake by the CST when compared to digested CST results described by Campbell et al. (2019). The modified model was further revised to omit three of the five K+ exchange equilibrium reactions described by ZAM to reduce the additional K+ loading seen by the model. Figure S.2 summarizes the revised model isotherm predictions plotted against measured Kd values.

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DOE OSTI2021

Characterization of CST Post-Processing AP-105 Hanford Tank Waste

The primary goal of the Tank Side Cesium Removal (TSCR) system, under development by Washington River Protection Solutions, LLC (WRPS), is to remove entrained solids and 137 Cs from the Hanford tank waste supernate to expedite production of low-activity waste. Ion exchange (IX) testing of 10.9 L of waste from Hanford tank 241-AP-105 (AP-105), performed by Pacific Northwest National Laboratory, used a lead-lag-polish column format, with a bed volume of 10 mL per column, to decontaminate tank waste supernate using crystalline silicotitanate (CST) as the IX media. The AP-105 Cs IX processing test, discussed elsewhere, resulted in a shorter transition zone (i.e., steeper load curve) than those defined by wastes from tanks 241-AP-107 and 241-AW-102.1 The shorter transition zone was indicative of a matrix effect retarding Cs capacity. Therefore, aliquots of spent CST from the lead, lag, and polish columns were subjected to a digestion protocol to quantify analytes retained by the CST and extrapolate the impact on Cs capacity. The spent CST was digested using a combination of 5 M HNO 3 and H 2 O 2 with vigorous heating and stirring. Due to the radiation dose accompanying the 137 Cs on the CST columns, a secondary Cs separation by ammonium molybdophosphate embedded in polyacrylonitrile (AMP-PAN) was performed to separate the 137 Cs from the CST so the samples could be contact-handled for analysis outside of a shielded facility.

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DOE OSTI2021

Temperature Effect of Cesium Exchange onto Crystalline Silicotitanate in AP-107 and AP-105 Hanford Tank Wastes and Two Simulants

Washington River Protection Solutions, LLC (WRPS) is charged with the development of the Tank Side Cesium Removal (TSCR) system to process Hanford tank waste supernates in preparation for vitrification. In addition to a filtration step, TSCR will remove cesium (Cs) using ion exchange columns filled with crystalline silicotitanate (CST) ion exchange media. CST is produced by Honeywell UOP, LLC. The documented safety analysis (DSA) developed for the TSCR system limits a single column loading to 141,600 Ci 137 Cs. Given a 137 Cs isotopic mass fraction of 20% and the planned CST bed size of 596 L (157.5 gal) in a TSCR column, this equates to 0.10 mmole Cs per g CST (Cs distribution coefficient, K d , 1400 mL/g). Factors that influence Cs uptake by CST include (but are not limited to) (1) CST production (lot-to-lot variations), (2) contact temperature, (3) contact duration, (4) competitors in the tank waste feed, (5) anionic composition of the tank waste feed, and (6) the 137 Cs isotopic mass fraction (differs slightly among tank wastes and decreases with time).

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DOE OSTI2020

Overview of 2016 through 2018 Testing of Air-Purifying Respirator (APR) Cartridge Performance on Multiple Hanford Tank Headspaces and Exhausters

Between 2016 and 2018, 28 air purifying respirator (APR) cartridge tests were performed on headspace vapors from seven Hanford waste storage tanks (SY-102, A-101, BY-108, AX-101, BY-110, SX-101, and SX-104) and seven waste tank exhausters (AP in 2016, AP in 2018, 702-AZ, AN and AW in 2016, and AX and 702-AZ in 2017). All but two tests were conducted under static conditions absent waste-disturbing activities in the subject tanks or tank farms. The two exceptions were cartridges tested with vapors from 702-AZ in 2017 when samples were taken during waste-disturbing activities. Multipurpose APR cartridges, SCOTT 7422-SD1 and 7422-SC1, were tested on samples from each of the 14 tanks or exhausters. Out of 612 Chemicals of Potential Concern (COPCs), only ammonia, mercury, N-nitrosodimethylamine (NDMA), 2,5-dimethylfuran, 2,5-dihydrofuran, furan, and 1,3-butadiene exhibited breakthroughs with outlet concentrations that were >10% of their Occupational Exposure Limits (OEL).

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DOE OSTI2020

Analysis of Air-Purifying Respirator (APR) and Powered Air-Purifying Respirator (PAPR) Cartridge Performance Testing on Hanford Tanks BY-108 and BY-110 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 air-purifying respirator (APR) and powered air-purifying respirator (PAPR) chemical cartridges commonly used by workers at Hanford Tank Farms to determine the period of time that 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. The Occupational Safety and Health Administration (OSHA) Standard promulgated in Title 29 of the 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 BY-110 and BY-108 headspace vapors, respectively. Two different APR cartridges from SCOTT Safety (Monroe, North Carolina) were assessed for the BY-110 headspace vapors, and two different PAPR cartridges—one from MSA Safety Inc. (Pittsburgh, Pennsylvania) and another from 3M (Maplewood, Minnesota)—were assessed for the BY-108 headspace vapors. Volume 1 of this report documents the testing, data analysis, results, conclusions, and recommendations resulting from the cartridge testing of vapors from the BY-110 and BY-108 headspaces. 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 OSTI2020

Overview of 2017 Through 2018 Testing of Powered Air-Purifying Respirator (PAPR) Cartridge Performance on Multiple Hanford Tank Headspaces and Exhausters

Between 2017 and 2018, 10 powered air-purifying respirator (PAPR) cartridge tests were performed on headspace vapors from three Hanford tanks (BY-108, SX-101, and SX-104) and two Hanford Tank Farm exhausters (AP in 2018 and AX in 2017). All tests were conducted under static conditions absent waste-disturbing activities in the subject tanks or tank farms. Multipurpose high-efficiency PAPR cartridges, MSA-TL (TL1) (MSA Safety Inc., Pittsburgh, Pennsylvania) and 3M FR-57 (TL2) (3M Company, Maplewood, Minnesota), were tested on each of the five tanks or exhausters. Out of 61 1 Chemicals of Potential Concern (COPCs), only ammonia and 2,5-dimethylfuran exhibited breakthroughs with outlet concentrations that were greater than 10% of their Occupational Exposure Limits (OEL). For 2,5-dimethylfuran, elevated concentrations found in blank tube samples made the elevated outlet measurements for this COPC questionable.

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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 OSTI2023

Results for the January 2023 Semiannual Tank 50 Salt Solution Sample

In this Technical Report, the chemical and radionuclide contaminant results from the January 2023 Semiannual sample of Tank 50 salt solution are presented in tabulated form. The information from this characterization will be used by Savannah River Mission Completion (SRMC) for the transfer of aqueous waste from Tank 50 to the Saltstone Production Facility (SPF), where the waste will be treated and disposed in the Saltstone Disposal Facility. This Technical Report compares results, where applicable, to SPF Waste Acceptance Criteria (WAC) LIMITS and TARGETS that were established at the time the Tank 50 sample was obtained.1 The chemical and radionuclide contaminant results from the characterization of the January 2023 semiannual sampling of Tank 50 were requested by SRMC personnel via a Task Technical Request (TTR)2 and details of the testing are presented in the Savannah River National Laboratory (SRNL) Task Technical and Quality Assurance Plan (TTQAP).3 This Technical Report is part of Deliverable 2 relating to Task 1 from the SRMC request.2 Data pertaining to the regulatory limits for Resource Conservation and Recovery Act (RCRA) metals per Task 2 from the SRMC request will be obtained semiannually for the January 2023 and July 2023 Tank 50 samples.

Crawford, Charles L.↗

DOE OSTI2020

Inspection Tools for Hanford Tanks and Waste Transport Systems - 20444

Recent integrity issues in the double-shell tanks (DST) at Hanford have motivated the need for developing innovative tools that can provide information regarding the health of the tanks. These issues include the primary linear failure of AY-102 and recent concerns of thinning in the DST secondary liners. Other concerns include erosion or corrosion on transfer lines and processing pipes. In recent years, Florida International University (FIU) has supported DOE-EM by developing tools that can assist in understanding the health of tanks and waste transport system at Hanford. More specifically, FIU has developed a miniature rover that can be deployed through small risers and gain access to refractory slots in the Hanford DSTs. It traverses through the slots on the primary liner upside down via magnets to avoid debris in the slots. Recent modifications include a spring loaded magnetic arm that allows the unit to traverse over large weld seams but does not reduce the overall functionality of the system. The system has also incorporated a control capsule that will sit within the annulus of the tank and improves on issues related to signal and voltage loss over long tether lines. Lastly, the unit is also being augmented with a second module that will include a means to prep the tank surface and obtain a thickness measurement using a dual element ultrasonic sensor. FIU has also developed a 6-inch peristaltic pipe crawler that operates similar to the previous pipe crawlers developed at FIU. This crawler is a marsupial type crawler that will navigate through the 6-inch drain lines, and deploy a small rover at the entrance of the drain slots. This rover will also traverse upside down on the secondary liner and provide information regarding the health of the liner. An initial prototype for the crawler unit has been developed, assembled and tested. The system is pneumatic and consists of three modules - two grippers and one extender. The validation tests are conducted in a mockup of the drain lines and demonstrate the system's ability to navigate through long pipe lengths and elbows. In this paper, a general overview of each of the aforementioned systems is presented along with results from testing and demonstrations that shows the applicability of each system. (authors)

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DOE OSTI2026

Tank 14H Preliminary Cease Waste Removal Sample Analyses

Savannah River Mission Completion Waste Removal and Tank Closure requested that Savannah River National Laboratory perform characterization analyses of Tank 14H in support of closure activities, specifically preliminary cease waste removal. This report provides important characterization of the prepared filtrate and air-dried solids in the January 2026 Tank 14H sample, HTF-14-26-1,2,3,4,5,6, for I-129, Tc-99, Cs-137, and Sr-90. The results reported here were utilized by SRMC to declare preliminary cease waste removal for Tank 14H.

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DOE OSTI2024

Enhanced prediction of Cs removal by CST from Hanford tank waste with K accountability

Abstract The treatment of Hanford tank waste is one of the most challenging environmental cleanup activities to date. To expedite the processing of liquid waste stored in underground tanks in Washington State it is necessary to remove the significant dose contributor, 137 Cs. Crystalline silicotitanate ion exchanger is currently used to remove 137 Cs from the aqueous phase of Hanford tank wastes in preparation for vitrification at the Waste Treatment and Immobilization Plant (WTP). Improving the understanding of potassium impacts on ion exchange behavior of Cs will help in the operation of a critical component of one of the most complex treatment processes in the world today. Optimization of this process can result in significant cost savings and less waste production. Toward this effort, a series of batch contact tests varied in potassium concentration were conducted to look at the impact of potassium concentration on Cs distribution. Experimental distribution ratios ( K d ) were compared to the distribution ratios predicted using the ZAM model. A significant underprediction of Cs capacity in the presence of potassium was seen with the existing model. A revision of the equilibrium constants was determined and provided a statistically better fit for determining the Cs K d values in tank waste matrices.

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DOE OSTI2022

Impact of dilution-induced precipitates on the filtration of Hanford liquid tank wastes

To facilitate its vitrification, a portion of the radioactive wastes currently stored at the Hanford Site will be staged and treated using tank-side operations to render their chemistry compliant with the requirements of Hanford’s low-activity waste vitrification facility. Initial sampling of staged feeds indicates that process-water dilution, used to reduce waste feed sodium content to levels acceptable for vitrification (5–6 M Na), may cause precipitation of fine, difficult to settle solids that could affect downstream tank-side filtration and ion-exchange. However, dilution-induced precipitation has not been demonstrated under controlled, rigorous laboratory conditions. This paper presents a set of qualitative and quantitative assessments of dilution-induced precipitation using a nonradioactive, Hanford Tank AP-105 simulated waste. Further, these studies found that dilution of AP-farm waste simulants induced precipitation of up to 150 ppm solids, regardless of whether dilution was done with process water (which contains, among other analytes, naturally occurring Ca and Mg) or deionized water. Naturally occurring process-water analytes appeared to accelerate the rate (and possibly extent) of precipitation. Filtration of diluted waste simulants also found that the precipitated solids challenged prototypic tank-side filter operations; however, the impact to filtration performance was readily managed through waste staging settle/decant operations.

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DOE OSTI2023

Methods for Estimating Hydrogen Fuel Tank Characteristics

The pressure vessels needed to store hydrogen for next-generation hydrogen fuel cell vehicles are expected to be a substantial portion of the total system mass, volume, and cost. Gravimetric capacity, volumetric capacity, and cost per kilogram of usable hydrogen are key performance metrics that the U.S. Department of Energy (DOE) uses to determine the viability of hydrogen fuel cell systems. Research and development related to hydrogen storage systems covers a wide range of potential operating conditions, from cryogenic temperatures to high temperatures (above ambient) and low pressure to high pressure. Researchers at PNNL have developed methods for estimating these key pressure vessel characteristics to support on-board hydrogen storage system design and performance evaluation and to support decision-making about DOE hydrogen storage system research investments. This article describes the pressure tank estimation methodology that has been used as a stand-alone calculation and has been incorporated into larger system evaluation tools. The methodology estimates the geometry, mass, and material cost of type I, type III, and type IV pressure vessels based on operating pressure and material strength at the system's operating temperature, using classical thin-wall and thick-wall pressure vessel stress calculations. The geometry, mass, and material cost requirements of the pressure vessel have significant impacts on the total system performance. For example, hydrogen storage materials that can separately achieve a very high hydrogen density can be deemed impractical for use in fuel cell vehicle hydrogen storage systems because the pressure tank containing them is too large, heavy, or expensive. This article describes the design philosophy and analytical process of the tank characteristic estimation methodology, which has been implemented in spreadsheet calculation tools and system-level analysis tools used by DOE researchers. Each of the three tank types (type I, type III, and type IV) uses a different analysis methodology with some common elements. This article also provides examples of implementing the methodology to perform parametric studies of all three pressure vessel types. The goal of this article is to present the methodology in sufficient detail so it can be implemented in other hydrogen fuel cell vehicle design and analysis tools.

42 ENGINEERING↗

DOE OSTI2021

Methylmercury Retention Evaluation to Support Tank 50 and Saltstone Waste Acceptance Criteria: Parts 2 and 3

The objective of this work was to provide a technical basis for the organic mercury waste acceptance criterion (WAC) for Tank 50 salt solution. The current mercury WAC for Tank 50 solution is 325 mg/L as Hg regardless of the form of mercury, which is about three times higher than any total Hg concentrations measured to date in Tank 50 solution. To date, the highest total Hg and MeHg + concentrations in the Tank 50 solution were 105 and 62 mg/L, respectively.

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DOE OSTI2021

Analysis of Defense Waste Processing Facility Sample: Recycle Collection Tank Sample Batch 4945

The Savannah River National Laboratory (SRNL) was requested by Savannah River Remediation (now Savannah River Mission Completion (SRMC)), through a Technical Task Request, to characterization the “as-received” Recycle Collection Tank (RCT) Sample identified as sample batch 4945 [Sludge Receipt and Adjustment Tank (SRAT) batch 796)], which was delivered to SRNL Shielded Cells on January 28, 2021. The RCT characterization data will be used as input to the Defense Waste Processing Facility (DWPF) Recycle Diversion Project. This RCT report is the first of three sample characterization reports that will be used for this DWPF Project. The other DWPF reports will involve the characterization of the Off-Gas Condensate Tank (OGCT) and the Slurry Mix Evaporator Condensate Tank (SMECT) samples.

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