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DOE OSTI2025

FY22 Development of Improved Grout Waste Forms for Supplemental Low Activity Waste Treatment

About 54 to 56 million gallons of radioactive mixed waste is currently stored in underground tanks at the United States Department of Energy’s (DOE’s) Hanford site in the State of Washington. This waste will be separated into low- and high activity waste fractions, which will then be vitrified respectively into Immobilized Low Activity Waste (ILAW) and Immobilized High Level Waste (IHLW) products for subsequent disposal. The ILAW product will be disposed of in an engineered facility at the Hanford site while the IHLW product is designed for acceptance into a national deep geological disposal facility for high level nuclear waste. Treatment of the tank waste will take place in the Hanford Tank Waste Treatment and Immobilization Plant (WTP), which is under construction. However, since the WTP Low Activity Waste (LAW) Vitrification Facility was not designed to process the entire inventory of Hanford LAW, up to half of the retrieved Hanford LAW will require supplemental immobilization. Immobilizing LAW in a cementitious waste form known as Cast Stone has been investigated as a possible candidate supplemental immobilization technology

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Summary of Savannah River Site FY24 Salt Waste Qualification Data

Savannah River Mission Completion (SRMC), the Liquid Waste Operations subcontractor at SRS, and Savannah River National Laboratory (SRNL) analyzed samples from Savannah River Site (SRS) Waste Tanks 21H, 41H, and 42H to support qualification of Salt Waste Processing Facility (SWPF) Waste Batches 10, 11, 12, and 13 for processing (the FY24 Salt Batch Qualification samples). These Tanks (i.e. 21H, 41H and 42H) are blend tanks for feed to SWPF. This report focuses on the characterization of the Salt Batch Qualification sub-samples (i.e., any adjustments after qualification or as a part of processing are documented elsewhere). None of the samples displayed any unusual or unexpected characteristics such as large amounts of solids, floating solids, or unusual color. Characterization of these samples confirmed similar chemical composition and characteristics to previous salt waste batches. The analytical results (both rapid, typically 4 weeks, and long-term, typically 8 weeks) for Salt Batches 10, 11, 12, and 13 are now summarized and discussed in this technical report. SRMC-Analytical Laboratory (SRMC-AL), for the first time, provided all the short-term analyses data used in the qualification evaluations of SWPF Salt Batches 10, 11, 12, and 13. These SRMC short-term results are presented along with the results for the long-term analyses provided by SRNL.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Improved Fundamental Understanding of Aluminum Chemistry and Interactions of Aluminate Anion with Co-Anions: ORNL Project Progress Report

The U.S. Department of Energy (DOE)’s Hanford Site in Washington State houses 177 underground storage tanks containing millions of gallons of nuclear and chemical waste with high aluminum content. Aluminum (Al) salt reactions with strong bases produce aluminum hydroxides, like boehmite (γ-AlOOH), which are main components of insoluble nuclear waste sludge. Understanding the morphology, crystallinity, and dissolution behavior of boehmite under waste tank conditions is necessary for improving waste management and mitigation strategies. The ORNL team uses in situ multimodal analysis strategy to study Al chemistry of simulated tank waste using microfluidic reactors and advanced chemical imaging and mass spectrometry (MS) techniques. Because the SALVI device is vacuum compatible and transferrable among different platforms, we can use it in scanning electron microscopy (SEM), vacuum ultraviolet single photon mass spectrometry (VUV SPI-MS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS) to study the chemical speciation and colloid stability in liquids in this project. Additionally, ex situ transmission electron microscopy (TEM) and x-ray diffraction (XRD) spectroscopy can be used to verify particle phase to further the understanding of the Al-bearing phases. This report gives a summary of the technical progress of the ORNL tasks. A plan for year 2 performance is recommended in the summary.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Assessment of Vibration and Shock Loading Environments on Steels Used in Railroad Applications Considering Hydrogen Embrittlement

Studies that examine the combined effects of hydrogen and rail loading environments in the context of hydrogen embrittlement of steels have not been performed. Large-scale hydrogen storage requires either gaseous hydrogen stored in pressure vessels and tubing or liquid hydrogen in cryogenic, insulated tanks. Since the focus of this study is on steels, we examine the influence of hydrogen on stainless steel used for high pressure tubing and cryogenic tanks and Cr-Mo steel liners used in gaseous pressure vessels. Literature studies show that despite hydrogen degradation, these steels can be used effectively and safely if the stresses are managed. The shock and vibration environment on railcars present unique environments where stresses and loading rates can be high. A literature review was conducted to understand the accelerations experienced in rail by examining instrumented railcars of nuclear fuel casks. Hydrogen studies were examined that focused on steel pressure hardware with an emphasis on fatigue, fast loading rates, and low temperatures. A simplified fatigue assessment was performed to examine design cycles for three different hydrogen components: stainless steel tubing, stainless steel cryogenic tanks, and gaseous pressure vessels. The assessments were idealized and used bounding cases of accelerations in both normal rail conditions and coupling events. In normal shock and vibration environments when accelerations were less than 2 g, infinite design life was calculated. In extreme shock or coupling environments, finite design life was calculated which was shown to be dependent on unsupported lengths of pressure components. It was shown that adjusting the unsupported length can reduce the bending stress thereby increasing design life.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Field Measurement of Central CO2 Heat Pump Water Heater for Multifamily Retrofit

Domestic hot water heating of multifamily buildings accounts for a substantial portion of the energy load of existing buildings. This load is made up of both the energy required to produce hot water and the energy needed to maintain the temperature of the heated water within a building’s distribution piping so that heat can be promptly delivered to building occupants as needed. Properly designed heat pump water heater (HPWH) systems have the ability to improve efficiency in both water heating and temperature control operations. Further, CO2 heat pump technology reflects a shift away from traditional refrigerants and toward refrigerants with low global warming potential (GWP). In this paper’s case study, a design consisting of multiple CO2 heat pump water heaters (commonly used in single-family homes) with a novel “swing tank” was proposed to meet the demand for domestic hot water heating and recirculation loop temperature maintenance. The proposed design was applied to the retrofit of a 60-unit, low-rise, multi-family building located in the Pacific Northwest of the United States. The purpose of this paper is to verify the performance of the system including the proposed “swing tank” in a centralized SHW system using CO2 HPWH. It also provides practical information and lessons learned from the retrofit project. Long-term monitoring data showed that the system had a coefficient of performance (COP) of three or greater and provided an average of 20 gallons of hot water per day per apartment. The results of this work indicate that residential-scale CO2 HPWH equipment and a “swing tank” design can efficiently provide domestic hot water heating and temperature maintenance for mid-sized multifamily buildings.

Banks, Adria↗

DOE OSTI2022

Assessment of the Effectiveness of Three Aftermarket Gasoline Fuel Stabilizers in Preventing Gum Formation and Loss of Oxidation Stability

We note that fuel stabilizers have long been marketed to consumers to prevent oxidation and gum formation. In the past, gasoline storage for long periods of time was commonly limited to off-road equipment that was used infrequently. Cars and trucks that were driven regularly consumed the fuel in their tanks rapidly enough to avoid excessive fuel aging. However, plug-in hybrid electric vehicles (PHEVs) may be operated frequently without engine operation, raising the possibility that fuel may be stored in the tank for longer periods of time. Studies of the oxidation of gasoline have provided scientific understanding of the process, but there is little if any scientifically backed information aimed at aiding consumers in assessing the need to use an aftermarket fuel stabilizer if they anticipate lengthy periods of fuel storage in their fuel tank. This study was conceived to address this information gap by evaluating three aftermarket stabilizer products alongside baseline gasoline using sealed samples over a period of 12 months of aging. The aging was carried out under ambient temperature conditions with an additional series of samples kept in refrigerated storage. Analyses of vapor pressure, copper strip corrosion, oxidation stability, existent gums, and potential gums were carried out using standard ASTM tests to evaluate the samples as aging progressed. The results show that baseline gasoline remained compliant with relevant specifications to at least 12 months of aging without the use of aftermarket stabilizer additives. Use of two of the aftermarket additives increased the oxidation stability of the baseline gasoline, but this added stability was not necessary to comply with gasoline specifications.

42 ENGINEERING↗

DOE OSTI2024

Long-Term Performance of Reference Electrodes in Alkaline Radioactive Waste Storage Environments

Accurate measurements of corrosion potential are important for assessing the likelihood of internal localized corrosion and stress corrosion cracking of carbon steel tanks used for storing radioactive wastes. Reference electrodes in underground radioactive waste storage tanks are challenging to deploy, and more difficult to extract and replace frequently due to radiological exposure and disposal constraints. Hence, electrodes that exhibit stable performance over long periods of immersion in these waste environments are desirable. The present study evaluates the stability of reference electrodes used in radioactive waste storage tanks over a much longer period than previously studied. Long-term tests on Ag/AgCl and Hg/HgO reference electrodes were performed in nonradioactive simulants formulated from wastes stored at the Hanford site. Electrode degradation, which was studied by various in situ and ex situ evaluation techniques, was correlated to changes in electrode fill chemistry from waste intrusion via the porous frit junction. An intentional contamination study was performed to better understand and predict contamination effects on electrode potential drift.

Materials Science↗

DOE OSTI2025

Annual carbon dioxide flux over seasonal sea ice in the Canadian Arctic

Continuous measurements of carbon dioxide (CO 2 ) flux were collected from a 10 m eddy covariance tower in a coastal-marine environment in the Canadian Arctic Archipelago over the course of a 17-month period. The extended length of data collection resulted in a unique dataset that includes measurements from two spring melt and summer seasons and one autumn freeze-up. These field observations were used to verify findings from previous theoretical and laboratory experiments investigating air-sea gas exchange in connection with sea ice. The results corroborated previous findings showing that thick ice cover under winter conditions acts as a barrier to gas exchange. In the spring, CO 2 fluxes were downward (uptake) in both the presence of melt ponds and during ice break-up. However, diurnal cycles were present throughout the early spring melt period, corresponding to the opposing influences of freezing and melting at the ice surface. Fluxes measured during melt periods confirmed previous laboratory tank measurements that showed a gas transfer coefficient of melting ice of 0.4 mol m −2 d −1 atm −1 . Open water CO 2 fluxes showed outgassing in early summer and uptake in mid-to-late summer, tied closely to trends in surface water temperature and its effect on the partial pressure of CO 2 in the water. The autumn period of the field campaign represents the first eddy covariance CO 2 fluxes measured over naturally forming sea ice. Our measurements showed mean upward fluxes (outgassing) of 1.1±1.5 mmol m −2 d −1 associated with the freezing of ice – the same order of magnitude found by previous laboratory tank experiments. However, peak flux periods during ice formation had measured fluxes that were a factor of 3 higher than the tank experiments, suggesting the importance of natural conditions (e.g., wind) on air-ice gas exchange. Conducting an Arctic-wide extrapolation we estimate CO 2 outgassing from the freezing period to be a counterbalance equivalent to 5 to 15 % of the magnitude of the estimated Arctic CO 2 sink. Overall, there was no evidence of dramatically enhanced gas exchange in marginal ice conditions as proposed by previous studies. Although the different seasons showed active CO 2 exchange, there was a balance between upward and downward fluxes at this specific location, resulting in a small net CO 2 uptake over the annual cycle of −0.3 g C m −2 .

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Modular nuclear reactors including fuel elements and heat pipes extending through grid plates, and methods of forming the modular nuclear reactors

A modular nuclear reactor comprises a plurality of sections arranged in a pattern and a side reflector material surrounding the plurality of sections. Each section includes a tank comprising a front plate, a back plate, side plates, a top plate, and a bottom plate. A plurality of grid plates are located within the tank. Each grid plate comprises a plurality of apertures and is vertically separated from an adjacent grid plate. The tank further includes a plurality of fuel elements extending through each grid plate. A plurality of heat pipes extend through each grid plate, the top plate, and an upper reflector. Methods of forming the modular nuclear reactor are also disclosed.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2021

A Predictive Model for Offgas Composition in Waste Glass Melters - Spring 2021 SULI General Audience Abstract

Approximately 56 million gallons of nuclear waste are currently stored in 177 underground storage tanks at the Hanford site in Washington state. A portion of the tank waste is targeted for immobilization by converting the nuclear waste to borosilicate glass through a process called vitrification. During vitrification, emissions are produced in addition to the intended glass product. These emissions, contained in a volume above the molten glass called the plenum, are composed of water vapor, air components, aerosols, particulates, and other gaseous species that result from evaporation, reactions, and air influx. The formation of these gasses causes the surface of the glass to foam. To reduce foaming, sucrose is added to the waste stream before the conversion to glass. Sucrose also reduces the formation of hazardous gasses in the plenum including nitrous oxides, NOx, and carboxides, COx. However, if excess sucrose is present, the reactions that produce the gasses in the plenum will be incomplete, and increased levels of NOx and COx can be observed. The Waste Treatment and Immobilization Plant at the Hanford site is equipped with the technology to treat the plenum emissions. Though many tests have been run to determine the presence of particulates in the plenum emissions, there is does not exist an established method to confidently predict the composition of the gaseous species in the plenum prior to treatment without physical testing. A model was created in the process modeling software Aspen Plus to predict the composition of NOx and COx in the plenum. The model employs a constant stirred tank reactor and user-defined reaction chemistry to determine the plenum composition. To verify the model, the offgas predicted by the model were compared to available offgas data for ten different feed compositions. It is demonstrated that the developed Aspen Plus model is capable of predicting the composition of NOx and COx in the plenum.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Optical monitoring to detect corrosion of power grid components

A corrosion monitoring system includes one or more objects coupled to respective portions of a transformer tank. The one or more objects are configured to corrode before the respective portions of the transformer tank. At least one optical sensor is coupled to each of the objects. The at least one optical sensor has an optical output that changes in response to strain of the object. An analyzer is coupled to the at least one optical sensor. The analyzer is configured to perform one or more of detecting and predicting corrosion of the transformer tank based on the output of the at least one optical sensor.

Teepe, Mark R.↗

DOE OSTI2021

Optical monitoring to detect contamination of power grid components

A monitoring system includes an array of optical sensors disposed within a transformer tank. Each optical sensor is configured to have an optical output that changes in response to a temperature within the transformer tank. An analyzer is coupled to the array of optical sensors. The analyzer is configured to determine a sensed temperature distribution based on the sensed temperature. The sensed temperature distribution is compared to an expected distribution. Exterior contamination of the transformer tank is detected based on the comparison.

Mostafavi, Saman↗

DOE OSTI2022

Gaseous hydrogen storage system with cryogenic supply

A gaseous hydrogen storage and distribution system with a cryogenic supply and a method for the cryogenic conversion of liquid hydrogen into high-pressure gaseous hydrogen are provided. The gaseous hydrogen storage and distribution system includes pressuring liquid hydrogen from a cryogenic tank using a low pressure liquid pump before vaporization within a relatively small vaporizer. The resulting high pressure gaseous hydrogen is transferred to a plurality of storage tanks at ambient temperature according to a desired fill sequence. The high pressure hydrogen gas is subsequently distributed from the storage tanks through a hydrogen fueling dispenser according to a desired dispensing sequence. The present system and method provide improvements in operational safety, eliminates the use of high pressure gas compressor, and minimizes boiling off and ventilation losses at a reduced cost when compared to existing thermal compression storage systems.

Feng, Zhili↗

DOE OSTI2022

Optical monitoring to detect corrosion of power grid components

Teepe, Mark↗

DOE OSTI2023

Optical monitoring to detect contamination of power grid components

Mostafavi, Saman↗

DOE OSTI2020

Sulfonamide and Sulfonamido-phenol Ligands for Extraction of f-Elements from Alkaline High-Level Waste

Alkaline High Level Waste (HLW) has been accumulated at Hanford and Savannah River Sites as a result of reprocessing for nuclear weapons production during the cold war. A large volume (∼100 MGal) has been accumulated in carbon steel tanks at Savannah River (SRS) and Hanford. The tank waste contains three separate phases generated when NaOH was added to previously acidic Purex raffinates: 1-2 Supernatant liquid, salt-cake, and sludge. The sludge consists mainly of insoluble hydroxides of transition metals while the supernate and salt-cake contain caustic-soluble materials, including salts of highly radioactive fission products Cs(I) and Sr(II). Current treatment of alkaline HLW in SRS includes: i) The Actinide Removal Process (ARP), which is based on sorption of {sup 90}Sr and Actinides (An) on monosodium titanate (MST), also known as 'alpha-strike' process, followed by ii) Caustic Side Solvent Extraction (CSSX),4 which is used for the extraction of {sup 137}Cs by modified calixarenes in a hydrocarbon diluent. Residual actinides in some tanks are removed after CSSX by an additional ARP process commonly referred to as 'alpha-finishing'. Despite the success of ARP for Sr and An removal, as it is a sorption process, it represents the kinetic bottleneck of integrated salt waste processing. Hence potential introduction of additional organic ligands for actinide extraction (in a modified CSSX process) could simplify the overall integrated process, making it more efficient and economical, with less titanate needed and shorter sorption time, as some of the actinide component would be removed during CSSX. In this study tri-sulfonamide and o-sulfonamido-phenol (mono-sulfonamide) ligands have been studied as extractants for Sm(III), which is being used as an Am(III) surrogate. Our prior studies in the group using a tri-sulfonamide (iPr-tsa-B) showed favorable extraction for Sm(III) nitrate salts from alkaline solutions. Mono-sulfonamides possess similar orientation of binding sites to pyrocatechols, which have been found to be good ligands for Am(III) binding and extraction from alkaline media. Tri-sulfonamide of the type iPr-tsa-B6 (1 mM in CH{sub 2}Cl{sub 2} solution) was studied for Ln{sup 3+} extraction using Sm(NO{sub 3}){sub 3}.6H{sub 2}0 (10 and 25 μM) in alkaline solution of NaOH (0.05, 0.1, 0.2, 0.3 mM) / 0.1 M NaNO{sub 3}. Stripping of the organic phase was done using 0.1 M HNO{sub 3} and quantification of Sm{sup 3+} was done using ICP-OES at 359.3 nm. The need to improve stability of the complex led to synthesis of compounds with N-donor site closer to the central benzene ring to facilitate cation-π interactions. Synthesis of tri-sulfonamide type A: a) Chloromethyl methyl ether, SnCl{sub 4}, CH{sub 2}Cl{sub 2}, 0 deg. C, N{sub 2}, 4 h, 57%; b) NaN{sub 3}, reflux in H{sub 2}O/acetone for 22 h, 80%; c) PPh{sub 3}, THF/H{sub 2}O, 22 h, 79%; d) p-toluene sulfonyl chloride, Et{sub 3}N, 1,2-DCE, 22 h. Extraction: Sm(NO{sub 3}){sub 3}.6H{sub 2}O (2 mM) in 5 ml of aqueous NaOH (pH 10.5 - 14) + 6 ml of CH{sub 2}Cl{sub 2} solution of msa (20 mole equiv.) were rotated on a wheel (60 rpm; 20 h). Stripping: 5 ml of 0.1 M HNO{sub 3} + CH{sub 2}Cl{sub 2} solution of msa (after extraction, centrifugation and filtration) was rotated on the wheel (60 rpm; 20 h). Sm{sup 3+} was quantified using UV-Visible spectrophotometry.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

A Dose Assessment Model for Radioactive Waste Exposed by Gully Erosion at West Valley - 20513

The Western New York Nuclear Service Center (WNYNSC), located approximately 48 km south of Buffalo, New York, is the site of a former nuclear fuel reprocessing and radioactive waste disposal facility. Spent nuclear fuel was processed there from 1966 to 1972, leaving behind radioactive and chemical wastes in two disposal areas and a waste tank farm. Site operations also resulted in releases of radioactivity to site soils, groundwater, and to surface waters draining the site. The New York State Energy Research and Development Authority (NYSERDA) and the U.S. Department of Energy (DOE) are collaborating in a process of decision making for decommissioning those facilities remaining at the WNYNSC following the completion of Phase 1 decommissioning. Neptune and Company, Inc. (Neptune) was contracted to develop a probabilistic performance assessment (PPA) computer model to assist the agencies in this process. The PPA Model includes a contaminant transport component focusing on the movement of contaminants within and among environmental media including groundwater and surface water transport, contaminant translocation by plants and animals, diffusion, and erosion. The model also includes evaluation of potential exposure and health effects for a Resident Farmer exposure scenario, where the Resident Farmer represents a critical group, described as that group of individuals reasonably expected to receive the greatest exposure to residual radioactivity for any applicable set of circumstances. The West Valley Site is located in the glaciated Allegheny Plateau region of western New York State. The waste reprocessing and disposal areas were constructed on a relatively fat area of plateau dissected by drainages of Buttermilk Creek, including Erdman Brook, Franks Creek, and Quarry Creek. An important aspect of the contaminant transport component of the PPA model is consideration of erosive processes such as slumping of the stream slopes and the advance of gullies from these streams. These erosion processes remove material from the plateau, growing the size of the creek valleys and making them wider and deeper. Of particular interest for the impact of erosion is radioactive waste contained in the Nuclear Regulatory Commission (NRC)-Licensed Disposal Area (NDA), the New York State-Licensed Disposal Area (SDA), and residual radiological inventory in the underground storage tanks at the Waste Tank Farm (WTF). The PPA Model is organized around geographically-defined facilities which were constructed upon the plateau, including the NDA, SDA, and WTF. Ongoing stream erosion processes will potentially transfer radioactive waste and residual inventory from these facilities to the ground surface on adjacent hillslope areas where erosion has breached the facility. Hence, it is important to evaluate the consequences of potential exposures to a Resident Farmer on the hillslopes below a breached facility. Two interrelated aspects of the dose assessment model related to hillslope exposure are discussed: 1) representation of the physical processes related to transport of radionuclides from facilities onto the hillslopes, and from the hillslopes into adjoining creeks where contaminated material migrates downstream with surface water and sediment, and; 2) adaptation of the activities associated with the Resident Farmer scenario to assess potential exposures to contamination in the hillslope areas. This discussion will cover the conceptual basis of the hillslope exposure and transport models, and also implementation in the PPA computer model. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

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.↗