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DOE OSTI2024

International Collaboration Activities in Geologic Disposal Research (FY24 Progress Report)

This report describes the FY24 status of international collaboration regarding geologic disposal research in the Office of Spent Fuel and Waste Science and Technology (SFWST) in the Department of Energy’s (DOE) Office of Nuclear Energy (NE). The mission of SFWST is to provide confidence in the safe long-term management of the nation’s spent nuclear fuel and high-level radioactive waste by reducing uncertainty and advancing technology for extended storage, transportation, and geologic disposal.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Development of local-power-free, remote α -particle detection using optical fibers

We demonstrate the application of fluorescence optical fiber coupled to a telecom grade fiber as a sensor for alpha particles using alpha-specific ZnS(Ag) scintillation materials whose wavelength is down-shifted into a low-loss region of the telecom grade fiber transmission band. Telecom-grade fiber optics offer a solution for sensing alpha radiation in deep repositories and cask storage for radioactive materials due to the stability of SiO 2 under normal environmental conditions and its relative radiation hardness at low radiation doses. Long-term nuclear waste storage facilities require sensors for the detection of leakage of radioactive materials that are maintenance-free, do not require power and can survive with no ‘wear out’ mechanisms for decades. By accomplishing the wavelength transformation, we maximize efficiencies in the detection of α-particles and signal transport and can detect alpha scintillation at distances on the order of >1 km with a sensor that is ~3% efficient and can be easily scaled as a sensor array. This paper describes the construction and testing of the sensor including manufacture of the controlled thickness films, verification of the wavelength shift from 450 to 620 nm and optimization of the sensitivity as a function of thickness. We also model the relative sensitivity of the film as a function of film thickness, and we demonstrate a signal-to-noise ratio of 10 at a range of greater than 1 km.

alpha particles↗
DOE OSTI2020

BWR Spent Nuclear Fuel Acquisition and Testing to Support DOE-NE High Burnup Spent Fuel Data Project

The Office of Spent Fuel and Waste Disposition (SFWD) within the US Department of Energy (DOE) Office of Nuclear Energy (NE) established the Spent Fuel and Waste Science and Technology (SFWST) campaign to conduct research and development (R&D) activities related to the storage, transportation, and disposal of spent nuclear fuel (SNF) and high-level radioactive waste. The SFWST program was created within SFWD to address issues of extended or long-term SNF storage and transportation. Some near-term objectives of SFWST are to use a science-based, engineering-driven approach to: Support the enhancement of the technical bases to support the continued safe and secure dry storage of SNF for extended periods; Support the enhancement of the technical bases for retrieving SNF after extended dry storage; Support the enhancement of the technical bases for transporting high burnup (HBU) fuel and transporting low burnup fuel and HBU fuel after dry storage DOE-NE, in partnership with the Electric Power Research Institute, developed the High Burnup Spent Fuel Data Project to perform a large-scale demonstration and laboratory-scale testing of HBU pressurized water reactor (PWR) fuels (exceeding 45 gigawatt-days per metric ton of uranium [GWd/MTU]). Under this project, 25 sister rods—which are rods that have the same design, power histories, and other characteristics—were removed from assemblies at the North Anna Nuclear Power Station and sent to Oak Ridge National Laboratory (ORNL) in January 2016. ORNL performed detailed nondestructive examination (NDE) on all 25 rods. The NDE consisted of visual examinations, gamma and neutron scanning, profilometry and rod length measurements, and eddy current examinations. After completing the NDE, 10 of the sister rods were delivered to Pacific Northwest National Laboratory (PNNL) in a NAC International, Inc. legal-weight truck cask in September 2018 for destructive examination (DE). To date, SFWD work has focused on the PWR fuel that is part of the Sister Rod Test program. No boiling water reactor (BWR) fuel has been tested in the program, and the data needs that were identified for the PWR fuel have not been collected for BWR fuel. The goal to obtain six to nine BWR rods and test them at ORNL will support closing this important data gap. BWR fuel comprises approximately 56% of the total fuel assemblies currently in storage at nuclear power plants in the United States. BWR nuclear fuel and cladding designs and manufacturing are significantly different from PWRs. Differences include the following: BWR fuel pellets are larger than PWR pellets; Variations of Zircaloy-2 (including liners) are used instead of the Zircaloy-4 cladding materials used in PWRs; Clad manufacturing and stress-relief processes are different between PWRs and BWRs; The fuel rod dimensions are different because larger rod diameters and thicker cladding are used in BWRs; BWR fuel typically has lower internal rod pressures and sees vastly different operating conditions than PWR fuel (i.e., two-phase flow); BWR assemblies are “canned,” meaning each assembly is surrounded by a metal fuel channel; BWR cladding is often composed of an inner pure Zr liner that has widely different mechanical properties than the Zircaloy-2 alloy and exhibits a stronger affinity for hydrogen; The BWR SNF generally has more total hydrogen in the cladding/liner than typical PWR fuel; The construction of the PWR and BWR assemblies is vastly different; BWR rods are solidly attached to the assembly nozzles and experience a much different vibration and shock load than PWR rods, which are “floating” within a grid system attached to guide tubes, and the rods sit loosely on the bottom end plates. These numerous differences will affect the way the BWR SNF responds under dry storage preparation processes (e.g., vacuum drying) and during transportation. The results collected in the PWR experimental program must be compared with a subset of similar data collected on BWR SNF to establish a technical basis for whether the larger PWR database is sufficient to bound the BWR SNF end-of-life conditions as is currently assumed for several fuel/clad properties. Changes that occur in both fuel types at HBU could exacerbate any mechanical property differences. As the fuel burnup increases, several changes occur that might affect the performance of the fuel, cladding, and assembly hardware in storage and transportation. These changes include increased cladding corrosion layer thickness, increased cladding hydrogen content, increased cladding creep strains, increased fission gas release, and the formation of the HBU structure at the surface of the fuel pellets. The Nuclear Regulatory Commission (NRC) limits the current maximum rod-averaged burnup to 62 GWd/MTU due to these changes and the lack of data at higher burnups.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Optimization of Dry Storage Canister Cutting Operations - 20534

A recent project investigated the optimal cutting method for the opening of a welded dry storage/shielded canister (DSC) or dual purpose canister (DPC) containing Used Nuclear Fuel (UNF). Due to the lack of a disposal path for UNF in the U.S., the majority of UNF is currently moved into welded DSCs and DPCs designed by Orano TN, NAC, and Holtec. As the DSCs/DPCs were neither designed nor licensed for disposal and may not be able to be emplaced in a geologic repository due to physical emplacement constraints, near-term thermal limitations, or long-term criticality issues, the UNF in these existing DSCs/DPCs may need to be repackaged into transportation, aging, and disposal canisters (TADs), generic standard TADs (STADs), transportation casks, new cask/canister systems, and/or cask/canister/package systems suitable for disposal. These DSCs/DPCs may also be opened to simply remove the UNF in preparation for recycling, re-storage, or placement into a waste package suitable for disposal. Regardless of need, the DSCs/DPCs would require to be cut open by a potentially large scale operation. This project examined the multiple means for cutting welded metal systems and considered several factors to determine an optimal approach. Issues arose around some of the cutting approaches when applied to systems with 2 or 3 lids and with pre-cutting gas testing required. The resulting preferences in cutting methods with an optimized application for the opening of DSCs/DPCs are presented. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Evaluating Liquid Waste Transfers and their Impacts to the SRS Tank Farm to Support Operations and Closure

The Liquid Waste (LW) contractor at the Savannah River Site, Savannah River Mission Completion (SRMC), supports the storage, processing, and safe disposition of legacy, radioactive liquid waste. The LW Tank Farms contain approximately 127 million liters (33.5 million gallons) of liquid waste within 43 active, underground waste tanks. To meet mission critical milestones for the closure of waste tanks and processing of 34 million liters (9 million gallons) of salt waste per year by the LW Salt Waste Processing Facility (SWPF), an increase in Tank Farm operations, including waste tank transfers, is required. Waste is compiled in salt and sludge batches in the Tank Farms and transferred to SWPF and the Defense Waste Processing Facility (DWPF) for treatment. All waste tank transfers, such as waste removal and batch compilation transfers, must be pre-evaluated to ensure Documented Safety Analysis (DSA) requirements are met via Evaluated Transfer Approval Forms (ETAFs). Facility conditions and configurations may change as a result of a waste transfer. These changes must be reflected in the Tank Farms Emergency Response Datasheet (ERD), which contains data utilized for operation and emergency situations.

Peterson, Shelby R.↗
DOE OSTI2025

FY25 Organic Evaporation Testing in Support of Hanford Sample-and-Send

The Hanford Waste Treatment and Immobilization Plant (WTP) is being built to treat and immobilize the approximately 56 million gallons of radioactive mixed waste stored in 156 underground storage tanks. The baseline method for immobilization of Low-Activity Waste (LAW) is vitrification, but additional immobilization capacity is needed to supplement the initial LAW melters. Additionally, efforts are being undertaken to accelerate the disposition of Pre-Treated Waste (PTW) in Hanford’s West Area. An alternative cementitious waste form is being investigated as an alternative 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 PTW and LAW is high enough, treatment may be needed to destroy or remove said organics to make a waste form compatible with disposal in a mixed low level waste landfill. This work evaluates evaporation as a potential avenue for treatment of LDR organics to eliminate the impediment and permit possible use of a cementitious waste form.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Disposition Options for Sodium Cooled Fast Reactor (A White Paper)

The sodium-cooled fast reactor (SFR) design concept is one of the six classes of nuclear reactors in the GenIV initiative. SFRs are uranium or plutonium-fueled reactors operating in the fast neutron spectrum using liquid sodium as the coolant. SFRs can be designed as a breeder reactor or actinide-burning reactor in addition to operating the thorium fuel cycle. While having different fuel designs, the anticipated waste streams, and the necessary management strategies for spent nuclear fuel (SNF) and radioactive wastes from SFRs are very similar. This includes the SNF, activated sodium coolant, in-core stainless-steel components, piping, resins and filters, solidified liquid waste, contaminated equipment, and other radioactive wastes. Modern SFR designs are based on a long and rich operating history of several liquid-metal-cooled fast reactors with sodium coolant. Several of these reactors have been shut down, the fuel has been placed in safe storage, and they have undergone some degree of decommissioning. As such, there is significant experience in the management of the SNF and radioactive wastes associated with operating these reactors. This white paper will identify the definitions and regulations that apply to the safe and secure management, storage, and disposal of radioactive waste and identify the key radioactive waste streams from SFRs. Idaho National Laboratory has significant experience in the management of the SNF from the SFR predecessors. This experience should form the basis for the management and disposition efforts of the radioactive waste from any new SFR-type small modular reactor or microreactor intended for deployment at the Idaho National Laboratory Site

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

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

The Hanford site has approximately 56 million gallons of radioactive mixed waste stored in 177 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 to supplement vitrification. However, one impediment to a cementitious waste form is the presence of Land Disposal Restricted (LDR) organic chemicals in tank waste. This work evaluates potential avenues to eliminate that impediment to permit possible use of a cementitious waste form and work towards a decision whether additional LDR organic pretreatment would be required. Savannah River National Laboratory (SRNL) performed testing using simulants to examine evaporation as a method to remove some prevalent organics from LAW. Spiking the caustic LAW simulant with selected regulated organic chemicals found one that clearly decomposes because of caustic instability. Oxidation testing of other organic chemicals found some LDR organics degrade as desired and others are stable in the presence of peroxide and permanganate. In addition to studies with simulants, a literature review was performed to evaluate radiological stability of LDR organics. Descriptions of the experimental details, equipment, and results are included in this report. Evaporation testing consisted of preparing the 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) and also at atmospheric pressure. 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. Organic chemicals were chosen for the work with a consideration of how their volatility compares with that of methanol. This was done by comparing the ratio of the pure water Henry’s law coefficient (K h ) of methanol to that of the compound in question (hereafter termed the K h ratio), where ratios above unity indicated less volatility than methanol. Methanol was chosen because it is a common regulated chemical with relatively low volatility but which has been removed by evaporation in previous laboratory work. While organic separation results depend on evaporator design, laboratory experiments verified that organic partitioning to the overhead condensate stream by evaporation is a practical process. The work reported here found difficulties in quantitative analysis of the organic chemicals in aqueous samples. Most of the time there was insufficient analysis to close a mass balance for evaporator runs, but qualitative evidence of carryover was obtained. The methods were also able to show whether organic chemicals were susceptible or resistant to solution oxidation in permanganate or hydrogen peroxide tests.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

An Evaluation of the Impact of Glycolate and Glycolate Mitigation on the Defense Waste Processing Facility Recycle Diversion Project Flowsheet

The Savannah River Site (SRS) Defense Waste Processing Facility (DWPF) processes radioactive High Level Waste (HLW) sludge solids from the Concentration, Storage, and Transfer Facilities (CSTF); which includes the SRS Tank Farm and Evaporator facilities, and a concentrated Cs-137 laden stream and a Monosodium Titanate (MST) and sludge solids stream from the SRS Salt Waste Processing Facility (SWPF). The waste is chemically adjusted with acids and reductant (currently with 50 wt.% nitric acid and ~90 wt.% formic acid, but eventually formic acid will be substituted with ~70 wt.% glycolic acid), and frit is added so that a durable, borosilicate glass waste form can be produced when the material is vitrified in the melter. As a result of the evaporation of water during both the melter feed preparation and the melter feed vitrification steps in DWPF, a recycle waste stream is generated, neutralized, and sent back to the CSTF. The recycle waste is a dilute aqueous stream originating from the collection of condensate liquids containing some minor sludge, MST, and frit solids and other waste components resulting from melter feed entrainment during foamover events and transfer of volatile species into the condensate. The recycle stream volume is significant and is expected to approach 3 million gallons per year once SWPF reaches full operation, requiring the use of multiple large CSTF tanks for storage. The recycle waste is currently collected in the SRS Tank Farm and periodically evaporated in the 242-16H (2H) Evaporator to conserve storage space.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Synthesis and Single Crystals of Refractory Oxides of Lanthanides and Thorium

At the completion of this program, we can report that we developed a considerable degree of technical improvements in our ability to perform hydrothermal reactions at high temperatures and pressures. We can now routinely perform reactions at 700-750°C and 200 MPa. Currently we are in the process of exploiting this new technology synthesizing a range of exotic new materials investigating relatively poorly understood materials. Our initial efforts focused on the chemistry of rare earth oxides with tetravalent and pentavalent oxides. We recently published a study of the lanthanides with Nb 5+ and Ta 5+ ions, where we grew oxides such as RENdO 4 and RETaO 4 as high quality single crystals. These compounds were targeted as potential hosts for luminescent and scintillation materials, particularly given that they are among the densest oxide hosts and hence have good potential as absorbers for high energy radiation like X-rays and gamma rays. We also isolated a range of unusual new rare earth tantalates with very complex structures. indicating that the chemistry is very sensitive to conditions. We performed some fairly comprehensive examinations of the solid-state chemistry of rare earth ions with various tetravalent metal ions especially Si 4+ , Ge 4+ , Sn 4+ and Ti 4+ . Given the potential role of rare earth silicates in immobilizing radioactive waste elements in long-term storage, and the similarity of our hydrothermal fluids with known geological conditions, this chemistry continues to be relevant. We prepared an extensive series of new lanthanide germanates (e.g. RE 13 Ge 6 O 31 (OH), BaRE 10 (GeO 4 ) 4 O 8 ). and found that there is there is almost no overlap between the chemistry of the rare earth silicates. Stannic oxide (SnO 2 ) is much more refractory and requires higher temperatures and of mineralizer concentrations. One significant result is the growth of RE 2 Sn 2 O 7 pyrochlore single crystals. These are of interest because the rare earth stannate pyrochlores are known to display a wide range of magnetic frustration such as spin ice behavior. We grew high quality single crystals of rare earth germanate and stannate pyrochlores and this led to a collaboration with Professor Kate Ross at Colorado State. Preliminary measurements, indicate that the crystals contain no detectable defects or site disorder. Initial neutron diffraction on single crystals was performed at Oak Ridge, and more detailed experiments involving the Ross group are underway at both NIST and ORNL. This particular chemistry has turned out to be the most potentially significant work on this project and the collaborative effort with Prof. Ross is the topic of a DoE renewal project on quantum materials. Our initial foray into the hydrothermal chemistry of rare earth titanates has also been very promising and a range of cubic and polar ferroic phases of the light rare earths RE 2 Ti 2 O 7 (RE = La - Pr) in the P2 1 phase. We also discovered an interesting new phase Ce 2 Ti 4 O 11 that can have implications in heavy metal immobilization and storage. along with a series of new rare earth titanates (La 5 Ti 4 O 15 (OH) Sm 3 TiO 5 (OH) 3 and Lu 5 Ti 2 O 11 (OH) with exceptionally complex structures. One interesting sidelight has been high temperature hydrothermal chemistry terbium, including the growth of large crystals of TbO(OH). This is not a new compound but it is the first time it has been grown as large single crystals. The Tb atom density is almost as high as that in Tb 2 O 3 and has a very high Verdet constant (ca. 70), making it a very attractive candidate as a Faraday rotator. Unfortunately it is not in a cubic structure but he material is hard, stable, pure and inexpensive, so should still be an attractive Faraday oscillator. We recently received a patent on this material. We also synthesized K 2 Tb(Ge 2 O 7 ) containing stable octahedral Tb 4+ ions, which appears to be the first example of a well-characterized Tb 4+ complex. Given that Tb 4+ has been proposed as a benign surrogate for more treacherous tetravalent ions such as Cf 4+ and Bk 4+ , we think that Tb 4+ silicates can be a particularly useful study for actinide immobilization and related work. We also began reaction studies with rare earths and both ReO 2 and RuO 2 . These resulted in large single crystals of species like RE 5 Ru 2 O 12 , RE 4 Re 2 O 11 , REReO 4 and RE 2 ReO 5 . Several of these samples have already been sent to ORNL for magnetic and neutron diffraction studies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Integration of the Back End of the Nuclear Fuel Cycle

Management of spent nuclear fuel and high-level radioactive waste consists of three main phases – storage, transportation, and disposal – commonly referred to as the back end of the nuclear fuel cycle. Current practice for commercial spent nuclear fuel management in the United States (US) includes temporary storage of spent fuel in both pools and dry storage systems at operating or shutdown nuclear power plants. Storage pools are filling to their operational capacity, and management of the approximately 2,200 metric tons of spent fuel newly discharged each year requires transferring older and cooler spent fuel from pools into dry storage. Unless a repository becomes available that can accept spent fuel for permanent disposal, projections indicate that the US will have approximately 136,000 metric tons of spent fuel in dry storage systems by mid-century, when the last plants in the current reactor fleet are decommissioned. Current designs for dry storage systems rely on large multi-assembly canisters, the most common of which are so-called “dual-purpose canisters” (DPCs). DPCs are certified for both storage and transportation, but are not designed or licensed for permanent disposal. The large capacity (greater number of spent fuel assemblies) of these canisters can lead to higher canister temperatures, which can delay transportation and/or complicate disposal. This current management practice, in which the utilities continue loading an ever-increasing inventory of larger DPCs, does not emphasize integration among storage, transportation, and disposal. This lack of integration does not cause safety issues, but it does lead to a suboptimal system that increases costs, complicates storage and transportation operations, and limits options for permanent disposal. This paper describes strategies for improving integration of management practices in the US across the entire back end of the nuclear fuel cycle. The complex interactions between storage, transportation, and disposal make a single optimal solution unlikely. However, efforts to integrate various phases of nuclear waste management can have the greatest impact if they begin promptly and continue to evolve throughout the remaining life of the current fuel cycle. A key factor that influences the path forward for integration of nuclear waste management practices is the identification of the timing and location for a repository. The most cost-effective path forward would be to open a repository by mid-century with the capability to directly dispose of DPCs without repackaging the spent fuel into disposalready canisters. Options that involve repackaging of spent fuel from DPCs into disposalready canisters or that delay the repository opening significantly beyond mid-century could add 10s of billions of dollars to the total system life cycle cost.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Managing Hanford's Direct Feed Low Activity Waste Program - 20002

The Office of River Protection (ORP) is responsible for the management and completion of the River Protection Project (RPP) mission, which comprises both the Hanford Site tank farms operations and the completion and operation of the Waste Treatment and Immobilization Plant Project. The RPP mission is to safely retrieve, treat, and immobilize Hanford's high-level and low-activity tank waste and close the tank farms to protect the Columbia River. The Direct-Feed Low-Activity Waste (DFLAW) Program is a major subset of the overall RPP mission, providing disposition of low-activity waste. The scope is to retrieve, treat, and immobilize the low-activity waste at the Low-Activity Waste Facility. DFLAW will begin operations no later than December 2023. The DFLAW Program overarches a suite of individual projects, activities, and infrastructure upgrades. The major projects and activities include multiple contractors under both ORP and the Richland Operations Office, underscoring the need for effective integration, coordination, and collaboration. The objectives of the DFLAW Program leadership team are to: - Effectively coordinate and integrate the projects that comprise the DFLAW Program - Manage the interfaces between the projects so that the integrated DFLAW Program is completed successfully - Ensure the DFLAW portfolio of projects operate as required without gaps or conflicts at the interfaces. DOE is accomplishing these objectives through a newly established leadership model that integrates the DOE and contractor work streams and promotes a teamwork model to enable collaborative success. Long considered one of the most formidable cleanup challenges at Hanford, the Department of Energy and its contractors are on the verge of achieving a cleanup commitment that has been decades in the making. DOE is preparing to vitrify (turn to glass) Hanford's chemical and radioactive tank waste using the DFLAW process. The Modified Consent Decree milestone for completing hot commissioning of the Hanford Site's Low- Activity Waste Facility is Dec. 31, 2023. While this milestone may seem distant under normal project management circumstances, it is a relatively short period of time for the operational and cultural transformation necessary to successfully begin treating tank waste at Hanford. Direct feed means separating the waste at a tank farm to remove the more radioactive portion (i.e., solids and cesium) so that the resulting low-activity (less radioactive) waste can be fed directly to the Waste Treatment and Immobilization Plant's Low-Activity Waste Facility. Starting DFLAW will require a singular, intensive leadership focus, along with a sustained, collective commitment to excellence and teamwork by the Department and its contractors. Major upgrades to Hanford's infrastructure will occur prior to startup. Supporting DFLAW operations requires significant integration between the DFLAW facilities - the Waste Treatment Plant, Hanford's tank farms, effluent treatment facilities, disposal facilities - and between all of the site contractors to achieve success. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Application of On-Line Monitoring and Real-Time Characterization of Low Level Waste Samples from Hanford Tanks - 20380

Waste and treatment stream characterization is an essential part of safe, efficient, and cost-effective processing of Hanford 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 Office of River Protection (ORP) progresses toward Hanford waste treatment and immobilization. The application of on-line monitoring can greatly improve operation time frames and reduce costs by providing real-time data and supporting the reduction of necessary grab sample collection. Recently, our team applied Raman online monitoring and chemometric modeling to the supernate of Hanford tank 241-AP-105, and demonstrated the quantitative measurement of nine analytes within this waste. Application of this method has been expanded to additional Hanford tank wastes, AW-102 and AP-107. The performance of the process monitoring instruments and the accuracy of the chemometric models will be assessed. On-line monitoring results will be compared to anion results determined from the current standard, ion-chromatographic and inductively coupled plasma mass spectrometry methods. Comparisons of both determined values and uncertainties of results will be presented. Results will be shared with personnel working on flowsheet interfaces for the Direct-Feed Low Activity Waste mission at Hanford. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Removal of Metal Oxides from Reactor Metals/Alloys by Laser Ablation

Storage of low and intermediate level radioactive waste in a deep geological repository (L and ILW DGR): - Large volumes of metallic waste = increased production of hydrogen gas. - Large fraction of the metallic wastes are out-of-core reactor components. - Carbon steel feeder pipes. - Radioactive contamination is concentrated within the surface oxides. - Removal of surface contaminants would lead to volume reduction of metallic waste that is stored in L and ILW DGR. - Current decontamination techniques generate large volumes of secondary waste. Objectives: Oxide removal from carbon steel using a ytterbium fiber laser (1064 nm) with a particular focus on identifying the key laser parameters that affect the removal efficiency. Advantages of laser ablation: Generate low volumes of waste, Flexibility of deployment, Remote operation. Grow an oxide film on carbon steel with the incorporation of cobalt. Optimize laser cleaning technology for the removal of surface oxides. Incorporate an oxide collection system for the ablated particles. Conclusions: Objective 1 - Simulated inactive oxides on carbon steel, using Co{sup 2+} as a surrogate for Co radionuclide. Objective 2 - Optimized laser parameters (200 MW/cm{sup 2}, 3 scans, 15 μm overlap); Complete removal of cobalt from surface and bulk metal with optimized cleaning settings. Objective 3 - Glass fiber media H14 HEPA filters had highest collection yield; High oxide collection yields (∼100%). Future Work: Further testing of the liquid trap will verify the efficacy of the HEPA filter and determine the amount of ablated oxides that pass through. Testing of the laser ablation system needs to be done on other reactor materials along with the incorporation of different transition metal cations. Improvements to the oxide collection system are required to improve collection yields.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Technology Development for Under Tank Inspection of Double-Shell Tanks - 20045

The Department of Energy (DOE) Office of River Protection (DOE-ORP) is responsible for management and cleanup of the tank farms located at the Hanford Site. Nuclear waste at Hanford is stored in 149 single-shell tanks (SSTs) and 27 double-shell tanks (DSTs). The vast majority of the liquid radioactive waste is stored in the DSTs. The 27 DSTs, located in six tank farms, were constructed from 1967 to 1986 and, compared to the SSTs, provide greatly improved protection from leakage and better accessibility for inspection. The DSTs and ancillary equipment are expected to exceed their design life before their waste is removed and sent to the Waste Treatment and Immobilization Plant. The DST Integrity Project (DSTIP) must ensure that the DST system can meet the River Protection Project mission goals. This paper provides a programmatic overview of the DSTIP with a focus on development of under-tank inspection technologies. Currently, two categories of nondestructive examination (NDE) techniques for DSTs are implemented on the Hanford site: (1) surface (SNDE) and (2) volumetric (VNDE). Further discussion on current inspection techniques is provided in this paper. The technology development approach for advanced VNDE techniques will also be generally discussed as a precursor for another more detailed WM2020 paper and presentation by PNNL. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Use of an Alternative Conceptual Model of Vadose Zone Heterogeneity to Evaluate Past Tank Leaks and Other Unplanned Releases within a Tank Farm at the Hanford Site - 20061

Washington State Department of Ecology (Ecology) requested that U.S. Department of Energy (DOE)-Office of River Protection (ORP) consider an evaluation of effects of fine-grained thin sediment layers on transport with a separate alternative conceptual model in its evaluation of the potential impact of tank leaks and other unplanned releases within the tank farm at the Hanford Site. For this alternative model, Ecology recommended that the model be developed based on the general framework of fine-grained units identified by a stakeholder group in their interpretations of variability in moisture content data collected in the vicinity of Waste Management Area (WMA) C. In discussions with DOE-ORP, Ecology acknowledged that the underlying data and interpretations of the occurrence and lateral continuity of the fine-grained thin layers identified by a stakeholder group are uncertain. However, DOE-ORP agreed to Ecology's recommendation and has provided support for the requested evaluation that involved development of an alternative model based on the general framework of the unpublished report by the stakeholder. DOE-ORP considered this evaluation to be a hypothetical evaluation of vadose zone heterogeneities at WMA C. General observations from the range of simulation cases examined in the evaluation of the effects of hypothetical vadose zone heterogeneities at WMA C are as follows. - The movement of the center of mass of the simulated plumes was generally vertically downward below the source for all simulations, including those that incorporated the hypothetical fine-grained units. - All simulations that incorporated hypothetical heterogeneity produced additional plume spreading over what was produced in simulations using Equivalent Homogeneous Media (EHM) model(s)a. The spreading resulted in a broadening of the fringes of the plume, resulting in a wider region of low concentration, but lower peak concentrations associated with the center of mass of the plume. - Simulations that used the silty-sand hydraulic properties, suggested by Ecology for the hypothetical fine-grained units, generally produced similar spreading and slightly lower peak mass flux at the water table when compared to the EHM modeling results. a The EHM-based models used at WMA C do not explicitly include small-scale fine-grained heterogeneities used in the model advocated by Ecology. - Simulations that used the silty-sand hydraulic properties, suggested by Ecology for the hypothetical fine-grained units, generally produced less spreading and an earlier arrival of mass flux at the water table when compared to the use of another set of hydraulic properties from a silty-sand sample collected at a nearby disposal facility. - The EHM representation of the vadose zone generally produced higher peak mass flux and an earlier occurrence of peak fluxes at the water table compared to all analyses incorporating additional hypothetical heterogeneity. Results of this alternative model evaluation of past leaks provided some insight into the transport effects of vadose zone heterogeneities at WMA C that helped resolve Ecology's comments and issues related to the effects of vadose zone heterogeneities on past leaks and losses from the WMA C tank farms area. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Demonstration Test Report: Vacuum Thermal Desorption (VTD) Testing to Support West Area Waste Feed Test 2

Approximately 54 million gallons of radioactive and hazardous waste are stored in underground storage tanks at the U.S. Department of Energy’s (DOE’s) Hanford Site in southeastern Washington State. The Hanford Waste Treatment and Immobilization Plant (WTP) is being constructed to immobilize the waste in glass waste forms. The baseline configuration of the WTP includes a Pretreatment Facility to separate the wastes into a small volume of high-level waste (HLW) containing most of the radioactivity and a larger volume of low-activity waste (LAW) containing most of the non-radioactive chemicals. The HLW will be converted to glass in the HLW vitrification facility for ultimate disposal at a federal repository.

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DOE OSTI2021

An Assessment of the Materials of Construction for the Transfer Lines and Unit Operations Equipment Associated with the Recycle Diversion Process

The Defense Waste Processing Facility (DWPF) processes and vitrifies radioactive waste that it receives from the Concentration, Storage, and Transfer Facility (CSTF) and Salt Waste Processing Facility (SWPF). As a result of the evaporation of water during both the melter feed preparation and the melter feed vitrification steps in DWPF, a recycle waste stream is generated, neutralized, and sent back to the CSTF. The recycle waste is a dilute water stream originating from the collection of condensate liquids containing some minor sludge and frit solids and other waste components primarily resulting from entrainment into the condensate during foam-over events. The recycle stream volume is significant and is expected to approach 3 million gallons per year once the SWPF reaches full operation. Diverting the bulk of the recycle waste stream from the CSTF is essential for the eventual closure of the waste tanks, and hence the completion of the SRS liquid waste mission.

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