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DOE OSTI2022

Thermal conversion in air of rare-earth fluorides to rare-earth oxyfluorides and rare-earth oxides

Phase transformations of seven different rare-earth fluorides (i.e., REF3) where RE = La, Ce, Pr, Nd, Tm, Yb, Lu at temperatures ranging from 400–1400°C in air were investigated with X-ray diffraction. All of the REF3 compounds first transformed to oxyfluorides and then to oxides, with the exception of CeF3, which transformed directly to an oxide. This study focuses on the phase transitions of REF3 to REOx by simple heat-treatment processes in air and shows plausibility to remove RE elements from fluoride salt streams from molten salt reactors through fluoride-to-oxyfluoride or fluoride-to-oxide conversion mechanisms, which will result in precipitation. This could be used to remove fission product poisons from molten salt reactor waste streams. A waste form option for the resulting REOx products is lanthanide aluminoborosilicate (LABS) glass. To demonstrate this NdF3 was converted to Nd2O3 and immobilized in a LABS glass.

oxyfluoride, molten salt reactors, fluoride salt w↗
DOE OSTI2019

Plutonium Migration during the Leaching of Cemented Radioactive Waste Sludges

One of the most challenging components of the UK nuclear legacy is Magnox sludge, arising from the corrosion of Mg alloy-clad irradiated metallic U fuel that has been stored in high pH ponds. The sludges mainly comprise Mg hydroxide and carbonate phases, contaminated with fission products and actinides, including Pu. Cementation and deep geological disposal is one option for the long-term management of this material, but there is a need to understand how Pu may be leached from the waste, if it is exposed to groundwater. Here, we show that cemented Mg(OH) 2 powder prepared with Pu(IV) aq is altered on contact with water to produce a visibly altered ‘leached zone’, which penetrates several hundred microns into the sample. In turn, this zone shows slow leaching of Pu, with long-term leaching rates between 1.8–4.4 × 10 -5 % of total Pu per day. Synchrotron micro-focus X-ray fluorescence mapping identified decreased Pu concentration within the ‘leached zone’. A comparison of micro-focus X-ray absorption spectroscopy (µ-XAS) spectra collected across both leached and unleached samples showed little variation, and indicated that Pu was present in a similar oxidation state and coordination environment. Fitting of the XANES spectra between single oxidation state standards and EXAFS modeling showed that Pu was present as a mixture of Pu(IV) and Pu(V). The change in Pu oxidation from the stock solution suggests that partial Pu oxidation occurred during sample ageing. Similarity in the XAS spectra from all samples, with different local chemistries, indicated that the Pu oxidation state was not perturbed by macro-scale variations in cement chemistry, surface oxidation, sample aging, or the leaching treatment. These experiments have demonstrated the potential for leaching of Pu from cementitious waste forms, and its underlying significance requires further investigation.

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

Examining Thermolytic Production of Hydrogen from Lubrication Oil

Savannah River National Laboratory (SRNL) was requested by Savannah River Remediation (SRR) to conduct testing via Technical Task Request (HR) to determine the thermolytic HGR of Mobil SHC™ 630, a lubrication oil. Currently, 35 gallons of contaminated Mobil SHC 630 is proposed for release into the recycle stream from the Defense Waste Processing Facility (DWPF) to Tank 22 and then to the 242-16H (2H) Evaporator system. Inhibited recycle waste in the Recycle Collection Tank (RCT) is transferred to Recycle Pump Tank (RPT) in the Low Point Pump Pit (LPPP) and then to the Concentration, Storage and Transfer Facilities (CSTF) H-area. The lubrication oil would be added directly to the RPT, bypassing the RCT. The current DWPF waste compliance plan for liquid transfers from the RCT to the CSTF limits the concentration of Mobil SHC 630 to <1,100 ppm which is equal to <9.3 gallons of Mobil SHC 630 when considering a 7,500 gal RCT batch with an initial Mobil SHC 630 concentration of 42 mg/L. Mobil SHC 630 is expected to be largely immiscible in the caustic aqueous waste stream. It is a blend of base oils including polyalphaolefin (PAO) base oil and additives such as triphenylphosphate and cresyl diphenyl phosphate at various concentrations (<0.25 wt%). While the base oils are expected to be largely unreactive in CSTF waste, the triarylphosphates additives would be expected to hydrolyze in the caustic waste, forming diarylphosphates and phenol. The tests described herein were governed by a single Run Plan and will determine thermolytic HGR from the caustic aqueous solution, as well as from any organic phases present.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Preliminary Evaluation of the SNF Transportation Infrastructure at Operating Commercial Nuclear Power Plant Sites - 18466

The U.S. Department of Energy (DOE) has a goal to develop solutions for the long-term, sustainable management of the nation's spent nuclear fuel (SNF) and high-level radioactive waste (HLW). The DOE Office of Nuclear Energy's (DOE-NE) Office of Integrated Waste Management (IWM) is applying integrated waste management system analysis, system engineering, and decision analysis principles to inform future decisions regarding potential future nuclear waste management system architectures. One aspect of an integrated nuclear waste management system architecture is transportation of spent nuclear fuel from the fleet of commercial nuclear reactors to interim storage and/or disposal facilities. This paper presents a preliminary evaluation of the SNF transportation infrastructure at existing commercial nuclear power plant sites. Reactor site surveys performed by DOE in the 1990's and early 2000's that described the transportation infrastructure at commercial reactor sites at that time served as the starting point for the evaluation. Geographical information systems (GIS) and available open-source information about the reactor sites were used to identify changes in the transportation infrastructure at operating commercial nuclear power plant sites. The data and schematics contained within the previous surveys were comparatively analyzed alongside the GIS tools Google Earth, Google Maps, and DOE's Stakeholder Tool for Assessing Radioactive Transportation (START) to determine potential transportation modes and to identify improvements to the transportation infrastructure that may be needed at each of the sites. The preliminary results obtained and the insight gained from this effort support both integrated waste management system architecture analyses and future planning efforts. This is a technical paper that does not take into account the contractual limitations under the Standard Contract for Disposal of Spent Nuclear Fuel and/or High-Level Radioactive Waste (Standard Contract) (10 CFR Part 961). Under the provisions of the Standard Contract, DOE does not consider spent nuclear fuel in multi-assembly canisters to be an acceptable waste form, absent a mutually agreed to contract amendment. To the extent discussions or recommendations in this paper conflict with the provisions of the Standard Contract, the Standard Contract provisions prevail. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Crystallization in High-Level Waste Glass: A Review of Glass Theory and Noteworthy Literature

There is a fundamental need to continue research aimed at understanding nepheline and spinel crystal formation in high-level waste (HLW) glass. Specifically, the formation of nepheline solids (K/NaAlSiO 4 ) during slow cooling of HLW glass can reduce the chemical durability of the glass, which can cause a decrease in the overall durability of the glass waste form. The accumulation of spinel solids ((Fe, Ni, Mn, Zn)(Fe, Cr) 2 O 4 ), while not detrimental to glass durability, can cause an array of processing problems inside HLW glass melters. In this review, the fundamental differences between glass and solid-crystals are explained using kinetic, thermodynamic, and viscosity arguments, and several highlights of glass-crystallization research, as it pertains to high-level waste vitrification, are described. In terms of mitigating spinel in the melter and both spinel and nepheline formation in the canister, the complexity of HLW glass and the intricate interplay between thermal, chemical, and kinetic factors further complicates this understanding. However, new experiments seeking to elucidate the contributing factors of crystal nucleation and growth in waste glass, and the compilation of data from older experiments, may go a long way towards helping to achieve higher waste loadings while developing more efficient processing strategies. Higher waste loadings and more efficient processing strategies will reduce the overall HLW Hanford Tank Waste Treatment and Immobilization Plant (WTP) vitrification facilities mission life.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Crystallization in High-Level Waste Glass: A Review of Glass Theory and Noteworthy Literature

There is a fundamental need to continue research aimed at understanding nepheline and spinel crystal formation in high-level waste (HLW) glass. Specifically, the formation of nepheline solids (K/NaAlSiO 4 ) during slow cooling of HLW glass can reduce the chemical durability of the glass, which can cause a decrease in the overall durability of the glass waste form. The accumulation of spinel solids ((Fe, Ni, Mn, Zn)(Fe,Cr) 2 O 4 ), while not detrimental to glass durability, can cause an array of processing problems inside of HLW glass melters. In this review, the fundamental differences between glass and solid-crystals are explained using kinetic, thermodynamic, and viscosity arguments, and several highlights of glass-crystallization research, as it pertains to high-level waste vitrification, are described. In terms of mitigating spinel in the melter and both spinel and nepheline formation in the canister, the complexity of HLW glass and the intricate interplay between thermal, chemical, and kinetic factors further complicates this understanding. However, new experiments seeking to elucidate the contributing factors of crystal nucleation and growth in waste glass, and the compilation of data from older experiments, may go a long way towards helping to achieve higher waste loadings while developing more efficient processing strategies. Higher waste loadings and more efficient processing strategies will reduce the overall HLW Hanford Tank Waste Treatment and Immobilization Plant (WTP) vitrification facilities mission life.

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

Real Time, In-line Monitoring of Hanford Tank Wastes - Year 1 Report

The team comprised of students, postdocs, early, mid and senior career scientists from Los Alamos National Laboratory, Savanah River National Laboratory, Georgia Tech and Florida International University, with the guidance of H2C, is developing a suite of in-line instruments for the Hanford high level waste (HLW) and low active waste (LAW) processes to provide near-real-time analysis of waste form physical properties and composition. The work builds on results from the recent DOE-ORP, EM Technology Development and other projects that demonstrated promise for the use of real-time in-line monitoring (RTIM) to measure chemical compositions of slurries of up to 20 weight % solids. The goal is for this instrument suite is to substantially reduce the need for sampling for process control. Sample waste, exposure associated with sample analysis, and the demand for an external laboratory facility would be greatly reduced. The throughput of waste treatment systems would be improved by elimination of the downtime caused by waiting for sample results. This translates into reduced process storage as process knowledge will be continuously updated in near-real-time. These breakthrough technologies would significantly reduce the life cycle cost and accelerate the schedule for the Hanford tank waste mission.

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DOE OSTI2020

Groundwater and Intruder Radionuclide Screening

Solid Waste Management (SWM) operates the E-Area Low-Level Waste Facility (ELLWF) where low level on-site and off-site solid waste streams are buried. The facility has been in operation since late 1994 and is currently projected to remain in operation until 2065. This facility can accommodate a broad range of waste forms resulting from the six different types of disposal unit options (i.e., varying degrees of engineered barriers → trenches to concrete vaults). This facility is currently operating under a Performance Assessment (PA) issued back in 2008, along with several subsequent supporting Special Analyses (SA). The Savannah River National Laboratory (SRNL) developed the prior PAs and SAs and has been tasked to update the facility’s PA. For operating the E-Area facility, a Waste Inventory Tracking System (e.g., WITS) is actively employed by waste generators where every radionuclide entering the facility (to be buried in one of its many disposal units) must be either directly or indirectly accounted for. Since there is a large number of radionuclides in existence (>3,000), the International Commission on Radiological Protection (ICRP-107) has provided guidance on the subset of radionuclides requiring further assessment in landfills such as the E-Area LLWF. The ICRP-107 publication provides critical radiological information on 1,252 radionuclides of 97 elements. This database is the critical starting point for developing a consistent inventory limit system. The explicit measurement and tracking of all radionuclides are not necessary when process knowledge, burial history, and radiological aspects are factored into conservative groundwater and intruder screening processes. Across the DOE complex these screening processes have been historically performed using the methodology suggested by the National Council on Radiation Protection and Measurements (NCRP) as presented in their original report (NCRP 1984) and then refined in a later report (NCRP 1996). In the recommended screening models employed within this report the traditional NCRP models are updated to better handle progeny and better reflect the known characteristics of E-Area. This improved screening process is referred to as the “NCRP-like” method. Various upgrades to the traditional NCRP methodology have been used by others (e.g., NRC funded effort by Kennedy and Strenge 1992). The more detailed models by Kennedy and Strenge (1992) were considered in this effort and are compared to the results from the more traditional NCRP-like models. The groundwater and inadvertent intruder screening analyses presented in this report start with this 1,252 radionuclide list and reduces it down to more manageable lists that are applicable to the various disposal unit types contained within E-Area. In order to reduce this starting list, some level of exposure risk must be considered acceptable. Historically, a dose (or concentration level) has been compared with a screening criterion set to 1% of a performance measure (e.g., a beta-gamma dose not to exceed the 4 mrem/yr beta-gamma performance measure x 0.01 = 0.04 mrem/yr). Thus, if a radionuclide produced a bounding or screening-level dose (or concentrations) less than the screening criterion, it could be safely removed from further consideration. Several tiers of screening and bounding level analyses have been considered in this report.

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

Groundwater and Intruder Radionuclide Screening

Solid Waste Management (SWM) operates the E-Area Low-Level Waste Facility (ELLWF) where low level on-site and off-site solid waste streams are buried. The facility has been in operation since late 1994 and is currently projected to remain in operation until 2065. This facility can accommodate a broad range of waste forms resulting from the six different types of disposal unit options (i.e., varying degrees of engineered barriers → trenches to concrete vaults). This facility is currently operating under a Performance Assessment (PA) issued back in 2008, along with several subsequent supporting Special Analyses (SA). The Savannah River National Laboratory (SRNL) developed the prior PAs and SAs and has been tasked to update the facility’s PA. For operating the E-Area facility, a Waste Inventory Tracking System (e.g., WITS) is actively employed by waste generators where every radionuclide entering the facility (to be buried in one of its many disposal units1) must be either directly or indirectly accounted for. Since there is a large number of radionuclides in existence (>3,000), the International Commission on Radiological Protection (ICRP-107) has provided guidance on the subset of radionuclides requiring further assessment in landfills such as the E-Area LLWF. The ICRP-107 publication provides critical radiological information on 1,252 radionuclides of 97 elements. This database is the critical starting point for developing a consistent inventory limit system. The explicit measurement and tracking of all 1,252 ICRP-107 radionuclides can be reduced when process knowledge, burial history, and radiological aspects are factored into conservative groundwater and intruder screening processes. Across the DOE complex these screening processes have been historically performed using the methodology suggested by the National Council on Radiation Protection and Measurements (NCRP) as presented in their original report (NCRP 1984) and then refined in a later report (NCRP 1996). In the recommended screening models employed within this report the traditional NCRP models are updated to better handle progeny and better reflect the known characteristics of E-Area. This improved screening process is referred to as the “NCRP-like” method. Various upgrades to the traditional NCRP methodology have been used by others (e.g., NRC funded effort by Kennedy and Strenge 1992). The more detailed models by Kennedy and Strenge (1992) were considered in this effort and are compared to the results from the more traditional NCRP-like models. The groundwater and inadvertent intruder screening analyses presented in this report start with this 1,252 radionuclide list and reduces it down to more manageable lists that are applicable to the various disposal unit types contained within E-Area. In order to reduce this starting list, some level of exposure risk must be considered acceptable. Historically, a dose (or concentration level) has been compared with a screening criterion set to 1% of a performance measure (e.g., a betagamma dose not to exceed the 4 mrem/yr beta-gamma performance measure x 0.01 = 0.04 mrem/yr). Thus, if a radionuclide produced a bounding or screening-level dose (or concentrations) less than the screening criterion, it could be safely removed from further consideration. Several tiers of screening and bounding level analyses have been considered in this report.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Proposed NRCDA Groundwater Pathway Conceptual Model

As requested by Solid Waste Management (SWM), this report documents the Savannah River National Laboratory’s (SRNL’s) evaluation of updated Naval Reactor waste container and inventory projections and proposes a Naval Reactor Component Disposal Area (NRCDA) groundwater (GW) pathway modeling approach for the next E-Area Low-Level Waste Facility (LLWF) Performance Assessment (PA). Two areas within the E-Area LLWF are used as disposal sites for reactor components from the U.S. Navy. Currently, components arrive by rail and are moved by crane to the 643-26E at-grade gravel disposal pad. Prior to operational closure, reactor components were stored and ultimately disposed in-place on the 643-7E NRCDA (Wilhite and Flach 2004). Naval Reactor (NR) waste is comprised of highly radioactive components consisting of activated corrosion-resistant metal alloy contained within welded thick steel casks, and auxiliary equipment primarily contaminated with Activated Corrosion Products (sometimes referred to as “crud” by the U.S. Navy) at low levels and contained within thinner-walled bolted containers. The 643-7E disposal pad, which contains 41 casks and has an interim soil cover, is closed to future receipts. The latest NR waste projections for the 643-26E disposal pad are substantially different from the original estimates due to a change in reactor maintenance. The original estimate was for 50 heavily shielded, welded casks and 50 thinner-walled bolted containers (primarily shield blocks). Currently, NR Programs project 33 heavily shielded, welded casks, of which 31 are already in-place on the 643-26E pad, and 381 thinner-walled bolted containers. In addition to new waste form projections, there have been changes in facility layout and closure plans as well as PA modeling improvements. This report documents these changes as well as key NRCDA recommendations from the 2015 PA Strategic Plan (Butcher 2016).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Low Activity Waste Feed Solids Characterization and Filterability Tests

The primary treatment of the tank waste at the DOE Hanford site will be done in the Waste Treatment and Immobilization Plant (WTP) that is currently under construction. The baseline plan for the WTP Pretreatment facility is to treat the waste, splitting it into High Level Waste (HLW) feed and Low Activity Waste (LAW) feed. Both waste streams are then separately vitrified as glass and sealed in canisters. The LAW glass will be disposed onsite in the Integrated Disposal Facility (IDF). There are currently no plans to treat the waste to remove technetium in the WTP Pretreatment facility, so its disposition path is the LAW glass. Options are being explored to immobilize the LAW portion of the tank waste, i.e., the LAW feed from the WTP Pretreatment facility. Removal of 99 Tc from the LAW Feed, followed by off-site disposal of the 99 Tc, would eliminate a key risk contributor for the IDF Performance Assessment (PA) for supplemental waste forms, and has potential to reduce treatment and disposal costs. Washington River Protection Solutions (WRPS) is developing some conceptual flow sheets for LAW treatment and disposal that could benefit from technetium removal. One of these flow-sheets will specifically examine removing 99 Tc from the LAW feed stream to supplemental immobilization. The conceptual flow sheet of the 99 Tc removal process includes a filter to remove insoluble solids prior to processing the stream in an ion exchange column, but the characteristics and behavior of the liquid and solid phases has not previously been investigated. This report contains results of testing of a simulant that represents the projected composition of the feed to the Supplemental LAW process. This feed composition is not identical to the aqueous tank waste fed to the Waste Treatment Plant because it has been processed through WTP Pretreatment facility and therefore contains internal changes and recycle streams that will be generated within the WTP process. Although a Supplemental LAW feed simulant has previously been prepared, this feed composition differs from that simulant because those tests examined only the fully soluble aqueous solution at room temperature, not the composition formed after evaporation, including the insoluble solids that precipitate after it cools. The conceptual flow sheet for Supplemental LAW immobilization has an option for removal of 99 Tc from the feed stream, if needed. Elutable ion exchange has been selected for that process. If implemented, the stream would need filtration to remove the insoluble solids prior to processing in an ion exchange column. The characteristics, chemical speciation, physical properties, and filterability of the solids are important to judge the feasibility of the concept, and to estimate the size and cost of a facility.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Sorption Modeling and Verification for Off-Gas Treatment

The project has made progress toward developing a comprehensive modeling capability for the capture of target species in off gas evolved during the reprocessing of nuclear fuel. The effort has integrated experimentation, model development, and computer code development for adsorption and absorption processes. For adsorption, a modeling library has been initiated to include (a) equilibrium models for uptake of off-gas components by adsorbents, (b) mass transfer models to describe mass transfer to a particle, diffusion through the pores of the particle and adsorption on the active sites of the particle, and (c) interconnection of these models to fixed bed adsorption modeling which includes advection through the bed. For single-component equilibria, a Generalized Statistical Thermodynamic Adsorption (GSTA) code was developed to represent experimental data from a broad range of isotherm types; this is equivalent to a Langmuir isotherm in the two-parameter case, and was demonstrated for Kr on INL-engineered sorbent HZ PAN, water sorption on molecular sieve A sorbent material (MS3A), and Kr and Xe capture on metal-organic framework (MOF) materials. The GSTA isotherm was extended to multicomponent systems through application of a modified spreading pressure surface activity model and generalized predictive adsorbed solution theory; the result is the capability to estimate multicomponent adsorption equilibria from single-component isotherms. This advance, which enhances the capability to simulate systems related to off-gas treatment, has been demonstrated for a range of real-gas systems in the literature and is ready for testing with data currently being collected for multicomponent systems of interest, including iodine and water on MS3A. A diffusion kinetic model for sorbent pellets involving pore and surface diffusion as well as external mass transfer has been established, and a methodology was developed for determining unknown diffusivity parameters from transient uptake data. Two parallel approaches have been explored for integrating the kernels described above into a mass-transport model for adsorption in fixed beds. In one, the GSTA isotherm kernel has been incorporated into the MOOSE framework; in the other approach, a focused finite-difference framework and PDE kernels have been developed. Issues, including oscillatory behavior in MOOSE solutions to advection-diffusion problems, and opportunities have been identified for each approach, and a path forward has been identified toward developing a stronger modeling platform. Experimental systems were established for collection of microscopic kinetics and equilibria data for single and multicomponent uptake of gaseous species on solid sorbents. The systems, which can operate at ambient temperature to 250°C and dew points from -69 to 17°C, are useful for collecting data needed for modeling performance of sorbents of interest. Experiments were conducted to determine applicable models and parameters for isotherms and mass transfer for water and/or iodine adsorption on MS3A. Validation experiments were also conducted for water adsorption on fixed beds of MS3A. For absorption, work involved modeling with supportive experimentation. A dynamic model was developed to simulate CO 2 absorption with chemical reaction using high alkaline content water solutions. A computer code was developed to implement the model based upon transient mass and energy balances. Experiments were conducted in a laboratory-scale column to determine model parameters. The influence of geometric parameters and operating variables on CO 2 absorption was studied over a wide range of conditions. This project has resulted in 7 publications, with 3 manuscripts in preparation. Also, 15 presentations were given at national meetings of ANS and AIChE and at Material Recovery and Waste Forms Campaign Working Group meetings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Technetium Inventory, Distribution, and Speciation in Hanford Tanks (Rev.1)

The purpose of this report is three fold: 1) assemble the available information regarding Tc inventory, distribution between phases, and speciation in Hanford’s 177 storage tanks into a single, detailed, comprehensive assessment; 2) discuss the fate (distribution/speciation) of Tc once retrieved from the storage tanks and processed into final waste forms; and 3) discuss/document in less detail the available data on the inventory of Tc in other “pools” such as the vadose zone below inactive cribs and trenches, below single-shell tanks (SSTs) that have leaked, and in the groundwater below the Hanford Site. This report was revised in September 2014 to add detail and correct inaccuracies in Section 5.0 on the fate of technetium (Tc) recycle from the off-gas systems downstream of the low-activity waste (LAW) melters back to the melters, based on several reports that were not found in the original literature search on the topic. The newly provided reports, from experts active in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) glass studies, the Vitreous State Laboratory at The Catholic University of America (VSL) melter and off-gas system demonstrations and overall WTP systems analysis, were not originally found on electronic databases commonly searched. The major revisions to Section 5.0 also required changes to Section 7.0 (Summary and Conclusions) and this executive summary.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Office of River Protection Advanced Low-Activity Waste Glass Research and Development Plan

The U.S. Department of Energy Office of River Protection (ORP) has initiated and leads an integrated Advanced Waste Glass (AWG) program to increase the loading of Hanford tank wastes in glass while meeting melter lifetime expectancies and process, regulatory, and product performance requirements. The integrated ORP program is focused on providing a technical, science-based foundation for making key decisions regarding the successful operation of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) facilities in the context of an optimized River Protection Project (RPP) flowsheet. The fundamental data stemming from this program will support development of advanced glass formulations, key product performance and process control models, and tactical processing strategies to ensure safe and successful operations for both the low-activity waste (LAW) and high-level waste vitrification facilities. These activities will be conducted with the objective of improving the overall RPP mission by enhancing flexibility and reducing cost and schedule. The purpose of this advanced LAW glass research and development plan is to identify the near-term, mid-term, and longer-term research and development activities required to develop and validate advanced LAW glasses, property-composition models and their uncertainties, and an advanced glass algorithm to support WTP facility operations, including both Direct Feed LAW and full pretreatment flowsheets. Data are needed to develop, validate, and implement 1) new glass property-composition models and 2) a new glass formulation algorithm. Hence, this plan integrates specific studies associated with increasing the Na2O and SO3/halide concentrations in glass, because these components will ultimately dictate waste loadings for LAW vitrification. Of equal importance is the development of an efficient and economic strategy for 99Tc management. Specific and detailed studies are being implemented to understand the fate of Tc throughout the WTP flowsheet and the underlying mechanisms that dictate its partitioning between streams within the LAW vitrification facility. These studies are aimed at increasing the single-pass Tc retention in glass and the potential use of high-temperature mineral phases to capture Tc. The Tc-bearing mineral phases would be thermally stable and resistant to Tc release during feed melting reactions or they could serve as alternative waste forms. The LAW glass research and development is focused on reducing the total volume of LAW glass produced and minimizing the impact of (or potentially eliminating) the need for recycle.

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

Conceptual Model Testing Related to SDU 6 Drainwell Observations

From its inception in the early 1950s through the end of the Cold War in the early 1990s, the Savannah River Site (SRS) produced nuclear materials for national defense in five reactors. Additionally, irradiated reactor fuel and target tubes were dissolved in nitric acid to recover plutonium and uranium using the PUREX (Plutonium Uranium Reduction EXtraction) process. Liquid waste from these chemical separations processes was then stored onsite in 51 underground tanks. Eight waste storage tanks have been operationally closed (i.e. cleaned and grouted) and the remaining tanks hold a mixture of liquids, insoluble solids, and precipitated salts (SRMC-LWP-2022-00001), the latter generated by evaporating water from the liquid waste. Waste is currently being retrieved from tanks and separated into 1) high-radioactivity, low-volume, and 2) low-radioactivity, high-volume components, principally through the Salt Waste Processing Facility (SWPF) (SRMC-LWP-2023-00001). The former waste stream is vitrified in the Defense Waste Processing Facility (DWPF), stored onsite, and destined for offsite disposal in a deep geologic repository. The latter stream is mixed with dry cementitious materials in the Saltstone Production Facility (SPF) and the wet slurry placed in onsite Saltstone Disposal Units (SDUs) within the Saltstone Disposal Facility (SDF), where it hardens into a cement waste form termed saltstone. A low-infiltration surface cover system will be placed over the SDF at closure, where SDUs will then be in the subsurface post-closure (SRR-CWDA-2019-00001).

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

Halogenation of used aluminum matrix test reactor fuel – a bench-scale demonstration with surrogate materials

In this work, experiments with surrogate materials were performed at bench scale to demonstrate a halogenation technique applicable to treatment of used aluminum matrix test reactor fuel. The technique involves dissolution and separation of aluminum from used aluminum matrix test reactor fuel in molten-halide salt systems prior to treatment and disposition of the fuel’s uranium and fission products. Demonstration of the halogenation technique was performed with neodymium metal as a non-radiological surrogate for uranium metal. Experiments involved blending forms of aluminum and neodymium metal with ammonium and lithium chloride or ammonium and lithium bromide, which upon heating decomposed into ammonia gas and the respective hydrogen chloride or bromide gas. The latter reacted with the metals to form the respective aluminum and neodymium halides. At elevated temperatures, aluminum halides gasified away from the respective neodymium halides, which fused with their respective lithium halides. Samples of fused and distillate salts were collected and analyzed, yielding extents of aluminum removal that ranged from 94.5–98.2% for chlorination runs and 91.4–97.8% for bromination runs. No neodymium was detected in the distillate fractions. Some experiments were repeated with excess reactants, and a portion of aluminum chloride distillate was processed into a consolidated waste form.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

HLW Melter Control Strategy Without Visual Feedback

Plans for the treatment of high level waste (HL W) at the Hanford Tank Waste Treatment and Immobilization Plant (WTP) are based upon the inventory of the tank wastes, the anticipated performance of the pretreatment processes, and current understanding of the capability of the borosilicate glass waste form. The WTP HLW melter design, unlike earlier DOE melter designs, incorporates an active glass bubbler system. The bubblers create active glass pool convection and thereby improve heat and mass transfer and increase glass melting rates. The WTP HLW melter has a glass surface area of 3.75 m 2 and depth of ~ 1.1 m. The two melters in the HLW facility together are designed to produce up to 7.5 MT of glass per day at 100% availability. Further increases in HL W waste processing rates can potentially be achieved by increasing the melter operating temperature above 1150°C and by increasing the waste loading in the glass product. Increasing the waste loading also has the added benefit of decreasing the number of canisters for storage.

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

Vitrification Testing of HLW with High Phosphate

Projections of the number of high level waste (HLW) canisters to be produced in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) (e.g., [1]) are based upon the inventory of the tank wastes, the anticipated performance of the sludge treatment processes, and current understanding of the capability of the borosilicate glass waste form. The WTP HLW melter design, unlike earlier Department of Energy (DOE) melter designs, incorporates a glass bubbler system. The bubblers create active glass pool mixing and thereby improve heat and mass transfer and glass melting rate. The WTP HLW melters each have a glass surface area of 3.75 m 2 and depth of ~1.1 m. The two melters in the HLW facility together are designed to produce up to 7.5 MT of glass per day at 100% availability. Further increases in HLW waste processing rates can potentially be achieved by optimization of the feed and glass formulations, increasing the melter operating temperature above 1150⁰C, and by increasing the waste loading in the glass product. Increasing the waste loading also has the added benefit of decreasing the number of canisters for storage.

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