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At least 811 records · Page 45
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Buffer Material Degradation in High Level Radioactive Waste Disposal - 18454

The concept of geological disposal for high-level radioactive waste (HLW) is based on a multi-barrier system comprising the natural geological barrier that repository host rock provides and its surroundings, as well as an engineered barrier system (EBS) that includes waste form, waste canisters, buffer materials, and backfill. The multi-barrier system is expected to perform its desired functions to isolate waste from the biosphere and achieve HLW disposal. Because of the interaction processes of radionuclide decay heat with hydraulic and water-mineral reactions in the radioactive waste repository, the bentonite buffer degradation resulting from the external temperature and pressure warrants investigation. However, seldom addressed in Taiwan is the influence of thermo-hydro-chemical (T-H-C) processes on buffer material degradation in the EBS of HLW disposal repositories as related to smectite clay dehydration. Therefore, we adopted the chemical kinetic model of smectite dehydration to calculate the amount of water expelled from smectite clay minerals caused by higher temperatures of waste decay heat. We discovered that smectite clay could cause volume shrinkage because of a loss of interlayer water, which can lead to bentonite buffer compression. The results of this study may be used in advanced research on the evolution of bentonite degradation for both performance assessments and safety analyses of final HLW disposal in Taiwan. (authors)

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

Large-scale production of 88 Y and 88 Zr/ 88 Y generators: A proof of concept study for a 70 MeV H – cyclotron

Here, the large-scale production of 88 Y with proton-induced reactions has been investigated from the perspective of new generation 70 MeV H – cyclotrons. Tandem target configurations are presented for both the direct production of 88 Y as well as for producing 88 Zr/ 88 Y generators. Based on the relevant excitation functions, physical yields have been derived for 88 Y production with Y 2 O 3 /SrCO 3 tandem targets and 88 Zr production with Zr/Y 2 O 3 tandem targets. Yields are presented for optimized targets (i.e. optimum yield) as well as for balanced thermal loads on the individual targets. Liquid 88 Zr/ 88 Y generators have been produced using both natural Zr and Nb target materials, the former for dedicated productions and the latter as a byproduct by processing spent irradiated Nb capsules which normally would constitute radioactive waste. These stock solutions, which contain both the target material and 88 Zr precursor, are retained virtually unchanged after processing except for the removal of 88 Y on AG MP-50 macroporous cation-exchange resin. Methods are presented for the preparation of Nb stock solutions in hydrofluoric acid and Zr stock solutions in sulfuric acid. It is shown that multi-Ci productions of 88 Y are feasible at a 70 MeV cyclotron facility, suitable for the needs of fracking applications. In addition, 88 Zr/ 88 Y generators can provide 88 Y with very high specific activity, suitable for labelling of biomolecules.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2015

Status of the nuclear measurement stations for the process control of spent fuel reprocessing at AREVA NC/La Hague

Nuclear measurements are used at AREVA NC/La Hague for the monitoring of spent fuel reprocessing. The process control is based on gamma-ray spectroscopy, passive neutron counting and active neutron interrogation, and gamma transmission measurements. The main objectives are criticality and safety, online process monitoring, and the determination of the residual fissile mass and activities in the metallic waste remained after fuel shearing and dissolution (empty hulls, grids, end pieces), which are put in radioactive waste drums before compaction. The whole monitoring system is composed of eight measurement stations which will be described in this paper. The main measurement stations no. 1, 3 and 7 are needed for criticality control. Before fuel element shearing for dissolution, station no. 1 allows determining the burn-up of the irradiated fuel by gamma-ray spectroscopy with HP Ge (high purity germanium) detectors. The burn-up is correlated to the {sup 137}Cs and {sup 134}Cs gamma emission rates. The fuel maximal mass which can be loaded in one bucket of the dissolver is estimated from the lowest burn-up fraction of the fuel element. Station no. 3 is dedicated to the control of the correct fuel dissolution, which is performed with a {sup 137}Cs gamma ray measurement with a HP Ge detector. Station no. 7 allows estimating the residual fissile mass in the drums filled with the metallic residues, especially in the hulls, from passive neutron counting (spontaneous fission and alpha-n reactions) and active interrogation (fission prompt neutrons induced by a pulsed neutron generator) with proportional {sup 3}He detectors. The measurement stations have been validated for the reprocessing of Uranium Oxide (UOX) fuels with a burn-up rate up to 60 GWd/t. This paper presents a brief overview of the current status of the nuclear measurement stations. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2011

Radioactive Demonstration of Final Mineralized Waste Forms for Hanford Waste Treatment Plant Secondary Waste (WTP-SW) by Fluidized Bed Steam Reforming (FBSR) using the Bench Scale Reformer Platform

The U.S. Department of Energy's Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. In addition, the WTP LAW vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as 137 Cs, 129 I, 99 Tc, Cl, F, and SO 4 that volatilize at the vitrification temperature of 1150°C in the absence of a continuous cold cap (that could minimize volatilization). The current waste disposal path for the WTP-SW is to process it through the Effluent Treatment Facility (ETF). Fluidized Bed Steam Reforming (FBSR) is being considered for immobilization of the ETF concentrate that would be generated by processing the WTP-SW. The focus of this current report is the WTP-SW. FBSR offers a moderate temperature (700-750°C) continuous method by which WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline ceramic (mineral) waste form. The mineral waste form that is produced by co-processing waste with kaolin clay in an FBSR process has been shown to be as durable as LAW glass. Monolithing of the granular FBSR product is being investigated to prevent dispersion during transport or burial/storage, but is not necessary for performance. A Benchscale Steam Reformer (BSR) was designed and constructed at the SRNL to treat actual radioactive wastes to confirm the findings of the non-radioactive FBSR pilot scale tests and to qualify the waste form for applications at Hanford. BSR testing with WTP SW waste surrogates and associated analytical analyses and tests of granular products (GP) and monoliths began in the Fall of 2009, and then was continued from the Fall of 2010 through the Spring of 2011. Radioactive testing commenced in 2010 with a demonstration of Hanford's WTP-SW where Savannah River Site (SRS) High Level Waste (HLW) secondary waste from the Defense Waste Processing Facility (DWPF) was shimmed with a mixture of 125/129 I and 99 Tc to chemically resemble WTP-SW. Prior to these radioactive feed tests, non-radioactive simulants were also processed. Ninety six grams of radioactive granular product were made for testing and comparison to the non-radioactive pilot scale tests. The same mineral phases were found in the radioactive and non-radioactive testing.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

WASTE TREATMENT PLANT (WTP) LIQUID EFFLUENT TREATABILITY EVALUATION (SEPTEMBER 2004)

A forecast of the radioactive, dangerous liquid effluents expected to be produced by the Waste Treatment Plant (WTP) was provided by Bechtel National, Inc. (BNI 2004). The forecast represents the liquid effluents generated from the processing of Tank Farm waste through the end-of-mission for the WTP. The WTP forecast is provided in the Appendices. The WTP liquid effluents will be stored, treated, and disposed of in the Liquid Effluent Retention Facility (LERF) and the Effluent Treatment Facility (ETF). Both facilities are located in the 200 East Area and are operated by Fluor Hanford, Inc. (FH) for the US. Department of Energy (DOE). The treatability of the WTP liquid effluents in the LERF/ETF was evaluated. The evaluation was conducted by comparing the forecast to the LERF/ETF treatability envelope (Aromi 1997), which provides information on the items which determine if a liquid effluent is acceptable for receipt and treatment at the LERF/ETF. The format of the evaluation corresponds directly to the outline of the treatability envelope document. Except where noted, the maximum annual average concentrations over the range of the 27 year forecast was evaluated against the treatability envelope. This is an acceptable approach because the volume capacity in the LERF Basin will equalize the minimum and maximum peaks. Background information on the LERF/ETF design basis is provided in the treatability envelope document.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Radionuclide inventory of vitrified waste after spent nuclear fuel reprocessing at La Hague

The primary aim of the present work was to determine the inventories of the radionuclides and stable elements in vitrified high-level waste produced at La Hague and delivered to Germany, which are of importance for long-term safety assessment of final repositories for radioactive wastes. For a subset of these radionuclides and stable elements, the inventories were determined - either by direct measurements or by involving established correlations - and reported by AREVA. This allowed verification of the validity of application of a model approach utilizing the data of burnup and activation calculations and auxiliary information on the reprocessing and vitrification process operated at La Hague. Having proved that such a model approach can be applied for prediction of inventories of actinides, fission and activation products in vitrified waste, the present work estimated the minimum, average and maximum inventories of the radionuclides, which are of importance for long-term safety assessment of final repositories for radioactive waste but were not reported by AREVA for delivered CSD-V canisters. The average and maximum inventories in individual CSD-V canisters predicted in the present approach were compared to the inventories predicted by Nagra for canisters with vitrified waste delivered from La Hague to Switzerland [1]. This comparison revealed a number of differences between these inventories despite the fact that the canisters delivered to Switzerland were produced in essentially the same way and from the common reprocessing waste stock as CSD-V canisters delivered to Germany. Therefore, a further work is required in order to identify the reason for the discrepancy in the present estimation versus the Nagra estimation [1]. Such a work should also address the recommendation by the international peer review of the Safety Report of the Project Opalinus Clay to obtain estimates of the inventories of long-lived mobile radionuclides (such as {sup 14}C, {sup 36}Cl, {sup 79}Se, and {sup 129}I), which contribute most to the dose estimates in the radiological safety assessments, if possible, in agreement with other countries with similar waste streams in order for a coordinated set of data to be generated [2]. Since vitrified waste from reprocessing of spent nuclear fuel at La Hague was delivered to several countries - Belgium, France, Germany, Japan, Netherlands, and Switzerland - an international effort can be recommended. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Corrosion Control during Closure Activities at the Savannah River Site - 13514

Liquid radioactive wastes from the Savannah River Site (SRS) separation process are stored in large underground carbon steel tanks. Until the waste is removed from storage, transferred, and processed, the materials and structures of the tanks must maintain a confinement function by providing a barrier to the environment and by maintaining acceptable structural stability during normal service and design basis events (e.g., earthquake conditions). A corrosion control program is in place to ensure that degradation of the steel does not impact the structural and leak integrity functions of these waste tanks. The SRS is currently retrieving waste from older waste tanks and processing the waste through the vitrification for long term stabilization. The retrieval processes prepare the tanks for ultimate closure (i.e., grouting) by removing sludge by mechanical and/or sluicing methods, dissolving salt cake by adding water, and chemical cleaning of the residual sludge with oxalic acid. Each of these retrieval methods will result in waste chemistry that does not meet the requirements of the current corrosion control program. Given the short-term exposure and limited remaining service life for the tanks in which retrievals are being performed, an assessment of the need for corrosion controls in these tanks was performed. The assessment reviewed the corrosion rates in the more aggressive environments and the postulated loads on the structure during the closure activities. The assessment concluded that the current corrosion control program may be suspended for a short period of time while final retrieval of the waste is performed. (authors)

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

The controlling role of atmosphere in dawsonite versus gibbsite precipitation from tetrahedral aluminate species

In highly alkaline solution, aluminum speciates as the tetrahedrally coordinated aluminate monomer, Al(OH)4- and/or dimer Al2O(OH)62-, yet precipitates as octahedrally coordinated gibbsite (Al(OH)3). This tetrahedral to octahedral transformation governs Al precipitation, which is crucial to worldwide Al production, and to the processing of caustic high-level radioactive wastes. Despite its significance, the transformation pathway remains unknown. Here we explore the roles of atmospheric water and carbon dioxide in mediating the transformation of the tetrahedrally coordinated potassium aluminate dimer salt (K2Al2O(OH)6) to gibbsite versus potassium dawsonite (KAl(CO3)(OH)2). A combination of in-situ attenuated total reflection infrared spectroscopy, ex-situ micro X-ray diffraction, and multivariate curve resolution-alternating least squares chemometrics analysis reveals that humidity plays a key role in the transformation by limiting the amount of alkalinity neutralization by dissolved CO2. Lower humidity favors higher alkalinity and incorporation of carbonate species in the final Al product to form KAl(CO3)(OH)2. Higher humidity enables more acid generation that destabilizes dawsonite and favors gibbsite as the solubility limiting phase. Because the transformation was restricted to occur in thin water films, the results suggest that transition from tetra- to octahedrally coordinated Al does not have to occur in bulk solution, as has often been hypothesized, but may instead appear on the source mineral surface.

Dembowski, Mateusz↗
DOE OSTI2018

Development of Hot-Isostatic Pressing for Treatment of UK ILW Radioactive Wastes - 18280

Hot-Isostatic Pressing (HIPing) has been proposed as an improved method for the treatment of radioactive wastes in the UK. Sludges and slurries housed on the Sellafield site are a prime candidate for HIP treatment due to their large volumes and issues associated with the use of the baseline cementation strategy. Options have been developed by GeoRoc Ltd to co-process these wastes, including a detailed conceptual plant design. This paper will describe research and development aimed at demonstrating the viability of the concept presented in this design. This paper summarizes two studies performed to address the knowledge gaps identified for treatment of these wastes using HIP technology. The first study related to the poorly characterized nature of the wastes, which requires any treatment option to be flexible in terms of the chemical and physical properties of the waste feed. The second study involved demonstrating that HIPing can be effectively utilized at a scale applicable to treat a waste inventory estimated to be in excess of 5,000 m{sup 3}. The first section of this paper presents a summary of research carried out to determine where variation in the waste stream composition may affect the processing and wasteform produced when HIPing Magnox sludges. This study aimed to qualify where restrictions on the process envelope may exist due to poorly defined waste-stream characteristics. A baseline wasteform was selected with the aim of achieving significant waste volume reduction, while producing a physically and chemically stable wasteform. A glass-bonded magnesium-titanate/magnesium-silicate wasteform was selected as the preferred option for the Magnox sludge wastes. A series of studies investigated the densification and phase formation of waste-forms by altering key variables in the Magnox sludge simulant. To test the extremes of the processable waste loading, samples were produced and characterized at 100 wt% waste-loading for Magnox sludge, Site-Ion Exchange Plant (SIXEP) sand/clinoptilolite and a 50:50 mix of the two waste-streams. Further studies involved a) altering the waste loading to additive mass ratio (to simulate changes in the waste loading/sludge solids content), b) varying the particle size distribution from the datum to include only small or large particulates in the sludge feed; and c) introducing up to 20 wt% metallic Magnox alloy, organic species or carbonate materials (to determine how their inclusion may affect the processing and densification of the materials). A U{sub 3}O{sub 8} loaded sample was also produced using the baseline Magnox sludge formulation. All the tests performed were shown to produce monolithic, well densified waste-forms with substantial volume reductions. Minimal variations from the baseline were noted but the waste-forms produced with these deviations was determined to be of comparable quality to of the baseline product. U{sub 3}O{sub 8} was shown to behave in a similar fashion to the ZrO{sub 2} surrogate used to simulate it in the process envelope studies and was encapsulated in the magnesium titanate/magnesium silicate matrix. This work demonstrates that HIP technology can successfully produce waste-forms across the broad process envelope expected in the Magnox sludge inventory. It is also possible to produce monolithic waste-forms at 100 wt% waste loading from Magnox sludges, SIXEP sand clinoptilolite slurries or a co-processed mixture of the two. The second part of this paper summarizes a commercially relevant demonstration of HIP technology for the treatment of sludge and slurry wastes housed at the Sellafield site (UK). This study culminated in production of the largest HIPed wasteform successfully produced to date. This study was performed in a series of stages. Investigations into formulation and properties of waste-forms were performed at a lab scale to evaluate suitable wasteform systems and identify suitable combinations of additives and waste loadings. Scale up demonstrations were then performed in stages with custom-designed HIP canisters. Scale-up and characterization of key wasteform properties were successfully performed with initial canister volumes of 50 ml, 400 ml and 8 L. Suitable front-end unit operations to produce a granular, free-flowing calcined simulant were demonstrated at an engineering scale. The demonstration was successful in processing a HIP canister with an initial starting volume in excess of 100 L. A 75 % volume reduction from the raw sludge was achieved at scale while demonstrating that HIP is applicable at suitably large scale for immobilization of ILW waste. (authors)

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

Density of Next-Generation Caustic-Side Solvent Extraction Solvent

This report recommends the appropriate modifier concentration to employ in the Next Generation Solvent (NGS) to be used in the Salt Waste Processing Facility (SWPF) at the Savannah River Site for removal of cesium from legacy tank waste. The Next Generation Caustic-Side Solvent Extraction (NG-CSSX) process employing the NGS is a marked improvement over the original Caustic-Side Solvent Extraction (CSSX) process, as it provides more effective removal of cesium from highly alkaline radioactive wastes and concentrates this removed cesium into an aqueous solution that is easy to vitrify for final disposal. Considerable effort has been devoted to optimizing the chemistry and process conditions of both systems, and their effectiveness has been demonstrated at the pilot scale at the Modular CSSX Unit (MCU). Due to the success of the demonstration and pilot-scale tests, the Salt Waste Processing Facility (SWPF) has been built to process larger volumes of waste with the CSSX process. To accelerate the waste-processing rate of the SWPF beyond its design throughput, plans call for the replacement of the CSSX process by the NG-CSSX process. To implement the NG-CSSX process in equipment optimized for CSSX, adjusting the density of the NGS to match the CSSX solvent density of 0.851 ± 0.0008 g/mL is considered advisable to obtain comparable hydraulic performance. Toward this objective, the density of the NGS has been measured at different temperatures and modifier concentrations to determine that a concentration of 0.650 M Cs-7SB modifier provides the best match for the desired density.

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

A Review of Tank 48H Treatment of Tetraphenylborate with Permanganate

Tank 48H contains roughly 270,000 gallons of radioactive waste material. The waste stored in this tank was to be processed in multiple stages utilizing facilities at the Savannah River Site (SRS) almost 30 years ago. The In-Tank Precipitation Process (ITP) was initiated in Tank 48H, which precipitated highly radioactive cesium-137 using sodium tetraphenylborate (NaTPB). While the process succeeded in precipitating the Cs, Sr, and other actinides, it also generated an unexpectedly large amount of benzene. The evolved benzene created a safety concern and made the waste incompatible with further downstream processing. This halted the ITP, and a new method of treatment was required to continue processing the legacy waste contained in Tank 48H. A myriad of treatment options have been proposed with multiple teams of researchers assembled to work on this highly complex issue over the last few decades. This review investigated one potentially viable treatment option, in-tank oxidation with sodium permanganate. Permanganate has been well known in literature as a strong oxidizing agent for organic compounds, as well as being utilized at the Savannah River Site (SRS) in other processes. A small number of studies have been conducted utilizing waste simulants to evaluate the use of permanganate as an oxidant for tetraphenylborate (TPB). A search of the literature and data from these studies indicates that permanganate could be a viable treatment for destruction of TPB in Tank 48H. While the scoping studies had a small number of individual experiments and nonideal conditions, the permanganate decomposed up to 90% of the TPB. A free hydroxide concentration above 1.0 M is required for tank corrosion control. Simulant studies indicate no decrease in TPB decomposition by permanganate until pH 14. The simulant studies show an increase in TPB decomposition as the temperature of the solution is increased to 40 °C. The post-reaction analysis of previous simulant tests did not look at all of the organic degradation products. Investigations into what these organic products are and in what quantity will help guide determinations as to whether the downstream processing facilities are able to handle the material that will be generated. Study on the time frame for the reaction between permanganate and TPB should be investigated as the literature reports only extend out to two weeks reaction time. The permanganate treatment conditions indicate no corrosion control concerns and a longer timescale reaction may be needed for in-tank treatment. In addition, further study would be useful to identify a lower boundary condition for the ratio of TPB and oxidant. The simulant tests applied large excesses of permanganate, and this may be unnecessary. The size constraint of the tank means that there will be practical limitations on the amount of sodium permanganate that can be added to the tank. The amount of permanganate should be minimized as much as possible while still ensuring decomposition of the TPB to minimize the amount of manganese dioxide solids generated.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Developments in the Regulatory Framework of Nuclear Waste Management in Germany - Licensing Procedures for storage of SNF and Public Involvement - 19612

According to article 6 of the German Atomic Energy Act (AtG), storage of Spent Nuclear Fuel requires a license. The competent licensing authority in this field is the Federal Office for Safety of Nuclear Waste Management (BfE). According to the Act for selecting a repository site for heat-generating radioactive waste (HAW) (Site Selection Act - StandAG) dating from 2017, BfE has been assigned the task of developing, conducting, and evaluating public participation procedures in the process of site search and selection for a deep geological repository for radioactive waste and SNF. Article 6 AtG applies to interim storage of SNF. If the legally defined licensing conditions by article 6 (2) AtG are met, the storage license applied for has to be granted. For on-site facilities, interim storage has been limited to 40 years. The licensing procedures for interim storage of SNF are carried out in accordance with the general administrative procedural rules. In certain cases due to the Environmental Impact Assessment Act (EIA Act), an EIA has to be carried out. In these cases, a formalized licensing procedure including an involvement of the public is conducted. The Nuclear Licensing Procedure Ordinance (AtVfV) originating from 1977 and reformulated in 1995 defines formalized rules for the public participation procedure which have to be followed strictly. These include a public hearing. The risen objections are evaluated by the licensing authority and taken account of in the licensing decision. The process of repository site selection defined by the StandAG exceeds these formalized procedures significantly: The objective of this process is to achieve a broad social consensus about the site selection procedure and about a repository site that will offer the best possible safety for one million years. Therefore, the process has to be particularly transparent, and involvement of the public - including newly developed forms of public involvement - is an essential part of it. BfE as competent authority in both the fields of repository site search and selection and licensing of interim storage of SNF has recently developed new strategies of involving the public concerning interim storage of SNF. Supplementing the standard licensing procedures, BfE presently informs and involves the public about topical issues regarding the present state and recent developments in the field of interim storage of SNF. Current central topics are for example the return of HAW and MAW from reprocessing of SNF in France and UK as well as perspective longer interim storage periods on the interface with final disposal. Regarding longer interim storage, host communities of interim storage facilities are concerned that interim storage might be extended indefinitely. Additionally, there is a strong fear of transports of radioactive waste and SNF from one place to another. (authors)

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

Advanced Low-Temperature Chlorination of Zirconium

Recovery of Zr from nuclear fuel is of high interest because the Zr cladding material comprises up to 50% of the high-level radioactive waste (HLW) that requires disposition. An ideal Zr-recovery process would not only recover the bulk Zr from the fuel or cladding but would also provide decontamination from the components that give rise to the HLW designation. A simplified decontamination pathway providing recovered Zr in compliance with low-level radioactive waste acceptance criteria could significantly reduce the burden of HLW requiring geologic disposition. A newly developed advanced low-temperature chlorination process presents an opportunity to recover a ZrCl4 product that is effectively decontaminated from the elements of concern. This advanced low-temperature chlorination process uses a mixture of the sulfur-containing chlorination compounds sulfur monochloride (S 2 Cl 2 ) and thionyl chloride (SOCl 2 ).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Thermal evaluations for mixed organic and nitrate salt drums in interim storage at the WCS Federal Waste Facility

Waste Control Specialists LLC (WCS) operates the Federal Waste Facility (FWF) in Texas that is licensed to process and store certain types of mixed low-level radioactive waste packages. The specific waste currently housed at WCS includes some of the transuranic (TRU) waste that originated at the DOE Los Alamos National Laboratory (LANL) and are destined for disposal at the DOE Waste Isolation Pilot Plant (WIPP) facility. The TRU waste within each Standard Waste Box (SWB) was packaged in 55-gallon drums at LANL. Some of the drums contain mixed organic and nitrate salt contents suspected of experiencing a chemical reaction. The drums (up to four drums in a SWB) were then overpacked in a SWB prior to shipment to WCS. In the most common configuration, WCS placed the SWB containing the drums on metal pallets and stored two SWBs into Modular Concrete Canisters (MCCs) in a double stacked array. The MCCs were placed in a staggered array at a segregated area of the FWF and covered with sand to mitigate the heating that occurred when stored above ground on waste pads. The temporary interment is also intended to provide additional containment of the suspect reactive waste to mitigate release of radioactivity in an incident such as that which occurred at WIPP for one such drum. Void space of each MCC was filled with 1-inch pea gravel to facilitate retrievability. Thermocouple probes were placed within each MCC to monitor heat generation from the SWBs and the MCC lids were closed. The primary objective of this analysis was to estimate the heat generation of the SWB drum contents when the SWB package temperature inside the MCC and the FWF ambient temperature were monitored.

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

DECOVALEX-2023: An international collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems

The DECOVALEX initiative is an international research collaboration (www.decovalex.org), initiated in 1992, for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems. DECOVALEX stands for “DEvelopment of COupled Models and VALidation against EXperiments”. The creation of this international initiative was motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel. DECOVALEX emphasizes joint analysis and comparative modeling of the complex perturbations and coupled processes in geologic repositories and how these impact long-term performance predictions. The most recent phase of the DECOVALEX Project, here referred to as DECOVALEX-2023, started in early 2020 and ended in late 2023. More than fifty research teams associated with 17 international DECOVALEX partner organizations participated in the comparative evaluation of eight modeling tasks covering a wide range of spatial and temporal scales, geological formations, and coupled processes. This Virtual Special Issue on DECOVALEX-2023 provides an in-depth overview of these collaborative research efforts and how these have advanced the state-of-the-art of understanding and modeling coupled THMC processes. While primarily focused on radioactive waste, much of the work included here has wider application to many geoengineering topics.

Coupled processes↗
DOE OSTI2021

Numerical study of the chemo-mechanical behavior of FEBEX bentonite in nuclear waste disposal based on the Barcelona expansive model

Experimental studies show that compacted bentonite used as a backfill material for nuclear waste repository experiences strong coupling between chemical and mechanical processes. Here, we use a dual-structure expansive soil model, referred to as the Barcelona Expansive Model (BExM), to predict the behavior of bentonite buffer in subsurface emplacement tunnels for high-level radioactive waste. After emplacement, the bentonite is subjected to complex and coupled Thermal-Hydraulic-Mechanical-Chemical (THMC) processes. The BExM constitutive model is implemented in a multi-phase reactive transport and geomechanics simulator, TOUGHREACT-FLAC3D, and the model is verified with one benchmark test on FEBEX bentonite. We utilize a one-way Chemo-Mechanical (C-M) coupling approach, in which chemical changes affect the mechanical behavior of bentonite through the BExM linked with the evolution of mass fraction of smectite, exchangeable cation concentration, and ionic strength via osmotic suction. The parameters of the new coupled model for FEBEX bentonite are calibrated against a series of laboratory experiments with various salinity solutions. Finally, coupled THMC modeling is conducted for a generic argillite repository with bentonite buffer under high temperature, focusing on the long-term chemical change and its effect on the mechanical process.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Preliminary analysis of species partitioning in the DWPF melter. Sludge batch 7A

The work described in this report is preliminary in nature since its goal was to demonstrate the feasibility of estimating the off-gas carryover from the Defense Waste Processing Facility (DWPF) melter based on a simple mass balance using measured feed and glass pour stream (PS) compositions and time-averaged melter operating data over the duration of one canister-filling cycle. The DWPF has been in radioactive operation for over 20 years processing a wide range of high-level waste (HLW) feed compositions under varying conditions such as bubbled vs. non-bubbled and feeding vs. idling. So it is desirable to find out how the varying feed compositions and operating parameters would have impacted the off-gas entrainment. However, the DWPF melter is not equipped with off-gas sampling or monitoring capabilities, so it is not feasible to measure off-gas entrainment rates directly. The proposed method provides an indirect way of doing so.

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

Big Data and AI at DoE's Legacy Sites - 20546

More than 30 years have passed since DOE started the decommissioning of nuclear weapon complexes and the clean-up of soil and groundwater. All the sites have been collecting and archiving soil and groundwater monitoring datasets; particularly contaminant concentration time-series. These datasets provide unparalleled opportunities to understand the system behavior (including more fundamental hydrological and geochemical processes, the response to various perturbations, the long-term trend and environmental decay rate towards the regulatory limit). This understanding is critical for providing multiple lines of evidences that can support site closure. In this study, we explore the machine learning (ML) and artificial intelligence (AI) applications to the long-term soil and groundwater management at DoE's legacy sites. ML can improve our understanding of the subsurface systems, which is critical for long-term monitoring and management of the sites, while AI can automate or support some of decision-making processes (e.g., anomaly detection, monitoring well placements). The particular focuses are to develop general algorithms to: (1) to identify distinct spatiotemporal patterns and to identify several groups that have similar temporal behaviors, using unsupervised clustering methods, (2) identify the different temporal scales of hydrological responses to climate perturbations by time-series analysis, and (3) reduce the number of monitoring wells by identifying the minimum sufficient number of wells to capture the heterogeneity of the groundwater contaminant plume and concentration distribution, using the Gaussian Process model. We demonstrate our methodology at the Savannah River Site F-Area. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗