Iron phosphate glass waste forms for vitrifying Hanford AZ102 low activity waste (LAW), part I: Glass formation model
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Materials Science↗
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Thermoanalytical investigation of the reactions causing the transuranic waste drum breach that occurred in the Waste Isolation Pilot Plant
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Scheele, Randall D.↗
Performance Testing to Advance Modular, Moving-Bed Gasification for the Generation of Low-Cost, Clean Hydrogen from Biomass Mixed with Legacy Coal Waste, Waste Plastic, and/or Other Waste
Project update on Performance Testing to Advance Modular, Moving-Bed Gasification for the Generation of Low-Cost, Clean Hydrogen from Biomass Mixed with Legacy Coal Waste, Waste Plastic, and/or Other Waste
Hack, Horst↗
Glass-bonded iodosodalite waste form for immobilization of 129I
Immobilization of radioiodine (e.g., 129I, 131I) is an important need for current and future nuclear fuel cycles. For the current work, iodosodalite [Na8(AlSiO4)6I2] was synthesized hydrothermally from metakaolin, NaI, and NaOH. Following hydrothermal treatment, dried unwashed powders were used to make glass-bonded iodosodalite waste forms by heating pressed pellets at 650, 750, or 850 °C with two different types of sodium borosilicate glass binders, i.e., NBS-4 and SA-800. These heat-treated specimens were characterized with X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, thermal analysis, porosity and density measurements, neutron activation analysis, and inductively-coupled plasma mass spectrometry. The pellets mixed with 10 mass% of NBS-4 or SA-800 and heat-treated at 750 °C contained relatively high percentage iodine retention (~44-47 % of the maximum iodine loading) with relatively low porosities, while other pellets with higher percentages iodine retention either contained higher porosity or were not completely sintered. ASTM C1308 chemical durability tests of monolithic specimens showed a large initial release of Na, Al, Si, and I on the first day, possibly from water-soluble salt crystals or non-durable amorphous phases. Release rates of Na and Si were higher than for Al and I, probably due to a poorly durable Na-Si-O phase from the glass bonding matrix. The cumulative normalized release of iodine was 12.5 g m-2 for the first 10 1-d exchanges, suggestive of coherent dissolution. The average release rate from 10-24 days during the 7-d exchange intervals was 0.2336 g m-2 d-1.
sodalite, iodosodalite, waste forms, iodine↗
Drying model of a high salt content cementitious waste form: Effect of capillary forces and salt solution
Highlights: • Drying model for a high salt content cementitious waste form is developed. • Water vapor diffusion and capillary liquid flow are distinguished. • Capillary and salt solution effects are considered in vapor-liquid equilibrium. A water transport model coupling capillary liquid flow with vapor diffusion is developed to describe the drying process for a cementitious waste form with high salinity porewater. Vapor-liquid equilibrium is formulated as the driving force for vapor diffusion and the model accounts for pore capillary and high salinity effects on water thermodynamic activity. Pore filling and porewater surface tension as a function of pore size distribution and water saturation have been quantified for the material. Geochemical speciation modeling is used to simulate porewater activity as a function of composition over the range of saturation. The theoretical relationship between relative humidity and water saturation generally agrees with experimental measurement, and the developed model is capable of predicting drying rates under various external relative humidity conditions. The model was developed to be incorporated into reactive transport models considering the effects of drying such as salt redistribution and efflorescence.
36 MATERIALS SCIENCE↗
Redox and volatility of Tc(CO)3 + compounds in waste glass melting
The behavior of non-pertechnetate (Tc(I)) species was studied by preparing three portions of dried low-activity waste-glass simulated feed, combining it with either the [fac-Tc(CO) (OH)] “tetramer,” the [fac-Tc(CO) (OH)(H O) ] “monohydroxo,” or the [fac-Tc(CO) Cl ] “trichloro,” and then heating samples to 600, 800, and 1000 °C. For the feeds and the heat-treated samples, Tc concentrations were measured by liquid scintillation counting (LSC) after NaOH and HNO fusion, and the results were used to determine the Tc volatility. For unheated samples and samples heated to 600 °C, the speciation of Tc was measured by X-ray absorption near-edge structure (XANES) analysis, while partitioning of Tc in the glass-forming melt was determined by leaching the samples in water and measuring the Tc concentration of the leachate. The current results are discussed in connection with previously reported data for Tc(VII) and Tc(IV) species to rationalize the potential mechanism on how different speciation of Tc affect its retention in glass. 3 4 3 2 2 3 3 3 2-
Luksic, SA↗
Quantitative Characterization of Aqueous Byproducts from Hydrothermal Liquefaction of Municipal Wastes, Food Industry Wastes, and Biomass Grown on Waste
Hydrothermal liquefaction (HTL) is a viable thermochemical process for converting wet solid wastes into biocrude which can be hydroprocessed to liquid transportation fuel blendstocks and specialty chemicals. The aqueous byproduct from HTL contains significant amounts (20 to 50%) of the feed carbon, which must be used to enhance economic sustainability of the process on an industrial scale. In this study, aqueous fractions produced from HTL of industrial and municipal waste were characterized using a wide variety of analytical approaches. Organic chemical compounds present in these aqueous fractions were identified using two-dimensional gas chromatography equipped with time-of-flight mass spectrometry. Identified compounds include organic acids, nitrogen compounds, alcohols, aldehydes, and ketones. Conventional gas chromatography and liquid chromatography methods were employed to quantify the identified compounds. Inorganic species, in the aqueous stream of hydrothermal liquefaction of these aqueous byproducts, also were quantified using ion chromatography and inductively coupled plasma optical emission spectroscopy. The concentrations of organic chemical compounds and inorganic species are reported, and the significance of these results is discussed in detail.
Maddi, Balakrishna (ORCID:0000000153536026)↗
Beta transmutations in apatites with ferric iron as an electron acceptor – implication for nuclear waste form development
Apatite-structured materials have been considered for immobilization of a number of fission products from reprocessing nuclear fuel because of their chemical durability as well as compositional and structural flexibility
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Life cycle analysis of polylactic acids from different wet waste feedstocks
Producing a valuable chemical product through diversion of wet wastes can simultaneously resolve the problems associated with increasing wastes and greenhouse gas emissions from conventional chemical production processes. In this work, we investigated the life-cycle greenhouse gas emissions, water, and fossil-fuel consumption for waste-derived polylactic acids (PLA) from three different waste feedstocks, namely wastewater sludge, food waste, and swine manure, using the Greenhouse Gases, Regulated Emissions, and Energy Use in Technologies (GREET) model. The decarbonization potential of replacing fossil-based resins with the waste-derived polymer was also investigated. The results show that swine manure-to-PLA pathway was the least carbon intensive (—1.4 kgCO 2 e/kg) among the three waste-to-PLA pathways on a cradle-to-grave basis, followed by the food waste case (—1.3 kgCO 2 e/kg) and then by the wastewater sludge case (0.6 kgCO 2 e/kg). In the baseline scenario, all three waste-to-PLA pathways were less carbon intensive than both fossil-based PET and HDPE on a cradle-to-grave basis: 66% (vs. PET) and 56% (vs. HDPE), 171 and 192%, 181 and 205% reduction in GHG emissions for wastewater sludge-, food waste-, and swine manure-to-PLA pathway, respectively. For all sensitivity cases investigated, the food waste- and swine manure-to-PLA pathways were significantly less carbon intensive than their fossil-counterparts. In terms of the annual decarbonization potential of replacing fossil-based PET or HDPE, the wastewater sludge- and food waste-pathway showed higher mitigation potential than the swine manure-pathway: i) 18–28 kilotons CO 2 e-reduction per year for wastewater sludge pathway; ii) 23–26 kTCO 2 e-reduction/yr for food waste pathway; and iii) about 5 kTCO 2 e-reduction/yr for swine manure pathway depending on the type of conventional resin replaced. However, given the abundant availability of the swine manure feedstocks across the United States, the decarbonization potential of swine manure-based pathway can also increase as the plant capacity or the number of plants grow.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Liquid secondary waste: Waste form formulation and qualification
The Hanford Site Effluent Treatment Facility (ETF) currently treats aqueous waste streams generated during site cleanup activities. When the Hanford Tank Waste Treatment and Immobilization Plant (WTP) begins operations, including Direct Feed Low Activity Waste (DFLAW) vitrification, a liquid secondary waste (LSW) stream from the WTP will need to be treated. The volume of effluent for treatment at the ETF will increase significantly. The powdered salt waste form produced by the ETF will be replaced by a stabilized solidified waste form for disposal in Hanford’s Integrated Disposal Facility (IDF). Washington River Protection Solutions is implementing a Secondary Liquid Waste Immobilization Technology Development Plan to address the technology needs for a waste form and solidification process to treat the increased volume of waste planned for disposal at the IDF. Waste form testing to support this plan is composed of work in the near term to provide data as input to a performance assessment (PA) for Hanford’s IDF. In 2015, three Hanford Liquid Secondary Waste simulants were developed based on existing and projected waste streams. Using these waste simulants, fourteen mixes of Hanford Liquid Secondary Waste were prepared and tested varying the waste simulant, the water-to-dry materials ratio, and the dry materials blend composition.1 In FY16, testing was performed using a simulant of the EMF process condensate blended with the caustic scrubber—from the Low Activity Waste (LAW) melter—, processed through the ETF. The initial EMF-16 simulant will be based on modeling efforts performed to determine the mass balance of the ETF for the DFLAW.2 The compressive strength of all of the mixes exceeded the target of 3.4 MPa (500 psi) to meet the requirements identified as potential IDF Waste Acceptance Criteria in Table 1 of the Secondary Liquid Waste Immobilization Technology Development Plan.3 The hydraulic properties of the waste forms tested (hydraulic conductivity and water characteristic curves) were comparable to the properties measured on the Savannah River Site (SRS) Saltstone waste form. Future testing should include efforts to first; 1) determine the rate and amount of ammonia released during each unit operation of the treatment process to determine if additional ammonia management is required, then; 2) reduce the ammonia content of the ETF concentrated brine prior to solidification, making the waste more amenable to grouting, or 3) manage the release of ammonia during production and ongoing release during storage of the waste form, or 4) develop a lower pH process/waste form thereby precluding ammonia release.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Modeling delayed thermal runaway in nitric acid-soaked cat litter mixed with radioactive waste
Thermal ignition of radioactive waste within a 55-gallon drum was simulated by using a pressure-dependent waste decomposition model (Hobbs et al. in Process Saf Environ Prot https://doi.org/10.1016/j.psep.2022.09.047, 2022) calibrated with data from full-scale drum experiments (Parker et al. in The thermolytic response of a surrogate RNS waste mixture at the drum scale. Los Alamos National Laboratory Report LA-UR-16-21760, 2016) and validated with experiments from multiple laboratories (Hobbs et al. in Thermal analysis of aged nitric acid-soaked kitty litter in TRU waste drums-23370.WM2023 Conference, Phoenix, AZ, 2023). The acceleration of nitric acid chemistry reacting with an organic cat litter leading to thermal ignition was likely triggered by a restricted vent in the drum. Here, we address whether the form of the rate equation in (Hobbs et al. in Process Saf Environ Prot https://doi.org/10.1016/j.psep.2022.09.047, 2022) is sufficient to extrapolate thermal ignition within aged drums of similar content that have been stored in Texas for over nine years by investigating four different reaction rate forms for waste decomposition. A critical reaction rate reduction analysis is performed on each of these models to determine if delayed thermal runaway within vented aged waste is possible after nine years. We found that a pressure-dependent first-order rate expression not only predicted the accidental ignition of the waste drum, but the form also matches multiple experiments from different laboratories. Even though the waste composition decreases over time, the model predicts that acceleration leading to thermal runaway is possible if the waste is confined, even after 9 years. In conclusion, waste containing oxidizers such as nitric acid should not be mixed with organic adsorbents, especially if the waste is confined.
cookoff↗
Designing Advanced Ceramic Waste Forms for Electrochemical Processing Salt Waste
This report describes the scientific basis underlying the approach being followed to design and develop “advanced” glass-bonded sodalite ceramic waste form (ACWF) materials that can (1) accommodate higher salt waste loadings than the waste form developed in the 1990s for EBR-II waste salt and (2) provide greater flexibility for immobilizing extreme waste salt compositions. This is accomplished by using a binder glass having a much higher Na 2 O content than glass compositions used previously to provide enough Na+ to react with all of the Cl– in the waste salt and generate the maximum amount of sodalite. The phase compositions and degradation behaviors of prototype ACWF products that were made using five new binder glass formulations and with 11-14 mass% representative LiCl/KCl-based salt waste were evaluated and compared with results of similar tests run with CWF products made using the original binder glass with 8 mass% of the same salt to demonstrate the approach and select a composition for further studies. About twice the amount of sodalite was generated in all ACWF materials and the microstructures and degradation behaviors confirmed our understanding of the reactions occurring during waste form production and the efficacy of the approach. However, the porosities of the resulting ACWF materials were higher than is desired. These results indicate the capacity of these ACWF waste forms to accommodate LiCl/KCl-based salt wastes becomes limited by porosity due to the low glass-to-sodalite volume ratio. Three of the new binder glass compositions were acceptable and there is no benefit to further increasing the Na content as initially planned. Instead, further studies are needed to develop and evaluate alternative production methods to decrease the porosity, such as by increasing the amount of binder glass in the formulation or by processing waste forms in a hot isostatic press. Increasing the amount of binder glass to eliminate porosity will decrease the waste loading from about 12% to 10% on a mass basis, but this will not significantly impact the waste loading on a volume basis. It is likely that heat output will limit the amount of waste salt that can be accommodated in a waste canister rather than the salt loading in an ACWF, and that the increase from 8 mass% to about 10 mass% salt loadings in ACWF materials will be sufficient to optimize these waste forms. Although the waste salt composition used in this study contained a moderate amount of NaCl, the test results suggest waste salts with little or no NaCl can be accommodated in ACWF materials by using the new binder glass, albeit at waste loadings lower than 8 mass%. The higher glass contents that will be required for ACWF materials made with salt wastes that do not contain NaCl are expected to result in much lower porosities in those waste forms.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
International Low Level Waste Management Practices and Technical Bases for Very Low Level Waste Classification - 19415
Different countries around the globe use varying schemes for the classification of radioactive waste. Many countries use adaptations of the International Atomic Energy Agency (IAEA) waste classification scheme. The United States uses the Class A, B, and C waste classification scheme that is loosely based on the IAEA concepts. Classification may be based on concentration limits or dose rate limits or a combination of concentration and dose rate limits. In some countries the existence of very low-level waste categories allows nuclear power plant waste to be disposed of in hazardous waste or shallow land burial sites separate from low and intermediate level waste disposal facilities. In the United States, the very low-level waste (VLLW) classification does not exist. Nuclear power plants use alternative disposal procedures under 10CFR20.2002 and other licensed processes in agreement states in order to dispose of very low activity waste in hazardous waste disposal sites. [1] Disposal of VLLW in hazardous waste or separate VLLW facilities is generally more cost effective than disposing of waste in radioactive waste sites and is protective of the health and safety of the public. This can become an important factor when large volumes of very low activity waste are generated during decommissioning of nuclear power plants. The Electric Power Research Institute (EPRI) Radiation Safety (RS) Program has developed technical bases for the establishment of a very low-level waste category. EPRI studied how VLLW waste is defined, managed, and disposed of in various countries. This included the study of disposal site design, characteristics, and how these sites protect the health and safety of the environment and the public from low levels of radioactivity. EPRI conducted a cost benefit analysis to understand the economic impact of disposing VLLW in hazardous waste disposal sites versus low-level waste disposal sites. Finally, EPRI calculated potential radionuclide limits that may be used to define very low-level waste. The purpose of this work was to provide an example of how one might approach defining limits for VLLW. The same or similar approaches could be applied to derive radionuclide limits for different dose limit objectives. This paper presents the results of research that explored the waste management and disposal practices at six countries around the world with additional focus and details on the implementation of the very low-level waste category. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Canadian Nuclear Laboratories Waste Management: Challenges and the Integrated Waste Strategy - 19160
Canadian Nuclear Laboratories (CNL) currently faces various waste management challenges and CNL's Integrated Waste Strategy is adapting to manage them. As Canada's premier nuclear science and technology organization, CNL is a global leader in developing peaceful and innovative applications from nuclear technology through its expertise in the scientific field, including physics, metallurgy, chemistry, biology and engineering. As demands change, CNL is shifting its focus to alpha therapies for cancer treatments and sustainable energy solutions. The next decade will see CNL decommission the sites it manages across Canada, whilst transforming Chalk River Laboratories (CRL) into a new, world-class facility which will have the capability to demonstrate the commercial viability of advanced reactor designs including Small Modular Reactors (SMRs). This is being enabled through an accelerated decommissioning program for all CNL operated sites, while renovating CRL, which includes revitalizing essential site infrastructure, and investment in new, world-class science facilities in a modern campus environment. With decommissioning and revitalization occurring simultaneously, the long-term strategy and vision for CNL presents some unique challenges to waste management. Therefore, integrated, collaborative and coordinated waste management is a vital component to ensuring a successful future. The Integrated Waste Strategy coordinates, and provides alignment of, waste management across CNL and: - Includes all CNL operated (Atomic Energy of Canada Limited (AECL) owned) sites; - Considers all CNL managed waste (including radioactive and non-radioactive operational, decommissioning, legacy and historic waste) for the planned lifetime of the sites; - Defines waste routes using a life cycle approach (from the generation of waste to final disposal) A baseline Integrated Waste Strategy and associated action plan to mitigate identified gaps and issues have been produced. A program of work is underway to close those gaps identified in a consistent, transparent, prioritized and justified manner. One of the key challenges is to ensure that waste management planning is completed effectively and in a timely manner. This will enable the provision of suitable and sufficient waste capability to meet CNL's long-term strategy. The Integrated Waste Strategy has been developed and maintained through engagement at all levels across CNL, ensuring buy-in of proposed solutions. Key process stakeholders include generators of CNL managed waste to ensure integrated consideration of legacy, current and future waste generation; waste management personnel to identify requirements, including processing, storage, transport and disposal; AECL as the client and waste liability owner; and the public to ensure they understand the 'big picture' regarding waste strategy. (author)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Implementing a Direct-Feed Low-Activity Waste Capability in the Hanford Waste Treatment Plant - 18332
The original design of the Waste Treatment and Immobilization Plant (WTP) requires that all waste be processed through the Pretreatment (PT) Facility in order to separate the low-activity waste and high-level waste streams. The U.S. Department of Energy (DOE) has developed a sequenced approach to completing the WTP Project, beginning with feeding some liquid waste directly to the Low-Activity Waste (LAW) Facility, bypassing the PT Facility. Sending low-activity waste from the tank farms to the LAW Facility is referred to as direct-feed LAW (DFLAW). Under this plan, low-activity waste will be pretreated in the Hanford tank farms for cesium and solids separation to meet LAW Facility waste acceptance criteria and produce an acceptable low-activity waste product. The waste feed will then be transferred to the LAW Facility where it will be immobilized in glass, poured into stainless steel containers, and then transported by truck to the Integrated Disposal Facility, a mixed low-level waste disposal site located in the Hanford 200 East Area. The DFLAW operation will deliver about 1 million gallons of double-shell tank waste for treatment each year of operation, and nominally produce 21 metric tons of immobilized low-activity waste glass per day. The resultant freed space in the double-shell tanks will support safe tank farm operations and staging of additional waste for treatment. In December 2016 DOE executed a contract modification and approved a change to the project's performance baseline to complete the LAW Facility, Balance of Facilities (BOF), and Analytical Laboratory (LAB) and incorporate modifications needed to allow direct feed of low-activity waste to the LAW Facility. The contract modification and revised performance baseline support completion and hot commissioning of WTP facilities needed for DFLAW operations is as early as January 2022. DOE has made significant progress on design, equipment procurements, and civil construction of modifications required to implement the DFLAW capability in the WTP, including progress on civil construction of a new effluent management facility, which will process secondary liquid waste resulting from LAW Facility vitrification operations. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Implementing a Low Activity Waste Direct Feed Capability in the Hanford Waste Treatment Plant - 17277
The original design of the Waste Treatment and Immobilization Plant (WTP) requires that all waste be processed through the Pretreatment (PT) Facility in order to separate the low-activity waste and high-level waste streams. The U.S. Department of Energy (DOE) has developed a sequenced approach to completing the WTP Project, beginning with feeding some liquid waste directly to the Low-Activity Waste (LAW) Facility, bypassing the PT Facility. Sending low-activity waste from the tank farms to the LAW Facility is referred to as direct-feed LAW (DFLAW). Using this approach, low-activity waste will be pretreated in a Low-Activity Waste Pretreatment System (LAWPS) for cesium and solids separation to meet LAW Facility safety basis requirements and produce an acceptable low-activity waste product. The waste feed will then be transferred to the LAW Facility where it will be immobilized in glass, poured into stainless steel containers, and then transported by truck to the Integrated Disposal Facility, a mixed waste burial ground located in the Hanford 200-East Area. The primary driver for the DFLAW approach is to enable commissioning of the LAW Facility for low-activity waste processing prior to the completion and availability of the PT and High-Level Waste (HLW) facilities. As such, the functions intended to be provided to the LAW Facility by the PT Facility and the common functionality with the HLW Facility must be refined and modified to enable DFLAW operations. The DFLAW approach will provide necessary systems and facilities to replace these enabling PT Facility functions until the PT Facility is completed and commissioned. For example, liquid effluents from the LAW Facility, primarily melter offgas condensate, will be processed in a new effluent management facility (EMF) within the WTP footprint rather than sending the effluent back to the PT Facility for processing. During DFLAW operations approximately 3 785 m{sup 3} (1 million gallons) of double-shell tank (DST) waste will be delivered to WTP for treatment each year of operation, and nominally produce 21 metric tons of immobilized low-activity waste glass per day. The resultant freed space in the DSTs will support safe tank farm operation and staging of additional waste for treatment. In December 2016, DOE executed a contract modification and approved an incremental change to the project's performance baseline to complete the WTP facilities needed to allow direct feed of low-activity waste to the LAW Facility. The revised performance baseline supports completion and cold commissioning of the WTP facilities needed for DFLAW operations no later than August 2023. The design of modifications to WTP facilities needed to enable DFLAW operations is more that 60 percent complete. DOE approved the preliminary safety basis for DFLAW modifications to WTP based on the 30 percent design package in early 2016. Early construction work for DFLAW modifications to WTP began in mid-2015. Long-lead procurement actions for some of the more complex equipment needed for LAW Facility effluent treatment were initiated in early 2016. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗