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This project focuses on the novel use of interfacial hydrated layers in ionic conducting ceramic materials for tritiated water (HTO) adsorption and recovery. Low-temperature water adsorption properties of nanoscale structured ceramics combined with hydrogen isotope exchange in their hydrated layers could provide a low-cost and transformative avenue to address tritium management challenges.
The solubility of uranium (VI) in Waste Isolation Pilot Plant (WIPP)-relevant brine was determined to support ongoing WIPP recertification activities. This research was performed by the Los Alamos National Laboratory Carlsbad Operations (LANL-CO) Actinide Chemistry and Repository Science Program (ACRSP). The WIPP Actinide Source Term Program (ASTP) did not develop a model for the solubility of actinides in the VI oxidation state. The solubility of UO 2 2+ , in the absence of WIPP specific data, is presently set to be equal to a conservatively high 1 mM within the WIPP Performance Assessment (PA) for all expected WIPP conditions (SOTERM, 2019) as selected at the recommendation of the Environment Protection Agency (EPA) (EPA, 2005). According to the current WIPP chemistry model assumptions and conditions, the expected pC H+ is about 9.5 and controlled by MgO buffering CO 3 2- . The goal of this study is to perform screening experiments that account for the contributions of organics and borate on uranium solubility. In this report, the solubility of U(VI) was determined at pC H+ 9 WIPP brine in the absence or presence of borate and organics at under-saturation approach. Experiments were equilibrated for about 135 days. Organic compounds present in WIPP waste can form strong complexes with actinides and can affect the oxidation states of actinides. The organic compounds addressed in WIPP performance assessment include EDTA (Ethylenediaminetetraacetic Acid), oxalate, citrate, and acetate (SOTERM, 2019). These data quantify the effects of WIPP-relevant concentrations of borate and organics effects on the solubility of U(VI) to challenge the predictions of the WIPP actinide model and inform decisions and recommendations made in the upcoming recertification of the WIPP (CRA-2024). The experiments performed were done according to the U.S. Department of Energy (DOE) approved Test Plan entitled “Experimental Strategy to Challenge Actinide Solubility Predictions” and designated LCO-ACP-26. All data reported were obtained under the LANL-CO Quality Assurance Program, which is compliant with the DOE Carlsbad Field Office, Quality Assurance Program Document (CBFO/QAPD) (QAPD, 2017).
This report provides experimental details and results on the elemental distributions (compositions), crystalline/amorphous phase distribution, and microstructures for DPF5-336 reference materials made with ERV3b salt that were subjected to the canister centerline cooling (CCC) heat treatment process. To fabricate these materials, ammonium dihydrogen phosphate was mixed with ERV3b salt simulant and a dechlorination procedure was run in the generation-2 dechlorinator at the Pacific Northwest National Laboratory up to 600°C in an alumina crucible. After the dechlorination process, the product was removed from the crucible, lightly crushed, loaded into a new alumina crucible, Fe 2 O 3 was added, and this was vitrified at 1100°C for 1 hour and quenched. The quenched material was mostly amorphous but showed some small diffraction peaks attributed to Li 3 Fe 2 (PO 4 ) 3 . This quenched material was ground to a fine particle size in a milling chamber, and this was subjected to the CCC cooling profile in duplicate within alumina and fused quartz crucibles. The CCC experiment is designed to simulate the slowest cooling profile (the vertical centerline) of a 0.61-m diameter canister where the slower cooling profile often results in the production of a variety of different crystalline phases upon formation of which result in a residual glass of unknown composition and properties. The information gleaned from these types of experiments will lead to improved composition-property predictions for materials with similar compositions. The results of the alumina and fused quartz experiments show different microstructures but similar diffraction patterns providing evidence of similar crystalline phases being present in each sample. Both samples had monazite [i.e., (Ce,Nd)PO 4 ] and mixtures of phases containing P, Fe, and alkali metal elements. This report completes the milestone M4FT-23PN030104042 with details provided in Appendix B.
Mineralization of industrial waste and earth-abundant CO2 into value-added products is a powerful method of utilizing domestic resources to produce value from waste. Carbonate minerals formed from Ca and Mg rich waste streams are key constituents in cement and concrete, which are in demand at the gigaton-scale every year. While thermodynamically favorable, CO2 mineralization is hindered by slow kinetics, and traditional thermochemical routes are too expensive to scale. Here, we demonstrate the advantages of an electrochemical method of waste valorization, which eliminates this limitation and improves kinetics. We highlight this method's ability to initiate crystallization under favorable local conditions, producing carbonates from mining waste at mildly acidic pH. We highlight the effects of key constituents in mining waste on the mineralization process.
The use of fuel reformate from catalytic processes is known to have beneficial effects on the spark-ignited (SI) combustion process through enhanced dilution tolerance and decreased combustion duration, but in many cases reformate generation can incur a significant fuel penalty. In a previous investigation, the researchers showed that, by controlling the boundary conditions of the reforming catalyst, it was possible to minimize the thermodynamic expense of the reforming process, and in some cases, realize thermochemical recuperation (TCR), a form of waste heat recovery where exhaust heat is converted to usable chemical energy. The previous work, however, focused on a relatively light-load engine operating condition of 2000 rpm, 4 bar brake mean effective pressure (BMEP). The present investigation demonstrates that this operating strategy is applicable to higher engine loads, including boosted operation up to 10 bar BMEP. By controlling the reforming catalyst boundary conditions, it is possible to achieve fuel reforming without experiencing high temperature exotherms that could be damaging to the catalyst. Additionally, the thermodynamic air handling consequences of operating a highly dilute strategy at high loads is quantified. Furthermore the results confirm that this operating strategy provides an efficiency benefit at all conditions investigated, with relative efficiency increases of 3-6%, and is therefore applicable over wider regions of the engine operating map.
In prior work, the EGR loop catalytic reforming strategy developed by ORNL has been shown to provide a relative brake engine efficiency increase of more than 6% by minimizing the thermodynamic expense of the reforming processes, and in some cases achieving thermochemical recuperation (TCR), a form of waste heat recovery where waste heat is converted to usable chemical energy. In doing so, the EGR dilution limit was extended beyond 35% under stoichiometric conditions. In this investigation, a Microlith®-based metal-supported reforming catalyst (developed by Precision Combustion, Inc. (PCI)) was used to reform the parent fuel in a thermodynamically efficient manner into products rich in H2 and CO. We were able to expand the speed and load ranges relative to previous investigations: from 1,500 to 2,500 rpm, and from 2 to 14 bar break mean effective pressure (BMEP). Experiments were conducted to determine the effects of the H/C ratio of the fuel on H2 production and on the engine efficiency in order to compare E10 gasoline (H/C = 1.95) and liquified petroleum gas (LPG), comprised primarily of propane (H/C = 2.67). Additionally, the compression ratio of the engine was increased to ascertain whether further efficiency improvements could be realized based on a reduced knock propensity of the dilute EGR mixture with the reformed fuel. Both the gasoline and propane reforming strategies provided efficiency gains up to 1.85 percentage points and further efficiency improvements with the increased compression ratio were realized. The fuel specific effects of gasoline vs. LPG, the effect of engine operating condition on reforming, and knock limits of the reformed mixture are discussed in detail.
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The National Renewable Energy Laboratory (NREL) develops and de-risks a portfolio of technologies for converting renewable carbon resources into sustainable fuels, including sustainable aviation fuel (SAF). NREL works with industry, academia, and other national laboratories to develop, scale, and de-risk technology pathways for producing SAF from renewable resources such as biomass and other forms of waste carbon, including carbon dioxide.
The National Nuclear Laboratory (NNL) and Kurion Veolia (Kurion) have installed a GeoMelt{sup R} In-Container Vitrification (ICV){sup R} radioactive waste treatment system in the Central Laboratory Active Rig Hall at Sellafield. This installation was completed in 2016. GeoMelt incorporates a range of patented and proprietary vitrification processing technologies that are configured in a variety of ways depending on the project and the waste. GeoMelt transforms hazardous chemical and radioactive wastes into an inert vitreous monolith. Hazardous organics are destroyed by pyrolysis and heavy metals and radionuclides are immobilized within the glass matrix where they are not preferentially leached into the environment. GeoMelt IVC produces a durable wasteform for a large variety of input wastes. The batch nature of the process which involves single-use refractory offers a wide range of process benefits over traditional vitrification technologies including: - a wide range of waste chemistries allowing high waste loadings; - compatibility with heterogeneous wastes including wastes with high metal content; - a technological simple solution without stirrers, bubblers, etc.; - No refractory corrosion concerns or melter drain failure scenarios; - Flexibility in glass chemistry and melter/disposal container configuration allows the wasteform to be specifically tailored to the storage or disposal site requirements. As part of the 2016 system commissioning at NNL's Central Laboratory, three demonstration melts were performed, one funded by Sellafield Ltd. and two by the Nuclear Decommissioning Authority (NDA). The first melt processed inactive soil with an inactive caesium tracer. The second melt processed inactive soil with a Cs-137 tracer. The third melt processed active waste soil from a variety of NDA nuclear licensed sites. The work conducted during commissioning was multi-purpose; it successfully demonstrated the benefits that the GeoMelt technology could bring to the UK NDA estate while performing equipment testing/troubleshooting and operator training. A significant benefit of the GeoMelt ICV technology is volume reduction for wastes which would otherwise experience a volume increase if encapsulated. Another benefit is the ability to treat difficult radioactive waste streams not amenable to encapsulation (e.g., reactive and/or organic wastes) with a very low energy consumption. The purpose of the first commissioning melt, Plant Performance Demonstration (PPD)-1, was to operate the GeoMelt system under typical conditions and to perform a post-melt mass balance of the caesium as a surrogate for Cs-137 in order to access retention of caesium in the final glass product. The melt processed a mixture of inactive soil obtained near the Sellafield site (as analogue for contaminated Sellafield soil), additives, and glass frit. An inactive caesium tracer was added to this melt as Cs{sub 2}CO{sub 3}. The purpose of the second commissioning melt, PPD-2, was to operate the GeoMelt system under typical conditions and to perform a post-melt activity balance using a Cs-137 tracer in order to assess retention of Cs-137 in the final glass product. Materials processed were inactive soil, glass frit, additives, and a radioactive caesium tracer (CsCl). The purpose of the third melt, Experiment-1 (EX-1) was to treat active waste and inactive waste simulant, as a demonstration of simultaneous processing of multiple waste streams. EX-1 consisted of processing active soil, Magnox sludge simulant, inactive soil, additives, and frit. The active soil used for this melt was obtained from the Hunterston A, Bradwell, Capenhurst, and Sellafield nuclear licensed sites. Since most soils are high in silica, the concept for this experiment was to use the active soils to provide glass formers while co-processing Magnox sludge simulant which does not contain glass formers. Beyond demonstration of capability areas of focus of this series of demonstrations included processing efficiency (kWh/kg treated) and caesium retention (%). This paper summarizes operations and results of the three melts. (authors)
This paper presents the features and performance record of the geo-polymer solidification technology, SIAL{sup R}, licensed for use by both the Slovakian (UJD SR) and Czech Nuclear (SUJB) regulators. An overview of its performance at Bohunice in Slovakia, where it has been used to successfully treat resins and sludge wasteforms will be provided along with references to other plants where it has been used. More recently, geo-polymers have been noted as an immobilization technology which shows potential for resins produced by treatment of radioactive contaminated water resulting from the clean-up of the Fukushima Daiichi Plant. The Nuclear Power Plant A-1 located in Jaslovske Bohunice was completed in 1972 and operated for 5 years until two accidents in 1976 and 1977. After the second accident in February 1977 (INES level 4) the Nuclear Power Plant was permanently shut down for decommissioning. Fuel assemblies and fuel cladding damaged in the accidents led to significant Sr-90, Cs-137 and transuranic contamination. As a consequence of the long-term corrosion of the barrier's material, highly contaminated sludge accumulated which could not be effectively immobilized using conventional methods such as cementation or bitumen treatment due to adverse physical-chemical properties and high specific activity of the waste (Cs-137). This challenge led to AMEC developing and licensing the geo-polymer, SIAL{sup R}. Today, this geo-polymer is one of the most proven and widely used for on-site solidification of radioactive materials such as sludge, resins, sorbents and organic liquids. There are numerous benefits to using this geo-polymer for waste immobilisation. It can be used at room temperature and can incorporate up to approximately four times as much waste (sludge, resin) as a Portland cement matrix equivalent depending on the waste being treated. In addition, it is characterized by excellent mechanical and physical properties, compared with the earlier generation techniques. This includes higher mechanical strength, lower leachability, low volatility, posing a low fire risk and excellent physical stability in the presence of frost and water (no distortion or cracking). Dedicated facilities to receive and encapsulate waste from different locations can be created but this geo-polymer can also provide efficient and practical on-site treatment of radioactive waste streams. This is achievable because the equipment used to encapsulate waste using SIAL{sup R} is also modular, flexible and versatile. At Bohunice, the facility for encapsulation was designed to occupy existing areas of the plant in close proximity to the tanks where the waste was being stored. This allowed for the removal of the waste using Remote Operated Vehicles (ROVs) and for the waste to be immediately treated on site without the need for transportation saving both time and resource. To achieve this, some of the rooms and areas of the building were assessed and modified to ensure that the waste package flow was suitable whilst ensuring that appropriate safety measures were in place such as adequate shielding to reduce or entirely eliminate dose uptake of workers. To date, SIAL{sup R} has been used to successfully immobilize approximately 500 tons of waste which includes sludge and resin from Bohunice, Slovakia and approximately 250 m{sup 3} of spent ion exchange resins from tanks on site at the Dukovany nuclear plant, Czech Republic. It now has a track record of over 15 years which includes on-going research and development. The International missions WANO and OSART evaluated the SIAL{sup R} matrix technology at NPP Dukovany as an example of good practice. (authors)
Nuclear energy is thought to be one of the energy sources that could help mitigating the global climate change together with the renewables, due to its low green-house-gases emissions, its reliability and its high load power. However, nuclear energy will only develop if future nuclear energy systems meet the criteria of sustainability in terms of durability, bearability and liveability. Nowadays, many countries chose the so-called once-through cycle which basically considers spent nuclear fuel as a waste, whereas others reprocess their spent fuel to recover the energetically-valuable material Pu (and partially U) to produce Mixed Oxide Fuel (MOX) to be irradiated in a second cycle (twice-through cycle). Both options can be considered relevant, fitting diverse criteria; but if we consider a long lasting prospective for nuclear options, the once-through cycle sustainability is clearly lower (low consumption of natural resource, no recycling of potentially valuable energetic material, larger volume of waste...). Reversely, twice-through cycle can be seen as a first step towards an improved sustainability with a partial recycling of U/Pu and the reduction of the waste volume and toxicity. However, it is likely not sufficient for the long-term and implementing more efficient recycling is a key-driver to improve the environmental friendship, the economics and the social acceptability of nuclear energy. Future nuclear fuel cycles will have to better preserve the natural resource by improving the actinides recycling, to minimize the volume and toxicity of nuclear waste, to ensure their long-term confinement and to prevent any proliferation-risk. Such a gradual and progressive process calls for implementing appropriate technologies, either for reactors but also for fuel treatment/recycling facilities. This paper will describe the successive step that would allow improving the overall sustainability. Indeed, recycled Pu can be once recycled in MOX fuel feeding similar PWRs (Pressurized Water Reactor). Together with the recycling of reprocessed uranium, this first step already allows preserving ∼17% of the natural U resource and to confine ultimate wastes without Pu in a tailored durable wasteform. Subsequent Pu multi-recycling requires introducing Fast Reactors (FR) to efficiently use U-238 available in natural and depleted uranium stockpiles. In parallel, recycling processes would have to be adapted for treating spent LWR and SFR MOX spent fuels, which is currently under study thanks to an ambitious R and D program dedicated on MOX treatment and recycling. For the longer term, minor actinides recycling would allow decreasing the waste burden towards future generations: (i) Am-recycling leads to decrease the waste residual heat-power and increase the repository density and lifespan, (ii) Cm-recycling leads to decrease waste long-term toxicity. The stepwise implementation of these different processes defines a path towards sustainability for nuclear energy that are described in this paper from the fuel cycle viewpoint. (authors)
The legacy of nuclear waste at the Sellafield site in the UK is an ongoing issue, and the current preferred route for the disposal of low and intermediate level waste is encapsulation in a cementitious matrix, formulated by blending Portland cement with blast furnace slag (BFS). Due to demands and economic challenges faced by the cement and steel industries, the supply of BFS to the UK nuclear industry has been inconsistent. These changes have caused the industry to move from a unique BFS powder supply with a certain specification to a combination of standard commercially available cementitious powders. The material currently used at the Sellafield site is a blend of ground granulated blast furnace slag (GGBS) and a coarser fraction of the same composition called Calumite, combined with Portland cement. This work involves future-proofing the supply of BFS for the UK nuclear industry by optimising the blend of the two fractions of BFS in order to replicate the unique specification required by Sellafield Ltd. The main emphasis is on the particle size distribution (PSD) and how this impacts the properties of the final wasteform. The study investigates the performance properties of the blended grouts such as workability, particle packing and heat evolution. Results show that the PSD of the cement powders affect both the physical and chemical properties of the cementitious matrix produced. (authors)
Thermal treatment of nuclear waste in the UK has seen much renewed interest recently, owing to the advantages that can be gained in terms of reduced waste volumes, compatibility with reactive metals and organics and its ability to treat mixed generic wastes. Vitrification is a treatment option which destroys organics and some hazardous inorganics such as asbestos, reduces wasteform volume, and produces a robust leach resistant wasteform. Kurion's GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} is a vitrification process where the treatment vessel can serve as an interim-storage, transport, and final long-term storage vessel - thus negating the need to pour glass into a separate container, effectively leading to a much simpler system than traditional waste melters. The UK's National Nuclear Laboratory (NNL) and Kurion have entered into a joint project to deploy an active waste ICV{sup TM} plant based on Kurion's GeoMelt{sup R} technology, at NNL's flagship Central Laboratory on the Sellafield site. NNL is the UK's national laboratory for civil nuclear science and technology, providing advice to government, protecting key skills, supporting industry and delivering national nuclear programs. NNL is bringing the Kurion GeoMelt{sup R} process alongside its existing capabilities in thermal waste treatment. Kurion provides technology solutions to minimize and stabilize nuclear and hazardous waste through its families of technologies: access, separation and stabilization processes. The GeoMelt{sup R} plant being installed at the NNL's Central Laboratory creates a platform to evaluate the vitrification technology for the variety of wastes from the NDA estate and creates a treatment path for problematic waste streams that currently have no disposition pathway. With the diverse facilities under NNL management coupled with the NNL's ability to import wastes from within the UK and Europe, this arrangement with Kurion provides waste owners with treatment disposition pathways for problematic wastes. The Kurion / NNL team completed non-radioactive commissioning of a GeoMelt{sup R} ICV{sup TM} treatment system in 2015. Commissioning consisted of performing two tests at NNL's Workington Laboratory. Commissioning Test 1 involved vitrification of 367 kg of glass frit over the course of approximately 18 hours. Commissioning Test 2 consisted of processing 470 kg of soil and additives in approximately 27 hours. The soil processed in the second test was non-radioactive soil from Sellafield and was used as an analog for radioactive soil to be processed during radioactive commissioning at the Central Laboratory at Sellafield. All commissioning test goals were easily achieved and all subsystems operated as designed. Radioactive commissioning will be carried out in early 2016. (authors)
One or more embodiments relates to a process for extracting Rare Earth Elements (REEs) from REE-bearing underclays, claystones, shales, coal-mining waste, and waste coal. In at least one embodiment the process includes contacting the REE-bearing underclays, claystones, shales, coal-mining waste, and waste coal with an Organic Acid Solution (OAS) comprising at least one organic acid and at least one ionic salt at a predetermined ambient temperature and predetermined pH; and separating the REE from the REE-bearing underclays, claystones, shales, coal-mining waste, and waste coal, forming REE+Yttrium (REY) concentrate.
Tc-99m, the most commonly used radioisotope in nuclear medicine, is produced from the decay of Mo-99 which is predominantly produced in reactors by irradiation of enriched uranium targets. This results in three waste streams, one of which is a uranium filter cake containing fission products. This filter cake could itself be treated as a waste stream, or processed to retrieve the enriched uranium for further use, thus producing additional waste streams during reprocessing. All wastes are considered intermediate-level wastes and require an appropriate wasteform design for termination. ANSTO is collaborating with NECSA (Nuclear Energy Corporation of South Africa) to develop wasteform and processing solutions for the treatment of intermediate level wastes (ILW) from the production of Mo-99. The work is supported by the U.S. Department of Energy's (DOE) National Nuclear Security Administration (NNSA) with technical support from Argonne National Laboratory (ANL). Here we highlight some of the outcomes of this collaboration which has seen the investigation and performance testing of a range of waste treatment technologies. Among the treatment options for the various waste streams, including the enriched uranium filter cake itself, were glass, glass-ceramic, ceramic and geopolymer wasteforms. All wasteforms were characterized (e.g., by X-ray diffraction (XRD) and scanning electron microscopy (SEM)) and their performance characteristics, for example compressive strength and aqueous durability, determined by standard methods and compared. Consideration has been given to the most suitable, practical and cost effective solutions for the immobilization of these Mo-99 wastes. This paper will discuss the down-selection of wasteforms and process technologies for Mo-99 wastes and compare these with regards to wasteform performance and process technology readiness. (authors)
ANSTO is building a nuclear waste treatment plant that represents a significant step change in the treatment of intermediate-level waste (ILW) from Molybdenum-99 nuclear medicine production. This industrial scale facility shall deploy ANSTO Synroc technologies; a wasteform tailored for immobilizing fission products, an integrated process line for converting liquid waste into free-flowing powder, automated canister filling and sealing, and a hot isostatic pressing (HIP) system designed for remote operation. The HIP represents the last processing step to consolidate the wasteform into a final durable solid compact with the required performance characteristics. This paper shall outline the various phases of development in realising the final plant design as well as timelines to progress through cold- and hot-commissioning. Further, plans for storage and final disposal of the HIPed canister product will be discussed. (authors)