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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,189 records · Page 66
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

pH-oscillations in the bromate–sulfite reaction in semibatch and in gel-fed batch reactors

The simplest bromate oxidation based pH-oscillator, the two component BrO{sub 3}{sup −}–SO{sub 3}{sup 2–} flow system was transformed to operate under semibatch and closed arrangements. The experimental preconditions of the pH-oscillations in semibatch configuration were predicted by model calculations. Using this information as guideline large amplitude (ΔpH∼3), long lasting (11–24 h) pH-oscillations accompanied with only a 20% increase of the volume in the reactor were measured when a mixture of Na{sub 2}SO{sub 3} and H{sub 2}SO{sub 4} was pumped into the solution of BrO{sub 3}{sup −} with a very low rate. Batch-like pH-oscillations, similar in amplitude and period time appeared when the sulfite supply was substituted by its dissolution from a gel layer prepared previously in the reactor in presence of high concentration of Na{sub 2}SO{sub 3}. The dissolution vs time curve and the pH-oscillations in the semibatch and closed systems were successfully simulated. Due to the simplicity in composition and in experimental technique, the semibatch and batch-like BrO{sub 3}{sup −}–SO{sub 3}{sup 2–} pH-oscillators may become superior to their CSTR (continuous flow stirred tank reactor) version in some present and future applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Reversible migration of silver on memorized pathways in Ag-Ge{sub 40}S{sub 60} films

Reversible and reproducible formation and dissolution of silver conductive filaments are studied in Ag-photodoped thin-film Ge{sub 40}S{sub 60} subjected to electric fields. A tip-planar geometry is employed, where a conductive-atomic-force microscopy tip is the tip electrode and a silver patch is the planar electrode. We highlight an inherent “memory” effect in the amorphous chalcogenide solid-state electrolyte, in which particular silver-ion migration pathways are preserved “memorized” during writing and erasing cycles. The “memorized” pathways reflect structural changes in the photodoped chalcogenide film. Structural changes due to silver photodoping, and electrically-induced structural changes arising from silver migration, are elucidated using Raman spectroscopy. Conductive filament formation, dissolution, and electron (reduction) efficiency in a lateral device geometry are related to operation of the nano-ionic Programmable Metallization Cell memory and to newly emerging chalcogenide-based lateral geometry MEMS technologies. The methods in this work can also be used for qualitative multi-parameter sampling of metal/amorphous-chalcogenide combinations, characterizing the growth/dissolution rates, retention and endurance of fractal conductive filaments, with the aim of optimizing devices.

36 MATERIALS SCIENCE↗
DOE OSTI2015

An atomistically informed mesoscale model for growth and coarsening during discharge in lithium-oxygen batteries

An atomistically informed mesoscale model is developed for the deposition of a discharge product in a Li-O{sub 2} battery. This mescocale model includes particle growth and coarsening as well as a simplified nucleation model. The model involves LiO{sub 2} formation through reaction of O{sub 2}{sup −} and Li{sup +} in the electrolyte, which deposits on the cathode surface when the LiO{sub 2} concentration reaches supersaturation in the electrolyte. A reaction-diffusion (rate-equation) model is used to describe the processes occurring in the electrolyte and a phase-field model is used to capture microstructural evolution. This model predicts that coarsening, in which large particles grow and small ones disappear, has a substantial effect on the size distribution of the LiO{sub 2} particles during the discharge process. The size evolution during discharge is the result of the interplay between this coarsening process and particle growth. The growth through continued deposition of LiO{sub 2} has the effect of causing large particles to grow ever faster while delaying the dissolution of small particles. The predicted size evolution is consistent with experimental results for a previously reported cathode material based on activated carbon during discharge and when it is at rest, although kinetic factors need to be included. The approach described in this paper synergistically combines models on different length scales with experimental observations and should have applications in studying other related discharge processes, such as Li{sub 2}O{sub 2} deposition, in Li-O{sub 2} batteries and nucleation and growth in Li-S batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material

Introducing nanostructural second phases has been proved to be an effective approach to reduce the lattice thermal conductivity and thus enhance the figure of merit for many thermoelectric materials. Furthermore studies of the formation and evolution of these second phases are central to understanding temperature dependent material behavior, improving thermal stabilities, as well as designing new materials. We examined powder samples of PbTe-PbS thermoelectric material using in situ neutron diffraction and small angle neutron scattering (SANS) techniques from room temperature to elevated temperature up to 663 K, to explore quantitative information on the structure, weight fraction, and size of the second phase. Neutron diffraction data showed the as-milled powder was primarily solid solution before heat treatment. During heating, PbS second phase precipitated out of the PbTe matrix around 480 K, while re-dissolution started around 570 K. The second phase remained separated from the matrix upon cooling. Furthermore, SANS data indicated there are two populations of nanostructures. The size of the smaller nanostructure increased from initially 5 nm to approximately 25 nm after annealing at 650 K, while the size of the larger nanostructure remained unchanged. Our study demonstrated that in situ neutron techniques are effective means to obtain quantitative information to study temperature dependent nanostructural behavior of thermoelectrics and likely other high-temperature materials.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Role of Mg{sup 2+}, Sr{sup 2+}, and F{sup –} ions in octacalcium phosphate crystallization

We have synthesized octacalcium phosphate (OCP) in the presence of inorganic additives (magnesium, strontium, and fluoride ions) and studied the composition, morphology, thermal stability, and dynamic dissolution of the samples thus obtained. It has been shown that, in addition to OCP, magnesium and strontium ions favor the formation of brushite and hydroxyapatite (HA), whereas fluoride ions favor the formation of HA and fluorohydroxyapatite (FHA). We have proposed a process for the preparation of powder materials whose resorption kinetics in corrosive liquid media are corrected by adding dopants capable of activating the dissolution process.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Dataset documenting reaction-induced changes to five fractured foamed wellbore cement cores during CO2 fluid flow

This dataset consists of reconstructed CT scans for four fractured foamed cement cores, generated in the lab using Portland Class H cement, and associated processed data. The cements were exposed to reactive brines, and CT scans were take at different time points through the experiment. The CT imaging allows for the tracking of dissolution-induced changes to fracture morphology, as well as alteration and dissolution in the cement matrix.

Computed Tomography↗
DOE OSTI2015

Application of Generic Disposal System Models

This report describes specific GDSA activities in fiscal year 2015 (FY2015) toward the development of the enhanced disposal system modeling and analysis capability for geologic disposal of nuclear waste. The GDSA framework employs the PFLOTRAN thermal-hydrologic-chemical multi-physics code (Hammond et al., 2011) and the Dakota uncertainty sampling and propagation code (Adams et al., 2013). Each code is designed for massively-parallel processing in a high-performance computing (HPC) environment. Multi-physics representations in PFLOTRAN are used to simulate various coupled processes including heat flow, fluid flow, waste dissolution, radionuclide release, radionuclide decay and ingrowth, precipitation and dissolution of secondary phases, and radionuclide transport through the engineered barriers and natural geologic barriers to a well location in an overlying or underlying aquifer. Dakota is used to generate sets of representative realizations and to analyze parameter sensitivity.

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

Alternative Chemical Cleaning Methods for High Level Waste Tanks: Simulant Studies

Solubility testing with simulated High Level Waste tank heel solids has been conducted in order to evaluate two alternative chemical cleaning technologies for the dissolution of sludge residuals remaining in the tanks after the exhaustion of mechanical cleaning and sludge washing efforts. Tests were conducted with non-radioactive pure phase metal reagents, binary mixtures of reagents, and a Savannah River Site PUREX heel simulant to determine the effectiveness of an optimized, dilute oxalic/nitric acid cleaning reagent and pure, dilute nitric acid toward dissolving the bulk non-radioactive waste components. A focus of this testing was on minimization of oxalic acid additions during tank cleaning. For comparison purposes, separate samples were also contacted with pure, concentrated oxalic acid which is the current baseline chemical cleaning reagent. In a separate study, solubility tests were conducted with radioactive tank heel simulants using acidic and caustic permanganate-based methods focused on the “targeted” dissolution of actinide species known to be drivers for Savannah River Site tank closure Performance Assessments. Permanganate-based cleaning methods were evaluated prior to and after oxalic acid contact.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Advances in Geologic Disposal System Modeling and Application to Crystalline Rock

The Used Fuel Disposition Campaign (UFDC) of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Fuel Cycle Technology (OFCT) is conducting research and development (R&D) on geologic disposal of used nuclear fuel (UNF) and high-level nuclear waste (HLW). Two of the high priorities for UFDC disposal R&D are design concept development and disposal system modeling (DOE 2011). These priorities are directly addressed in the UFDC Generic Disposal Systems Analysis (GDSA) work package, which is charged with developing a disposal system modeling and analysis capability for evaluating disposal system performance for nuclear waste in geologic media (e.g., salt, granite, clay, and deep borehole disposal). This report describes specific GDSA activities in fiscal year 2016 (FY 2016) toward the development of the enhanced disposal system modeling and analysis capability for geologic disposal of nuclear waste. The GDSA framework employs the PFLOTRAN thermal-hydrologic-chemical multi-physics code and the Dakota uncertainty sampling and propagation code. Each code is designed for massively-parallel processing in a high-performance computing (HPC) environment. Multi-physics representations in PFLOTRAN are used to simulate various coupled processes including heat flow, fluid flow, waste dissolution, radionuclide release, radionuclide decay and ingrowth, precipitation and dissolution of secondary phases, and radionuclide transport through engineered barriers and natural geologic barriers to the biosphere. Dakota is used to generate sets of representative realizations and to analyze parameter sensitivity.

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

Dynamic Behavior of Natural Seep Vents: Analysis of Field and Laboratory Observations and Modeling (Final Scientific/Technical Report)

In this project, we have analyzed data collected by the U.S. Department of Energy (DOE), National Energy Technology Laboratory (NETL) in a high pressure water tunnel (HPWT) and data from two research cruises to natural seeps in the Gulf of Mexico to adapt and validate a numerical model to predict the dynamics of natural seeps in the deep oceans. The HPWT data include video observations of the shrinkage rate of individual methane and natural gas bubbles under simulated deep-water conditions. Field data were collected during two cruises by the Gulf Integrated Spill Research (GISR) Consortium led by Texas A&M University and funded by the Gulf of Mexico Research Initiative (GoMRI). These data included in situ observations from a remotely operated vehicle (ROV) of gas bubbles at two natural seep sites in the Gulf and acoustic observations of the natural seep bubble flares in the ocean water column. The acoustic data were from multibeam echosounders, one mounted in a forward-looking orientation on the ROV and another mounted down-looking in the haul of the ship. All of these laboratory and field data were focused on the dynamics of natural gas bubbles at temperatures and pressures favorable for clathrate hydrate formation between the gas and water. Our analyses of this data focused on understanding the mechanisms responsible for gas bubble dissolution within the hydrate stability zone (HSZ) of the oceans. Ice-like hydrate shells may form on the bubble-water interface under these conditions, and it was unknown how this might affect the mass transfer of gas into the ocean. We were able to extract bubble shrinkage rates from the HPWT datasets. Using this data we determined that mass transfer coefficients with and without a hydrate shell match empirical values for bubbles in contaminated systems (so-called dirty bubbles contaminated by naturally occurring surfactants). We also showed that free gas, and not gas hydrate, is the dominant dissolving phase when the hydrate sub-cooling is below 11 degree Celsius (temperature difference between hydrate the hydrate formation temperature and ambient temperator) or the pressure is reducing as bubbles rise through the ocean water column. Using this mass transfer model, our numerical model of bubble dissolution matched the over 200 HPWT experiments with an average error of 10% for predicting the bubble size at the end of an experiment. From field data in the literature, we also observed that gas bubbles dissolve faster when they are initially released, following mass transfer coefficients for so-called clean-bubbles (those not yet contaminated by surfactants). Shortly after release within the HSZ, a hydrate shell forms on the bubble-water interface, and the mass transfer reduces to rates matching those of dirty bubbles. We correlated this transition time from clean to dirty bubble behavior with the initial bubble surface area and the hydrate sub-cooling. With this model for hydrate formation time and using the mass transfer coefficients deduced from the HPWT data, we validated our numerical model for predicting the rise heights of natural seep flares in the oceans. Flare heights are commonly observed in haul-mounted acoustic multibeam data. The numerical model predicts bubbles to rise high in the ocean water column owing to the slower mass transfer rates for dirty bubbles that accompany the majority of their rise time. We found that the numerical model predictions matched the observed flare heights within 5% to 10% accuracy when we compared the rise heights of the largest bubbles released from the seafloor with the bubbles acoustically visible in the multibeam data. Bubbles become acoustically transparent as they shrink to sizes of order 1 mm in diameter for the multibeam frequencies used in the field. The forward-looking multibeam on the ROV also provided data on the lateral spreading of bubbles in natural seep flares. Our analysis of this data showed that spreading follows a diffusion process, with the effective diffusivity correlating with the wobbling length scale of these ellipsoidal bubbles. When we apply this diffusivity in a random displacement model of bubble spreading, our numerical simulations match closely the lateral spread observed by the M3 in the ocean water column. Finally, we compared the seep model predictions for the acoustic properties of these natural seep plumes with that observed by the acoustic instruments in the field. The M3 and EM 302 observations were converted to relative values of target strength using a calibration we obtained in the laboratory for the M3 and using an algorithm from the manufacturer for the EM 302. Comparing the numerical seep model to these data, we obtain good agreement over the whole height of rise of these bubble flares. This further validates the numerical model. Overall, our validated seep model captures the key dynamics of gas bubbles released from natural seeps in the oceans and helps to predict the fate of methane in the water column.

03 NATURAL GAS↗
DOE OSTI2021

Blast furnace slag reactions in various solutions (Interim Report)

Blast furnace slag (BPS) is a critical component of grout formulations for the remediation of low activity nuclear waste. This interim report describes the initial results of a study designed to investigate the fundamental mechanisms of BPS dissolution. The goal of the work is to delineate the physicochemical aspects of the slag that impart beneficial properties to grout formulations to enable the consistent production of a slag-replacement material (“designer slag”) that performs better than what is commercially available. This report documents the dissolution experiments that were conducted using nine different initial solution compositions. Solution measurements for each solution, including pH and solution composition, are given for 1, 7, 14, 28, and 56 day intervals samples. Scanning electron microscopy images are presented for the 56 day samples from each of the solutions. Inferences about reaction mechanisms and 56-day mineralogy are made based on the information collected to date. Some conclusions are made based on the work performed for this interim report, and a path forward including the strategy for making stronger conclusions based on X-ray diffraction (XRD) analyses is presented.

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

Chemical Recycling of Mixed Plastics and Valuable Metals in the Electronic Waste Using Solvent-Based Processing

Annually, 20-55 million tons of electronic waste (e-waste) is produced worldwide (5% of all municipal solid waste). Although e-waste embodies only 2% of America’s municipal waste, it accounts for a significantly larger proportion of the heavy metals and flame retardants present in the waste stream. Currently, less than 20% of all e-waste is recycled in the United States because the heterogeneity of the feedstock limits the opportunity for reuse in high value products and processing of the waste itself is often too costly to justify handling. To address this concern, the aims of this study are: 1) to identify the major plastic and metal compositions within electronic shredder residue (ESR), 2) to formulate solvents and processing conditions to separate 90% of the plastics targeted from consumer shred ESR, and 3) to develop a process design model to estimate the cost and energy efficiency of the proposed solvent-based processing. In this study, a pre-sorted heterogeneous ESR feedstock (one where aluminum, magnetic components, and hazardous battery materials removed by an e-waste recycling facility) was used, with the major compositions of the ESR characterized. It was found that 25 wt.% of the feedstock was composed of plastics, 6 wt.% rubber, 27 wt.% printed circuit boards, 23% wire, and the remainder metals and capacitors. Within the plastic portion, polystyrene (PS, 40 wt.%), acrylonitrile butadiene styrene (ABS, 25 wt.%), and styrene-acrylonitrile (SAN, 9wt.%) were identified to compose the majority of the screened plastics using Fourier transform infrared spectroscopy (FTIR). Next, selective solvents were screened using Hansen Solubility Parameter Theory (HSP) for dissolving PS and ABS. The pre-screening results show that methylene chloride (dichloromethane, DCM) and tetrahydrofuran (THF) are capable of dissolving the most PS and ABS, while methanol (MeOH) and ethylene glycol (EG) are capable of precipitating the most PS and ABS. These solvents were subsequently used to recover polymers and remove. flame retardants within the ESR feedstock. By optimizing the dissolution time and the solvents used, the highest polymer dissolution yield (99 wt.%%) was achieved using DCM for 48 hr. Both pre-screened anti-solvents (MeOH and EG) showed the highest polymer precipitation yield (71 wt.%). In terms of flame retardant removal rate, EG was found to have a high phosphorus-containing flame retardant removal rate (up to 98%). Characterization shows that the proposed solvent-based processing can preserve a high molecular weight fraction of the polymers and effectively remove flame retardants. Cost analysis indicates that the amount of the solvent/anti-solvent recovered after the reaction would play a critical role in reducing the operating costs. The energy analysis shows that the proposed solvent-based processes can save up to 60% of the embodied energy used to manufacture plastics used in electronics (PS and ABS were used for calculations). The results from this project prove the potential of solvent-based processing to produce secondary materials (plastics and metals) from e-waste for cross-industry reuse.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2021

Effects of Carbonate Minerals on Shale-Hydraulic Fracturing Fluid Interactions in the Marcellus Shale

Natural gas extracted from tight shale formations, such as the Marcellus Shale, represents a significant and developing front in energy exploration. By fracturing these formations using pressurized fracturing fluid, previously unobtainable hydrocarbon reserves may be tapped. While pursuing this resource, hydraulic fracturing operations leave chemically complex fluids in the shale formation for at least two weeks. This provides a substantial opportunity for the hydraulic fracturing fluid (HFF) to react with the shale formation at reservoir temperature and pressure. In this study, we investigated the effects of the carbonates on shale-HFF reactions with a focus on the Marcellus Shale. We performed autoclave experiments at high temperature and pressure reservoir conditions using a carbonate-rich and a decarbonated or carbonate-free version of the same shale sample. We observed that carbonate minerals buffer the pH of the solution, which in turn prevents clay dissolution. Carbonate and bicarbonate ions also scavenge reactive oxidizing species (ROS), which prevents oxidation of shale organic matter and volatile organic compounds (VOCs). Carbonate-free samples also show higher pyrite dissolution compared to the carbonate-rich sample due to chelation reactions. This study demonstrates how carbonate minerals (keeping all other variables constant) affect shale-HFF reactions that can potentially impact porosity, microfracture integrity, and the release of heavy metals and volatile organic contaminants in the produced water.

58 GEOSCIENCES↗
DOE OSTI2013

Capability to Recover Plutonium-238 in H-Canyon/HB-Line - 13248

Plutonium-238 is used in Radioisotope Thermoelectric Generators (RTGs) to generate electrical power and in Radioisotope Heater Units (RHUs) to produce heat for electronics and environmental control for deep space missions. The domestic supply of Pu-238 consists of scrap material from previous mission production or material purchased from Russia. Currently, the United States has no significant production scale operational capability to produce and separate new Pu-238 from irradiated neptunium-237 targets. The Department of Energy - Nuclear Energy is currently evaluating and developing plans to reconstitute the United States capability to produce Pu-238 from irradiated Np-237 targets. The Savannah River Site had previously produced and/or processed all the Pu-238 utilized in Radioisotope Thermoelectric Generators (RTGs) for deep space missions up to and including the majority of the plutonium for the Cassini Mission. The previous full production cycle capabilities included: Np- 237 target fabrication, target irradiation, target dissolution and Np-237 and Pu-238 separation and purification, conversion of Np-237 and Pu-238 to oxide, scrap recovery, and Pu-238 encapsulation. The capability and equipment still exist and could be revitalized or put back into service to recover and purify Pu-238/Np-237 or broken General Purpose Heat Source (GPHS) pellets utilizing existing process equipment in HB-Line Scrap Recovery, and H-Canyon Frame Waste Recovery processes. The conversion of Np-237 and Pu-238 to oxide can be performed in the existing HB-Line Phase-2 and Phase- 3 Processes. Dissolution of irradiated Np-237 target material, and separation and purification of Np-237 and Pu-238 product streams would be possible at production rates of ∼2 kg/month of Pu-238 if the existing H-Canyon Frames Process spare equipment were re-installed. Previously, the primary H-Canyon Frames equipment was removed to be replaced: however, the replacement project was stopped. The spare equipment is stored and still available for installation. Out of specification Pu-238 scrap material can be purified and recovered by utilizing the HB-Line Phase- 1 Scrap Recovery Line and the Phase-3 Pu-238 Oxide Conversion Line along with H-Canyon Frame Waste Recovery process. In addition, it also covers and describes utilizing the Phase-2 Np-237 Oxide Conversion Line, in conjunction with the H-Canyon Frames Process to restore the H-Canyon capability to process and recover Np-237 and Pu-238 from irradiated Np-237 targets and address potential synergies with other programs like recovery of Pu-244 and heavy isotopes of curium from other target material. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

Reprocessing system with nuclide separation based on chromatography in hydrochloric acid solution

We have proposed the reprocessing system with nuclide separation processes based on the chromatographic technique in the hydrochloric acid solution system. Our proposed system consists of the dissolution process, the reprocessing process, the minor actinide separation process, and nuclide separation processes. In the reprocessing and separation processes, the pyridine resin is used as a main separation media. It was confirmed that the dissolution in the hydrochloric acid solution is easily achieved by the plasma voloxidation and by the addition of oxygen peroxide into the hydrochloric acid solution.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Scaling gas-phase treatment of vadose-zone contaminants for field application at the Hanford site - 15133

In situ vadose zone remediation approaches are being evaluated as potential options to mitigate the transport of inorganic and radionuclide contaminants from the vadose zone to the groundwater at the U.S. Department of Energy's Hanford site. Some of the candidate approaches are based on changing the contaminant or subsurface conditions in a way that slows downward migration of the contaminants through the vadose zone using amendments delivered in the gas-phase. Ammonia-vapor treatment of uranium relies on induced sediment dissolution and precipitation processes that decrease the amount of mobile uranium in the vadose zone. Previous laboratory studies have demonstrated the decrease in uranium mobility caused by ammonia treatment. As part of development efforts for the ammonia technology, scale-up issues were identified and have been addressed through a series of laboratory and modeling efforts. Key scale-up elements are scoping calculations to support treatment design and understanding ammonia transport. Recent research has extended the concept of geochemical manipulation by ammonia to investigate a combined-gas treatment for sequestering Tc-99 in the vadose zone. The technique uses a combination of geochemical Tc-99 reduction with hydrogen sulfide gas and induced sediment mineral dissolution and precipitation with ammonia vapor, creating conditions for deposition of stable precipitates that decrease the mobility of Tc-99. Laboratory experiments have demonstrated the effectiveness of this treatment under a variety of operational and sediment conditions important to the scale-up and evaluation of potential addition field applications. (authors)

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

ITEAM - An international mechanistic approach to modeling glass behavior over geologic time scales - 15527

Vitrification is a common worldwide solution for radioactive waste immobilization. Although the excellent chemical durability of glass has been demonstrated in ancient man-made and natural analogues, the lack of an international consensus on a glass corrosion rate law limits the application of glass in high-level waste repository performance models. The contributions of physical and chemical processes controlling the long-term glass dissolution rate in geologic disposal remain uncertain resulting in this non-consensus. A thorough mechanistic understanding of waste form durability in geologic environments would improve public and regulator confidence. In addition, this understanding could lead to cost savings if it becomes possible to take credit for the true durability of the waste form itself in system evaluations rather than requiring expensive engineered barrier systems. To this end, five nations (US, UK, France, Japan, and Belgium) have joined together to formulate a joint plan for collaborative research into the mechanisms controlling the long-term corrosion of glass. Over the last five years, the coordinated research performed by these countries has produced a new level of understanding about the glass corrosion mechanisms, specifically as they apply to glasses similar in composition to the French R7T7 glass. Some recent results are presented as they relate to several mechanisms that are thought to control glass alteration at long time periods. It is important to understand the effects of each particular mechanism on the overall radionuclide release and the relative importance of each process model to the performance assessment calculation. In addition, a new series of experiments calls out potential sources of error due to the use of irregular shapes (such as crushed glass powder) in dissolution experiments. (authors)

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

Advanced Waste Management Concepts for Uranium and Plutonium Multi-Recycling - 18533

The multiple recycling of plutonium and uranium will play a major role in gradually achieving a fully closed nuclear fuel cycle in the future, once the first Generation IV fast reactors (FR) are deployed in the NPP fleet. To reach this objective, optimizations of current processes and technologies and, in some cases, the development of innovative concepts are required to meet the scientific, technical and economic challenges imposed by the treatment of spent fuels with an increasingly higher Pu content. Based on the significant past experience acquired by France in LWR and FR MOX fuel treatment, the CEA is running R and D studies to develop new efficient processes for Pu recycling and for FR MOX fuel fabrication. More compact and economically competitive processes, ensuring the safety/security of the facilities (particularly as regards criticality and proliferation resistance) have to be developed taking into account that the amounts of plutonium involved will be one order of magnitude higher than in UOX fuels. New concepts of head-end treatment, dissolution, and separation have been proposed. Consequently, effluent and waste management must be adapted to these processes and to the characteristics of fast reactor MOX fuels. New waste treatment processes are suggested: 1) Cladding waste and undissolved metallic particles could be treated simultaneously in a melting process. The molten metal could be decontaminated by a specific slag and the oxides recovered, in particular PuO{sub 2}, would be recycled at the frond-end of the process, 2) Fission Products and Actinides (FPA) containment glass will also be optimized to accommodate significant amounts of iron, nickel and chromium coming from hull corrosion, and / or decontamination slag coming from the metal melting process. 3) New peraluminous-type glass formulations are under development to accept increased amounts of FPA, as well as iron, nickel, and chromium. The first trials to evaluate the melting process have indicated that metallic compounds from the dissolution residues could be easily incorporated into a molten metal at levels of 1, 2 and 3 w%. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗