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At least 577 records · Page 32

Thermo-rheological snapshot of melter feed conversion to glass

Slurry feed charged into an electric melter creates a layer of reacting and melting material (termed cold cap) that floats on the surface of molten glass. The rheological behavior of heated melter feed affects the spreading of slurry at the top of the cold cap and the stability of the primary foam, affecting cold-cap coverage and melter plenum temperatures. The apparent viscosity of a high-alumina high-level waste melter feed was assessed by thermomechanical analysis, high-temperature viscometer, and the hot stage microscopy method, yielding viscosity estimates from ≈10 7.5 Pa s at 550°C to ≈10 2.5 Pa s at 1050°C. As the temperature of feed materials increased, their state changed from rigid solid to dilatant fluid, to pseudoplastic bubbly liquid with dissolving solids, to fully developed foam, and finally to Newtonian glass melt.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Integrated low-temperature PVC and polyolefin upgrading

Polyolefins and their chlorinated derivatives such as polyvinyl chloride (PVC) are among the most prevalent plastics in global production and waste streams. Traditional waste-to-energy methods such as incineration and pyrolysis, as well as most chemical upcycling methods for PVC utilization, require thorough, high-temperature dechlorination to prevent the release of toxic chlorinated compounds. Here, we present here a strategy for upgrading discarded PVC into chlorine-free fuel range hydrocarbons and hydrogen chloride in a single-stage process catalyzed by chloroaluminate ionic liquids. This approach offsets endothermic dechlorination and carbon-carbon bond cleavage with exothermic alkylation and hydrogen transfer by isobutane or isopentane in a low-temperature tandem process. The light isoalkanes are available from refinery processes and partly from recycling of the product stream. This process is suitable for handling real-world mixed and contaminated PVC and polyolefin waste streams.

Zhang, Wei [East China Normal Univ. (ECNU), Shangh↗

Path Toward a Breeding, Proliferation-Resistant, Thermal-Spectrum Molten Salt Reactor

Liquid-fueled, thermal-spectrum molten salt breeder reactors (TS-MSBRs) offer the potential for affordable, safe, inexhaustible energy with minimal potential for nuclear material misuse and without significant actinide waste generation. Realizing the full set of TS-MSBR capabilities is only now becoming possible with the advent of advanced fuel-salt processing techniques, improved materials, and a more detailed understanding of fuel-salt properties. Additionally, modern higher-fidelity modeling and simulation methods enable a more detailed evaluation of TS-MSBR design options. TS-MSBRs, however, remain immature and will require substantial, sustained development resources.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Disposal of hypergolic propellants, phase 6 task 4. Disposal pond products

Waste monomethyl hydrazine scrubber liquor, consisting of aqueous solutions containing small amounts of CH4, Cl2, CH3Cl, CH2Cl2, and CHCl3 as well as large amounts of CH3OH is scheduled to be dumped in stabilization ponds along with nitrate and nitrite salt solutions obtained as waste liquors from the N2O4 scrubbers. The wastes are investigated as to the hazardous materials generated by such combinations of items as described as well as the finite lifetime of such materials in the stabilization ponds. The gas liquid chromatograph was used in the investigation. A series of experiments designed to convert nitrate and nitrite salts to the environmentally innocuous N2O and N2 using solar energy is reported. Results indicate that this solar conversion is feasible.

Cohenour, B. C.↗

Superconductivity out of a non-Fermi liquid: Free energy analysis

In this paper, we present an in-depth analysis of the condensation energy E c for a superconductor in a situation when superconductivity emerges out of a non-Fermi liquid due to pairing mediated by a massless boson. This is the case for electronic-mediated pairing near a quantum-critical point in metal, for pairing in SYK-type models, and for phonon-mediated pairing in the properly defined limit, when the dressed Debye frequency vanishes. We consider a subset of these quantum-critical models, in which the pairing in a channel with a proper spatial symmetry is described by an effective 0 + 1 dimensional model with the effective dynamical interaction V(Ω m ) = g¯ γ /|Ω m | γ , where γ is model-specific (the γ model). In previous papers, we argued that the pairing in the γ model is qualitatively different from that in a Fermi liquid, and the gap equation at T = 0 has an infinite number of topologically distinct solutions, Δ n (ω m ), where an integer n, running between 0 and infinity, is the number of zeros of Δ n (ω m ) on the positive Matsubara axis. This gives rise to the set of extrema of E c at E c,n , of which E c,0 is the global minimum. Here, the spectrum E c,n is discrete for a generic γ < 2 but becomes continuous at γ = 2–0. Here, we discuss in more detail the profile of the condensation energy near each E c,n and the transformation from a discrete to a continuous spectrum at γ → 2. We also discuss the free energy and the specific heat of the γ model in the normal state.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nuclear Safety [Vol. 33, No. 4, October-December 1992]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 499 Technical Note: Nuclear Regulatory Commission’s Examination Question Bank System, C. L Jensen and N. L. Skinner; 506 Report on the Specialists’ Meeting on Passive and Active Safety Features of Liquid-Metal Fast Breeder Reactors Organized by the International Atomic Energy Agency at Oarai Engineering Centre of Power Reactor and Nuclear Development Corporation, Japan, November 5-7,1991, S. R. Paranjpe; ACCIDENT ANALYSIS: 514 A Review of Hydrogen Production During Melt/Water Interaction in LWRs, D. F. Fletcher, B. D. Turland, and S. P. A. Lawrence; 535 A Review of the U 3 0 8 -Al Reaction as a Potential Heat Source in Research and Test Reactor Accidents, J. L. Snelgrove; CONTROL AND INSTRUMENTATION: 543 Multilevel Interfaces for Power Plant Control Rooms II: A Preliminary Design Space, K. J. Vicente; DESIGN FEATURES: 549 Twenty-Second DOE/NRC Nuclear Air Cleaning and Treatment Conference, R. R. Bellamy, D. W. Moeller, and M. W. First; 562 Book Review: Safety Assessment of Unit 5 (WWER-440/W-213) of the Greifswald Nuclear Power Station, M. H. Fontana; WASTE AND SPENT FUEL MANAGEMENT: 576 Activities Related to Waste and Spent Fuel Management, M. D. Muhlheim and E. G. Silver; OPERATING EXPERIENCES: 586 Analysis of Corrective Actions Applied to Nuclear Power Plant Operations, A. E. Cross; 593 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 596 Operating U.S. Power Reactors, Compiled by M. D. Muhlheim and E. G. Silver; 609 Non-Commercial Power Operating Experience; 614 World Nuclear Performance, Compiled by M. D. Muhlheim; RECENT DEVELOPMENTS: 623 General Administrative Activities, Compiled by M. D. Muhlheim and E. G. Silver; 635 Reports, Standards, and Safety Guides, D. S. Queener; 639 Proposed Rule Changes as of June 30, 1992; ANNOUNCEMENTS: 513 Fourth International Conference on Nuclear Fuel Reprocessing and Waste Management RECOD '94; 585 International Topical Meeting on Advanced Reactors Safety; 622 International Workshop on Implementation of ALARA at Nuclear Power Plants; 648 Short Course on Nuclear Criticality Safety; 648 8th Topical Meeting on Problems in Reactor Physics MEPhi-VOLGA-93; 643 The Authors; 646 Reviewers of Nuclear Safety, Vol. 33

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Phenomenological Model of Nonlinear Dynamics and Deterministic Chaotic Gas Migration in Bentonite: Experimental Evidence and Diagnostic Parameters

Understanding gas migration in compacted clay materials, e.g., bentonite and claystone, is important for the design and performance assessment of an engineered barrier system of a radioactive waste repository system, as well as many practical applications. Existing field and laboratory data on gas migration processes in low-permeability clay materials demonstrate the complexity of flow and transport processes, including various types of instabilities, caused by nonlinear dynamics of coupled processes of liquid–gas exchange, dilation, fracturing, fracture healing, etc., which cannot be described by classical models of fluid dynamics in porous media. We here show that the complexity of gas migration processes can be explained using a phenomenological concept of nonlinear dynamics and deterministic chaos theory. To do so, we analyzed gas pressure and gas influx (i.e., input) and outflux (i.e., output), recorded during the gas injection experiment in the compact Mx80-D bentonite sample, and calculated a set of the diagnostic parameters of nonlinear dynamics and chaos, such a global embedding dimension, a correlation dimension, an information dimension, and a spectrum of Lyapunov exponents, as well as plotted 2D and 3D pseudo-phase-space strange attractors, based on the univariate influx and outflux time series data. These results indicate the presence of phenomena of low-dimensional deterministic chaotic behavior of gas migration in bentonite. In particular, during the onset of gas influx in the bentonite core, before the breakthrough, the development of gas flow pathways is characterized by the process of chaotic gas diffusion. After the breakthrough, with inlet-to-outlet movement of gas, the prevailing process is chaotic advection. During the final phase of the experiment, with no influx to the sample, the relaxation pattern of gas outflux is resumed back to a process of chaotic diffusion. The types of data analysis and a proposed phenomenological model can be used to establish the basic principles of experimental data-gathering, modeling predictions, and a research design.

36 MATERIALS SCIENCE↗

Selective permeation up a chemical potential gradient to enable an unusual solvent purification modality

The need for energy-efficient recovery of organic solutes from aqueous streams is becoming more urgent as chemical manufacturing transitions toward nonconventional and bio-based feedstocks and processes. In addition to this, many aqueous waste streams contain recalcitrant organic contaminants, such as pharmaceuticals, industrial solvents, and personal care products, that must be removed prior to reuse. We observe that rigid carbon membrane materials can remove and concentrate organic contaminants via an unusual liquid-phase membrane permeation modality. Surprisingly, detailed thermodynamic calculations on the chemical potential of the organic contaminant reveal that the organic species has a higher chemical potential on the permeate side of the membrane than on the feed side of the membrane. This unusual observation challenges conventional membrane transport theory that posits that all permeating species move from high chemical potential states to lower chemical potential states. Based on experimental measurements, we hypothesize that the organic is concentrated in the membrane relative to water via favorable binding interactions between the organic and the carbon membrane. The concentrated organic is then swept through the membrane via the bulk flow of water in a modality known as “sorp-vection.” We highlight via simplified nonequilibrium thermodynamic models that this “uphill” chemical potential permeation of the organic does not result in second-law violations and can be deduced via measurements of the organic and water sorption and diffusion rates into the carbon membrane. Moreover, this work identifies the need to consider such nonidealities when incorporating unique, rigid materials for the separations of aqueous waste streams.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

129 I and 99 Tc Distribution Coefficients of Subsurface Sediments Collected from the Proposed Site of the Environmental Manage Disposal Facility

Performance Assessment calculations are presently underway to evaluate the Environmental Management Disposal Facility (EMDF), a proposed new low-level radioactive waste (LLW) disposal facility on the U.S. Department of Energy’s Oak Ridge Reservation (ORR). Among the large number of input parameters needed for such calculations, are distribution coefficients (K d values; radionuclide concentration solid:liquid ratio) that provide a measure of the tendency of radionuclides to bind to sediments. The objective of this study was to measure K d values of two radionuclides that may pose a disproportionately large amount of risk, 129 I and 99 Tc. The average I K d value for the 10 geological materials recovered from the proposed EMDF site was 52.3 mL/g and ranged from 2.7 to 140.9 mL/g. These values were consistent, but somewhat larger than previous measurements made with ORR sediments and were about an order of magnitude greater than those used in previous EMDF PA calculations. The median Tc K d value was 807.2 mL/g, much greater than previously reported using ORR geological materials. Five of the ten tested geological materials sorbed large quantities of Tc, suggesting that the weakly sorbing Tc(VII) species had been reduced to the very strongly binding and sparingly soluble Tc(IV) species. The five strongly sorbing sediment had apparent solubility values of approximately <10 -8 mol/L. Based on sediment properties and general ORR geological considerations, it was proposed that much of the I and Tc sorption could be attributed to the low pH (average pH = 4.94), low redox status, and/or the elevated levels of iron oxides, manganese oxides, and natural organic matter. An implication of this study is that the areas of the EMDF subsurface environment may have natural properties for attenuating I and Tc movement, thereby potentially reducing risk posed by burial of LLW at this site.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Modeling of multi-component precipitation and crystallization for zero-liquid-discharge desalination

This study proposes novel ZLD treatment trains that integrate multi-component chemical precipitation and multi-effect evaporative crystallization for efficient brine management. The methodology emphasizes sustainability by integrating CO₂ for chemical precipitation and reducing environmental impact, exemplified with two case studies: produced water that includes industrial waste heat utilization by adopting the emerging vacuum air-gapped membrane distillation (VAGMD) technology, and brackish groundwater that is abundant in sulphate which undergoes treatment by low-salt-rejection reverse osmosis (LSRRO) with interstage chemical precipitation. Here, this study is the first of its kind to simultaneously account for reducing risk of mineral scaling and effective recovery of valuable solids when incorporating VAGMD and LSRRO in ZLD treatment trains. Using Reaktoro and WaterTAP, both Python-based, open-source platforms, we model the recovery of high-purity magnesium, calcium, and sodium salts while optimizing energy consumption and operational efficiency in proposed ZLD pathways for case studies of produced water and brackish desalination brine management. Validation with experimental and reference data confirms the reliability of the models used. In both case studies, the optimized ZLD process achieves recovery rates of 97%, 99%, and 90% for Mg, Ca, and Na, with purities exceeding 99%, and brine volume reduced to less than 4% of the initial feed flow.

3D CT scans↗

Heat pipe radiator

A 15,000 watt spacecraft waste heat rejection system utilizing heat pipe radiator panels was investigated. Of the several concepts initially identified, a series system was selected for more in-depth analysis. As a demonstration of system feasibility, a nominal 500 watt radiator panel was designed, built and tested. The panel, which is a module of the 15,000 watt system, consists of a variable conductance heat pipe (VCHP) header, and six isothermalizer heat pipes attached to a radiating fin. The thermal load to the VCHP is supplied by a Freon-21 liquid loop via an integral heat exchanger. Descriptions of the results of the system studies and details of the radiator design are included along with the test results for both the heat pipe components and the assembled radiator panel. These results support the feasibility of using heat pipes in a spacecraft waste heat rejection system.

Swerdling, B.↗

Microgravity Experiments of Solid Waste Conversion into Useful Commodities

This Summer I participated in two projects at Kennedy Space Center in Cape Canaveral, Florida. The projects focus on the NASA's Deep Space Gateway applications for future Mars travel. All of these projects use recycling technology to use resources found on Earth and on other planets for fuel and other environmental applications. The first project I took the lead on is “Plasma Arc Gasification.” Plasma is a high temperature and very efficient way to process waste to create usable byproducts. The plasma chamber in temperature is comparable to that of the sun and this energy will help create an environment in which the waste can be recycled properly for not only plant support, but also for possible fuel application as well. I preformed the tests in a quartz tube, which is used to hold the waste (cotton, plastics, nylon, paper and a human waste simulant) and the waste is then combusted using O2 (present in air) into gases such as H2, H2O, CH4 and CO2. I determined which gases are present using a Fourier-transform infrared spectroscopy (FTIR) machine, which analyzes the peaks of the gases using liquid nitrogen. Problems arose in the beginning from the reactor emitting electromagnetic waves (EMI) that interfered with the technology of the experiment, specifically the thermocouples. This was solved through multiple tests with the positioning of the thermocouple power supply further away from the plasma reactor. I worked with another intern, Daniel Santander, who developed a space plant chamber which uses CO2 and H2O (harvested from the plasma reactor) to grow plants in space. The chamber possess a CO2 monitor, which controls the amount of gas that enters the chamber, along with a water integration system to supply the amount of water needed for proper plan growth. This technology will then be used for plant growth in space for the Astronauts on future space flights and possibly on the International Space Station (ISS). The second project I worked on is the “Orbital Syngas / Commodity Augmentation Reactor (OSCAR)” which focuses on the issues experienced in long-duration space flight regarding waste disposal. In previous space flight missions, waste was stored on board and returned to Earth for disposal. This technique is not applicable to long space flight missions to Mars due to the rocket being months away from Earth. OSCAR is using microgravity waste disposal techniques to produce fuels from the recycled waste. The waste is converted to syngas through a thermal degradation process. This process helps create an environmentally friendly way to dispose and reuse trash on board the space craft. Currently waste is being tested in the form of cotton and plastics. OSCAR is designed as a microgravity reactor that is currently being tested in a drop tower rig at Glenn Research Center. I helped design the 3D model for the insulation that will line the reactor. The first few trials, I dissolved the plastic of the mold in acetone. This method worked, but was very costly. I then received a silicone material to construct the mold from Swamp Works here at Kennedy. Through multiple trials with the silicone, this method worked best for developing the end pieces of the insulation for the chamber.

Plasma↗

GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} for Fukushima Daiichi Water Treatment Secondary Wastes - 20212

The Japanese government is supporting development work implemented jointly by Veolia subsidiaries Kurion Japan, K.K., Veolia Nuclear Solutions (VNS), Inc., and Veolia Nuclear Solutions Federal Services, LLC for treating radioactive waste generated from Fukushima Daiichi Nuclear Power Station (NPS) water treatment using the GeoMelt{sup TM} In-Container Vitrification (ICV){sup TM} technology. The initial work consisted of glass formulation and engineering-scale testing which was completed in 2018, in the frame of an IRID (International Research Institute for Nuclear Decommissioning) program as part of a project subsidized by Japan's Ministry of Economy, Trade and Industry (METI). The Fukushima Daiichi NPS Mid- and Long-Term Road-map requires investigation of methods to stabilize solid wastes (and to immobilize radioisotopes in the wastes) generated as a result of emergency response and decommissioning activities. Cooling water treatment has resulted in a significant amount of solid and slurry secondary wastes (mostly adsorbents and ion-exchange materials) which will require processing at some point. GeoMelt{sup R} ICV{sup TM} is a joule-heated melter technology which uses a refractory-lined single-use container combining the melter and disposal container. There is no pouring required nor concerns with refractory corrosion which allows the process to accommodate a wide range of waste chemistries and high waste loadings. The testing described here consisted of three engineering-scale melts, each processing between 212 kg and 240 kg of waste simulants, glass formers, and non-radioactive cesium (Cs) and strontium (Sr) tracers. Continuous isokinetic stack sampling of off-gas emissions was performed for each test in order to calculate Cs and Sr retention in the glass wasteform. Single-pass retention of Cs in the final glass wasteform ranged from 91.46 to 99.30%, and single-pass retention of Sr ranged from 99.76 to 100%. Planned particulate recycle will increase these retention levels. Melt 1 processed a mixture of KUR-EH (a zeolite-based ion-exchange material), simulated Advanced Liquid Processing System (ALPS) Carbonate and Iron Slurries, and glass additives. Melt 2 processed a mixture of KUR-EH, KUR-TSG (a titanate-based adsorbent), and glass additives. Melt 3 processed a mixture of KUR-EH, simulated barium sulfate/iron ferrocyanide sludge (AREVA sludge), and glass additives. Waste loadings for these melts ranged from 70 weight percent (wt%) to 82 wt%. Vitrification produces a waste form much denser than the stored water treatment secondary waste wastes, resulting in significant volume reduction. Volume reductions for the three tests ranged from 74 to 79 vol%. Vitrification produces a chemically durable wasteform. Pacific Northwest National Laboratory (PNNL) tested three glass samples from each engineering-scale melt) by the Materials Characterization Center 1 (MCC-1) test, an international standard leach test of the chemical durability of nuclear waste glasses. PNNL also obtained one U.S. reference glass (EA Glass) and two Japan reference glasses P0798) and tested these under the same MCC-1 conditions (90 deg. C, 10 m-1, DIW, and 7, 14, 28-day) as the GeoMelt{sup R} ICV{sup TM} glasses. The GeoMelt{sup R} ICV{sup TM} glasses exhibited lower total normalized releases and 14- to 28-day normalized release rates than the three reference glasses. These results suggest that the GeoMelt{sup R} ICV{sup TM} glasses have durabilities on par with high-level waste glasses under standard test conditions. Post-melt process sampling and analysis indicated no Cs migration into the melter refractory materials and very little deposition of Cs or Sr onto the melter hood or off-gas piping internals. The results of the testing indicated good Cs retention in the glass, high volume reduction and waste loadings, and excellent chemical durability. These factors are important to minimize treatment costs and to protect workers and the environment. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Possible impacts of molten salt reactors on the International Monitoring System

Molten salt reactors (MSRs) are gaining support as many countries look for ways to increase power generation and replace aging nuclear energy production facilities. MSRs have inherently safe designs, are scalable in size, can burn transuranic wastes from traditional solid fuel nuclear reactors, can store excess heat in thermal reservoirs for water desalination, and can be used to produce medical isotopes as part of the real-time liquid-fuel recycling process. The ability to remove 135 Xe in real time from the fuel improves the power production in an MSR because 135 Xe is the most significant neutron-absorbing isotope generated by nuclear fission. Xenon-135, and other radioactive gases, are removed by sparging the fuel with an inert gas while the liquid fuel is recirculated from the reactor inner core through the heat exchangers. Without effective abatement technologies, large amounts of radioactive gas could be released during the sparging process. This work examines the potential impact of radioxenon releases on samplers used by the International Monitoring System (IMS) to detect nuclear explosions. Here, atmospheric transport simulations from seven hypothetical MSRs on different continents were used to evaluate the holdup time needed before release of radioxenon so IMS samplers would register few detections. Abatement technologies that retain radioxenon isotopes for at least 120 d before their release will be needed to mitigate the impacts from a molten salt breeder reactor used to replace a nuclear power plant. A holdup time of about 150 d is needed to reduce emissions to the average level of current nuclear power plants.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

A lunar transportation system

Due to large amounts of oxygen required for space travel, a method of mining, transporting, and storing this oxygen in space would facilitate further space exploration. The following project deals specifically with the methods for transporting liquid oxygen from the lunar surface to the Lunar Orbit (LO) space station, and then to the Lower Earth Orbit (LEO) space station. Two vehicles were designed for operation between the LEO and LO space stations. The first of these vehicles is an aerobraked design vehicle. The Aerobrake Orbital Transfer Vehicle (OTV) is capable of transporting 5000 lbm of payload to LO while returning to LEO with 60,000 lbm of liquid oxygen, and thus meet mission requirements. The second vehicle can deliver 18,000 lbm of payload to LO and is capable of bringing 60,000 lbm of liquid oxygen back to LEO. A lunar landing vehicle was also designed for operation between LO and the established moon base. The use of an electromagnetic railgun as a method for launching the lunar lander was also investigated. The feasibility of the railgun is doubtful at this time. A system of spheres was also designed for proper storing and transporting of the liquid oxygen. The system assumes a safe means for transferring the liquid oxygen from tank to tank is operational. A sophisticated life support system was developed for both the OTV and the lunar lander. This system focuses on such factors as the vehicle environment, waste management, water requirements, food requirements, and oxygen requirements.

Source record↗

Improved Regenerative Sorbent-Compressor Refrigerator

Conceptual regenerative sorbent-compressor refrigerator attains regeneration efficiency and, therefore, overall power efficiency and performance greater than conventional refrigerators. Includes two fluid loops. In one, CH2FCF3 (R134a) ciculates by physical adsorption and desorption in four activated-charcoal sorption compressors. In other, liquid or gas coolant circulated by pump. Wave of regenerative heating and cooling propagates cyclically like peristatic wave among sorption compressors and associated heat exchangers. Powered by electricity, oil, gas, solar heat, or waste heat. Used as air conditioners, refrigerators, and heat pumps in industrial, home, and automotive applications.

Jones, Jack A.↗

129 I, 99 Tc, And U Distribution Coefficients of Subsurface Sediments Collected from the Proposed Site of the Environmental Management Disposal Facility

Performance Assessment calculations were completed in 2020 to evaluate the Environmental Management Disposal Facility (EMDF), a proposed new low-level radioactive waste (LLW) disposal facility on the U.S. Department of Energy’s Oak Ridge Reservation (ORR). Among the large number of input parameters needed for such calculations, are distribution coefficients (K d values; radionuclide concentration solid:liquid ratio) that provide a measure of the tendency of radionuclides to bind to sediments. The objective of this study was to measure K d values of three radionuclides that may pose a disproportionately large amount of risk, U, 129 I and 99 Tc. The average I K d value for the 14 geological materials recovered from the proposed EMDF site was 37.8 mL/g and ranged from -1.8 to 140.9 mL/g. These values were consistent, but somewhat larger than previous measurements made with ORR sediments and were about an order of magnitude greater than those used in previous EMDF PA calculations. The median Tc K d value was 365.7 mL/g, much greater than previously reported using ORR geological materials. Five of the 14 tested geological materials sorbed large quantities of Tc, suggesting that the weakly sorbing Tc(VII) species had been reduced to the sparingly soluble Tc(IV) species. The five strongly sorbing sediments had apparent Tc solubility values of approximately <10 -8 mol/L. The median U K d value was 5,726 mL/g. All of the tested geological materials had large K d values, ranging from 625 to >10,208 mL/g. Among the sediment samples that exhibited strong U binding, the apparent solubility value was approximately <10 -9 mol/L. Based on sediment properties and general ORR geological considerations, it was proposed that much of the I and Tc retention could be attributed to the site materials exhibiting low pH (average pH = 4.94), low redox status, and/or the elevated levels of iron oxides, manganese oxides, and natural organic matter. Similarly, the extremely high U binding measured in these sediments may also be attributed to the low conditions of carbonates, which can complex and therefore solubilize uranyl in these tests due to the low pH, and also the relatively high concentrations of iron and organic coatings on these samples. An implication of this study is that the areas of the EMDF subsurface environment may have natural properties for attenuating I, Tc, and U movement, and potentially other radionuclides, thereby possibly reducing risk posed by burial of LLW at this site. This document is a revision of SRNL-STI-2021-00404, Revision 0 that includes new data describing U K d values and new I and Tc K d values for four Nolichucky sediments. These new results were integrated into the data presented in the original document.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

129 I, 99 Tc, and U Distribution Coefficients of Subsurface Sediments Collected from the Proposed Site of the Environmental Management Disposal Facility

Performance Assessment calculations were completed in 2020 to evaluate the Environmental Management Disposal Facility (EMDF), a proposed new low-level radioactive waste (LLW) disposal facility on the U.S. Department of Energy’s Oak Ridge Reservation (ORR). Among the large number of input parameters needed for such calculations, are distribution coefficients (K d values; radionuclide concentration solid: liquid ratio) that provide a measure of the tendency of radionuclides to bind to sediments. The objective of this study was to measure K d values of three radionuclides that may pose a disproportionately large amount of risk, U, iodine-129 ( 129 I) and technetium-99 ( 99 Tc). The average 129 I K d value for the 14 geological materials recovered from the proposed EMDF site was 37.8 mL/g and ranged from 0.45 to 140.9 mL/g. These values were consistent, but somewhat larger than previous measurements made with ORR sediments and were about an order of magnitude greater than those used in previous EMDF PA calculations. The median 99 Tc K d value was 365.7 mL/g, much greater than previously reported using ORR geological materials. Five of the 14 tested geological materials sorbed large quantities of 99 Tc, suggesting that the weakly sorbing 99 Tc(VII) species had been reduced to the sparingly soluble 99 Tc(IV) species. The five strongly sorbing sediments had apparent 99 Tc solubility values of approximately <10 -8 mol/L. The median U K d value was 5,726 mL/g. All of the tested geological materials had large K d values, ranging from 625 to >10,208 mL/g. Among the sediment samples that exhibited strong U binding, the apparent solubility value was approximately <10 -9 mol/L. Based on sediment properties and general ORR geological considerations, it was proposed that much of the 129 I and 99 Tc retention could be attributed to the site materials exhibiting low pH (average pH = 4.94), and/or the elevated levels of iron oxides, manganese oxides, and natural organic matter. Similarly, the extremely high U binding measured in these sediments may also be attributed to the low conditions of carbonates, which can complex and therefore solubilize uranyl in these tests due to the low pH, and also the relatively high concentrations of iron and organic coatings on these samples. An implication of this study is that the areas of the EMDF subsurface environment may have natural properties for attenuating 129 I, 99 Tc, and U movement, and potentially other radionuclides, thereby possibly reducing risk posed by burial of LLW at this site.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗