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At least 37 records · Page 2

Treatment of Radioactive Metallic Waste from Operation of Nuclear Power Plants by Melting - The German Way for a Consistent Recycling to Minimize the Quantity of Radioactive Waste from Operation and Dismantling for Disposal - 12016

During maintenance of nuclear power plants, and during their decommissioning period, a large quantity of radioactive metallic waste will accrue. On the other hand the capacity for final disposal of radioactive waste in Germany is limited as well as that in the US. That is why all procedures related to this topic should be handled with a maximum of efficiency. The German model of consistent recycling of the radioactive metal scrap within the nuclear industry therefore also offers high capabilities for facilities in the US. The paper gives a compact overview of the impressive results of melting treatment, the current potential and further developments. Thousands of cubic metres of final disposal capacity have been saved. The highest level of efficiency and safety by combining general surface decontamination by blasting and nuclide specific decontamination by melting associated with the typical effects of homogenization. An established process - nationally and internationally recognized. Excellent connection between economy and ecology. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The use of aluminum nitride to improve Aluminum-26 Accelerator Mass Spectrometry measurements and production of Radioactive Ion Beams

We present results and discuss the use of aluminum nitride as a promising source material for Accelerator Mass Spectrometry (AMS) and Radioactive Ion Beams (RIBs) science applications of 26 Al isotopes. The measurement of 26 Al in geological samples by AMS is typically conducted on Al 2 O 3 targets. However, Al 2 O 3 is not an ideal source material because it does not form a prolific beam of Al- required for measuring low-levels of 26 Al. Multiple samples of aluminum oxide (Al 2 O 3 ), aluminum nitride (AlN), mixed Al 2 O 3 –AlN as well as aluminum fluoride (AlF 3 ) were tested and compared using the ion source test facility and the stable ion beam (SIB) injector platform at the 25-MV tandem electrostatic accelerator at Oak Ridge National Laboratory. Negative ion currents of atomic and molecular aluminum were examined for each source material. It was found that pure AlN targets produced substantially higher beam currents than the other materials and that there was some dependence on the exposure of AlN to air. The applicability of using AlN as a source material for geological samples was explored by preparing quartz samples as Al 2 O 3 and converting them to AlN using a carbothermal reduction technique, which involved reducing the Al 2 O 3 with graphite powder at 1600 °C within a nitrogen atmosphere. The quartz material was successfully converted to AlN. Thus far, AlN proves to be a promising source material and could lead towards increasing the sensitivity of low-level 26 Al AMS measurements. The potential of using AlN as a source material for nuclear physics is also very promising by placing 26 AlN directly into a source to produce more intense radioactive beams of 26 Al.

Janzen, Meghan S.↗

Design and construction of a new detector to measure ultra-low radioactive-isotope contamination of argon

Large liquid argon detectors offer one of the best avenues for the detection of galactic weakly interacting massive particles (WIMPs) via their scattering on atomic nuclei. The liquid argon target allows exquisite discrimination between nuclear and electron recoil signals via pulse-shape discrimination of the scintillation signals. Atmospheric argon (AAr), however, has a naturally occurring radioactive isotope, 39Ar, a ß emitter of cosmogenic origin. For large detectors, the atmospheric 39Ar activity poses pile-up concerns. The use of argon extracted from underground wells, deprived of 39Ar, is key to the physics potential of these experiments. The DarkSide-20k dark matter search experiment will operate a dual-phase time projection chamber with 50 tonnes of radio-pure underground argon (UAr), that was shown to be depleted of 39Ar with respect to AAr by a factor larger than 1400. Assessing the 39Ar content of the UAr during extraction is crucial for the success of DarkSide-20k, as well as for future experiments of the Global Argon Dark Matter Collaboration (GADMC). This will be carried out by the DArT in ArDM experiment, a small chamber made with extremely radio-pure materials that will be placed at the centre of the ArDM detector, in the Canfranc Underground Laboratory (LSC) in Spain. The ArDM LAr volume acts as an active veto for background radioactivity, mostly ?-rays from the ArDM detector materials and the surrounding rock. This article describes the DArT in ArDM project, including the chamber design and construction, and reviews the background required to achieve the expected performance of the detector.

Noble liquid detectors, Dark Matter detectors, Cry↗

Four-harmonic buncher for radioactive and stable beams switching at the ATLAS facility [Four-harmonic buncher for radioactive and stable beams combination at the ATLAS facility]

Here, the Argonne Tandem Linac Accelerator System (ATLAS) is planning an upgrade to a multi-user facility to simultaneously accelerate both stable beams from an ECR ion source and radioactive beams from an Electron Beam Ion Source charge breeder. The ATLAS Multi-User Upgrade will need to provide high transmission of ion beams with a mass-to-charge ratio up to 7 as it enables more options to alternate radioactive and stable beams. Currently, the bunching is provided with a lumped circuit multi-harmonic buncher, which cannot effectively operate at the required amplitude of the saw-tooth voltage for ions with mass-to-charge ratio of 7 due to thermal issues. RadiaBeam Systems in collaboration with Argonne National Laboratory has designed a four-harmonic coaxial resonator buncher with the ATLAS fundamental frequency of 12.125 MHz, and a compact, less than 2-m-long, footprint, capable of providing the required voltage of 6.2 kV. This device allows fast and reliable pre-bunching of DC ion beams with the capability of fast switching of heavy-ion radioactive and stable beams for delivery to multiple users. In this paper, we will discuss the RF and engineering design considerations of this buncher.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Biogeochemical Changes at Early Stage After the Closure of Radioactive Waste Geological Repository in South Korea

Permanent disposal of low- and intermediate-level radioactive wastes in the subterranean environment has been the preferred method of many countries, including Korea. A safety issue after the closure of a geological repository is that biodegradation of organic materials due to microbial activities generates gases that lead to overpressure of the waste containers in the repository and its disintegration with the release of radionuclides. As part of an ongoing large-scale in situ experiment using organic wastes and groundwater to simulate geological radioactive waste repository conditions, we investigated the geochemical alteration and microbial activities at an early stage (~63 days) intended to be representative of the initial period after repository closure. The increased numbers of both aerobes and facultative anaerobes in waste effluents indicate that oxygen content could be the most significant parameter to control biogeochemical conditions at very early periods of reaction (<35 days). Accordingly, the values of dissolved oxygen and redox potential were decreased. The activation of anaerobes after 35 days was supported by the increased concentration to ~50 mg L-1 of ethanol. These results suggest that the biogeochemical conditions were rapidly altered to more reducing and anaerobic conditions within the initial 2 months after repository closure. Although no gases were detected during the study, activated anaerobic microbes will play more important role in gas generation over the long term.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site

This paper reviews the origin and chemical and rheological complexity of radioactive waste at the U.S. Department of Energy’s Hanford Site. The waste, stored in underground tanks, was generated via three distinct processes over decades of plutonium extraction operations. Although close records were kept of original waste disposition, tank-to-tank transfers and conditions that impede equilibrium complicate our understanding of the chemistry, phase composition, and rheology of the waste. Tank waste slurries comprise particles and aggregates from nano to micron scales, with varying densities, morphologies, heterogeneous compositions, and complicated responses to flow regimes and process conditions. Further, remnant or changing radiation fields may affect the stability and rheology of the waste. These conditions pose challenges for transport through conduits or pipes to treatment plants for vitrification. Additionally, recalcitrant boehmite degrades glass quality and must be reduced prior to vitrification, but dissolves much more slowly than predicted given surface normalized rates. Existing empirical models based on ex situ experiments and observations lack true predictive capabilities. Recent advances in in situ microscopy, aberration corrected TEM, theoretical modeling across scales, and experimental methods for probing the physics and chemistry at mineral-fluid and mineral-mineral interfaces are being implemented to build robustly predictive physics-based models.

Environmental Molecular Sciences Laboratory↗

Immobilization of organic radioactive and non-radioactive liquid waste in a composite matrix

A method for immobilizing liquid radioactive waste is provided, the method having the steps of mixing waste with polymer to form a non-liquid waste; contacting the non-liquid waste with a solidifying agent to create a mixture, heating the mixture to cause the polymer, waste, and filler to irreversibly bind in a solid phase, and compressing the solid phase into a monolith. The invention also provides a method for immobilizing liquid radioactive waste containing tritium, the method having the steps of mixing liquid waste with polymer to convert the liquid waste to a non-liquid waste, contacting the non-liquid waste with a solidifying agent to create a mixture, heating the mixture to form homogeneous, chemically stable solid phase, and compressing the chemically stable solid phase into a final waste form, wherein the polymer comprises approximately a 9:1 weight ratio mixture of styrene block co-polymers and cross linked co-polymers of acrylamides.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Direct reaction experimental studies with beams of radioactive tin ions

The tin chain of isotopes provides a unique region in which to investigate the evolution of single-particle structure, spreading from N = 50 at {sup 100}Sn, through 10 stable isotopes and the N = 82 shell closure at {sup 132}Sn out into the r-process path. Direct reactions performed on radioactive ion beams are sensitive spectroscopic tools for studying exotic nuclei. Here we present one experiment knocking out neutrons from tin isotopes that are already neutron deficient and two reactions that add a neutron to neutron-rich {sup 130}Sn. Both techniques rely on selective particle identification and the measurement of γ rays in coincidence with charged ions. We present the goals of the two experiments and the particle identification for the channels of interest. The final results will be presented in future publications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Modeling delayed thermal runaway in nitric acid-soaked cat litter mixed with radioactive waste

Thermal ignition of radioactive waste within a 55-gallon drum was simulated by using a pressure-dependent waste decomposition model (Hobbs et al. in Process Saf Environ Prot https://doi.org/10.1016/j.psep.2022.09.047, 2022) calibrated with data from full-scale drum experiments (Parker et al. in The thermolytic response of a surrogate RNS waste mixture at the drum scale. Los Alamos National Laboratory Report LA-UR-16-21760, 2016) and validated with experiments from multiple laboratories (Hobbs et al. in Thermal analysis of aged nitric acid-soaked kitty litter in TRU waste drums-23370.WM2023 Conference, Phoenix, AZ, 2023). The acceleration of nitric acid chemistry reacting with an organic cat litter leading to thermal ignition was likely triggered by a restricted vent in the drum. Here, we address whether the form of the rate equation in (Hobbs et al. in Process Saf Environ Prot https://doi.org/10.1016/j.psep.2022.09.047, 2022) is sufficient to extrapolate thermal ignition within aged drums of similar content that have been stored in Texas for over nine years by investigating four different reaction rate forms for waste decomposition. A critical reaction rate reduction analysis is performed on each of these models to determine if delayed thermal runaway within vented aged waste is possible after nine years. We found that a pressure-dependent first-order rate expression not only predicted the accidental ignition of the waste drum, but the form also matches multiple experiments from different laboratories. Even though the waste composition decreases over time, the model predicts that acceleration leading to thermal runaway is possible if the waste is confined, even after 9 years. In conclusion, waste containing oxidizers such as nitric acid should not be mixed with organic adsorbents, especially if the waste is confined.

cookoff↗

EFFECT OF A HIGH OPACITY ON THE LIGHT CURVES OF RADIOACTIVELY POWERED TRANSIENTS FROM COMPACT OBJECT MERGERS

The coalescence of compact objects is a promising astrophysical source of detectable gravitational wave signals. The ejection of r-process material from such mergers may lead to a radioactively powered electromagnetic counterpart signal which, if discovered, would enhance the science returns. As very little is known about the optical properties of heavy r-process elements, previous light-curve models have adopted opacities similar to those of iron group elements. Here we consider the effect of heavier elements, particularly the lanthanides, which increase the ejecta opacity by several orders of magnitude. We include these higher opacities in time-dependent, multi-wavelength radiative transport calculations to predict the broadband light curves of one-dimensional models over a range of parameters (ejecta masses {approx}10{sup -3}-10{sup -1} M{sub Sun} and velocities {approx}0.1-0.3 c). We find that the higher opacities lead to much longer duration light curves which can last a week or more. The emission is shifted toward the infrared bands due to strong optical line blanketing, and the colors at later times are representative of a blackbody near the recombination temperature of the lanthanides (T {approx} 2500 K). We further consider the case in which a second mass outflow, composed of {sup 56}Ni, is ejected from a disk wind, and show that the net result is a distinctive two component spectral energy distribution, with a bright optical peak due to {sup 56}Ni and an infrared peak due to r-process ejecta. We briefly consider the prospects for detection and identification of these transients.

79 ASTRONOMY AND ASTROPHYSICS↗

Modeling and Qualification of a Modified Emission Unit for Radioactive Air Emissions Stack Sampling Compliance

A planned laboratory space and exhaust system modification to the Pacific Northwest National Laboratory Material Science and Technology Building indicated a new evaluation of the mixing at the air sampling system location would be required for compliance to ANSI/HPS N13.1-2011. The modified exhaust system would add a third fan thereby increasing the overall exhaust rate out the stack thus voiding the previous mixing study. Prior to modifying the radioactive air emissions exhaust system, a three-dimensional computational fluid dynamics computer model was used to evaluate the mixing at the sampling system location. Modeling of the new original three-fan system indicated that not all mixing criteria could be met. A second modeling effort was conducted with the addition of an air blender downstream of the confluence of the three fans which then showed satisfactory mixing results. The final installation included an air blender, and the exhaust system underwent full-scale tests to verify velocity, cyclonic flow, gas, and particulate uniformity. The modeling results and those of the full-scale tests show agreement between each of the evaluated criteria. The use of a computational fluid dynamics code was an effective aid in the design process and allowed the sampling system to remain in its original location while still meeting the requirements for sampling at a well-mixed location.

atmospheric emissions, air monitoring, environment↗

High Chrome Refractory Characterization: Part II . Accumulation of Spinel Corrosion Deposits in Radioactive Waste Glass Melters

High Cr 2 O 3 containing Monofrax ™ K‐3 is a robust refractory that is used in radioactive waste glass melters worldwide. Monofrax ™ K‐3 contains highly reduced phases. Conversely, many of the radioactive feeds being processed are highly oxidizing. The K‐3 refractory corrosion rates in oxidizing (high nitrate) feeds were ~1.8–2.8 times higher than the rates determined using reducing feeds. The corrosion product formed is a mixture of spinel and glass (slag) that can accumulate on the melter floor. A methodology to calculate the depth of slag deposits from refractory corrosion is presented and verified with slag measurements from the Defense Waste Processing Facility ( DWPF ) melter after it had processed oxidized feeds for 1.75 years. The calculations show that had the facility continued to process oxidized feeds the melter lifetime (based on when the deposits could have reached and blocked the pour spout riser) would have been ~4.5 years. The DWPF changed to a reducing flow sheet after ~3 years of operation. The lifetimes of Melter #1 and Melter #2, assuming a failure due to pour spout blockage, are calculated as 7.7–12 years based on corrosion rates measured with reducing feeds. Lifetimes of 9 and >11 years have actually been achieved.

Jantzen, Carol M.↗

Thermodynamic assessment of the hollandite high‐level radioactive waste form

Abstract Hollandite has been studied as a candidate ceramic waste form for the disposal of high‐level radioactive waste due to its inherent leach resistance and ability to immobilize alkaline‐earth metals such as Cs and Ba at defined lattice sites in the crystallographic structure. The chemical and structural complexity of hollandite‐type phases developed for high‐level waste immobilization limits the systematic experimental research that is required to understand phase development due to the large number of potential additives and compositional ranges that must be evaluated. Modeling the equilibrium behavior of the complex hollandite‐forming oxide waste system would aid in the design and processing of hollandite waste forms by predicting their thermodynamic stability. Thus, a BaO–Cs 2 O–TiO 2 –Cr 2 O 3 –Al 2 O 3 –Fe 2 O 3 –FeO–Ga 2 O 3 thermodynamic database was developed in this work according to the CALPHAD methodology. The compound energy formalism was used to model solid solution phases such as hollandite while the two‐sublattice partially ionic liquid model characterized the oxide melt. Results of model optimizations are presented and discussed including a 1473 K isothermal BaO–Cs 2 O–TiO 2 pseudo‐ternary diagram that extrapolates phase equilibrium behavior to regions not experimentally explored.

Utlak, Stephen A.↗

Water Migration and Swelling in Engineered Barrier Materials for Radioactive Waste Disposal

Deep, underground repositories are needed to isolate radioactive waste from the biosphere. Because bentonite is an integral component of many multibarrier repository systems, information on the hydraulic behavior of bentonite is crucial for modeling the long-term viability of such systems. In this paper the hydraulic behavior of bentonite samples was analyzed as a function of aggregate size, and samples were subjected to hydrothermal treatments involving contact with NaCl, KCl, and deionized water. Neutron and X-ray imaging were used to quantify water sorption into packed bentonite samples and bentonite swelling into the water column. The distance between the original clay-water interface and the wetting front was determined as a function of time. Average water uptake exhibited a square-root-of-time dependence in freshly prepared samples, but more variable rates were observed for samples previously in contact with water. The radiography was supported by small-angle neutron scattering analysis and ultra-small-angle neutron scattering analysis of aggregate size distributions and by inelastic neutron scattering to understand the physicochemical environment of the sorbed water. Results showed that hydrothermal treatment with KCl had the greatest effect of increased water transport in the bentonite, possibly as a result of the interaction of K + with smectite layers in the clay.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radioactive Iodine and Krypton Control for Nuclear Fuel Reprocessing Facilities

Nuclear fission results in the production of fission products and activation products, some of which tend to be volatile during used fuel reprocessing. These can evolve in volatile species in the reprocessing facility off-gas streams, depending on the separations and reprocessing technologies that are used. Radionuclides that have been identified as “volatile radionuclides” are noble gases (most notably isotopes of Kr and Xe); 3H; 14C; and 129I. Radionuclides that tend to form volatile species that evolve into reprocessing facility off-gas systems are more challenging to efficiently control compared to radionuclides that tend to stay in solid or liquid phases. Future used fuel reprocessing facilities in the United States can require efficient capture of some volatile radionuclides in their off-gas streams to meet regulatory emission requirements. In aqueous reprocessing, these radionuclides are most commonly expected to evolve into off-gas streams in tritiated water [3H2O (T2O) and 3HHO (THO)], radioactive CO2, noble gases, and gaseous HI, I2, or volatile organic iodides. The fate and speciation of these radionuclides from a non-aqueous fuel reprocessing facility is less well known at this time, but active investigations are in progress. An Off-Gas Sigma Team was formed in late FY 2009 to integrate and coordinate the Fuel Cycle Research and Development (FCR&D) activities directed towards the capture and sequestration of the these volatile radionuclides (Jubin 2012a). The Sigma Team concept was envisioned to bring together multidisciplinary teams from across the DOE complex that would work collaboratively to solve the technical challenges and to develop the scientific basis for the capture and immobilization technologies such that the sum of the efforts was greater than the individual parts. The Laboratories currently participating in this effort are Argonne National Laboratory (ANL), Idaho National Laboratory (INL), Oak Ridge National Laboratory (ORNL), Pacific Northwest National Laboratory (PNNL), and Sandia National Laboratories (SNL). This article focuses on control of volatile radionuclides that evolve during aqueous reprocessing of UNF. In particular, most of the work by the Off-gas Sigma Team has focused on the capture and sequestration of 129I and 85Kr, mainly because, as discussed below, control of 129I can require high efficiencies to meet regulatory requirements, and control of 85Kr using cryogenic processing, which has been the technology demonstrated and used commercially to date, can add considerable cost to a reprocessing facility.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analytical Determination of Radioactive Strontium and Cesium by Thermal Ionization Mass Spectrometry

Thermal ionization mass spectrometry (TIMS) has been evaluated for the detection of the radioactive isotopes of strontium and cesium. The instrument was investigated for the analysis of isotopic ratios of 89Sr to 90Sr and 135Cs to 137Cs in the presence of atomic isobars (Y and Zr for Sr analysis and Ba for Cs analysis). Signicant discrimination using TIMS was found for both Sr and Cs through evaluation using stable isotopes. Fusion procedures with different flux were evaluated for preparation of sample matrices. Chemical separations were developed and used after fusion to isolate the Sr and Cs from a prepared background matrix (i.e., Montana Soil). A graded approach, increasing in stable background isotopes, was performed to monitor the chemistry and instrument response. A thermal neutron irradiation was performed to produce a sample that contained the radioisotopes of Sr and Cs. Even though the irradiated sample was not a certified standard it does provide accurate expectation values via published, well understood cumulative fission yield data. The results presented in this work correlate extremely well with the published data. Furthermore, a significant decrease in uncertainty (by a factor of 5 { 10) was found for the isotopic ratios measured with TIMS compared to the published values.

TIMS, environmental contamination, radiostrontium,↗