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At least 847 records · Page 47

Multivariate Analysis for Quantification of Plutonium(IV) in Nitric Acid Based on Absorption Spectra

Development of more effective, reliable, and fast methods for monitoring process streams is a growing opportunity for analytical applications. Many fields can benefit from on-line monitoring, including the nuclear fuel cycle where improved methods for monitoring radioactive materials will facilitate maintenance of proper safeguards and ensure safe and efficient processing of materials. On-line process monitoring with a focus on optical spectroscopy can provide a fast, non-destructive method for monitoring chemical species. However, identification and quantification of species can be hindered by the complexity of the solutions if bands overlap or show condition-dependent spectral features. Plutonium (IV) is one example of a species which displays significant spectral variation with changing nitric acid concentration. Single variate analysis (i.e. Beer’s Law) is difficult to apply to the quantification of Pu(IV) unless the nitric acid concentration is known and separate calibration curves have been made for all possible acid strengths. Multivariate, or chemometric, analysis is an approach that allows for the accurate quantification of Pu(IV) without a priori knowledge of nitric acid concentration.

Lines, Amanda M.↗

Experimental Investigation of Uranium Volatility during Vapor Condensation

The predictive models that describe the fate and transport of radioactive materials in the atmosphere following a nuclear incident (explosion or reactor accident) assume that uranium-bearing particulates would attain chemical equilibrium during vapor condensation. Here, we show that kinetically driven processes in a system of rapidly decreasing temperature can result in substantial deviations from chemical equilibrium. This can cause uranium to condense out in oxidation states (e.g., UO 3 vs UO 2 ) that have different vapor pressures, significantly affecting uranium transport. To demonstrate this, we synthesized uranium oxide nanoparticles using a flow reactor under controlled conditions of temperature, pressure, and oxygen concentration. The atomized chemical reactants passing through an inductively coupled plasma cool from ~5000 to 1000 K within milliseconds and form nanoparticles inside a flow reactor. The ex situ analysis of particulates by transmission electron microscopy revealed 2–10 nm crystallites of fcc-UO 2 or α-UO 3 depending on the amount of oxygen in the system. α-UO 3 is the least thermodynamically preferred polymorph of UO 3 . The absence of stable uranium oxides with intermediate stoichiometries (e.g., U 3 O 8 ) and sensitivity of the uranium oxidation states to local redox conditions highlight the importance of in situ measurements at high temperatures. Therefore, we developed a laser-based diagnostic to detect uranium oxide particles as they are formed inside the flow reactor. Our in situ measurements allowed us to quantify the changes in the number densities of the uranium oxide nanoparticles (e.g., UO 3 ) as a function of oxygen gas concentration. Our results indicate that uranium can prefer to be in metastable crystal forms (i.e., α-UO 3 ) that have higher vapor pressures than the refractory form (i.e., UO 2 ) depending on the oxygen abundance in the surrounding environment. This demonstrates that the equilibrium processes may not dominate during rapid condensation processes, and thus kinetic models are required to fully describe uranium transport subsequent to nuclear incidents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Potential Interactions of Novec 1230 and Its Thermal Degradation Products with Actinide Metals and Oxides

The environmentally friendly and mainly chemically inert fire suppressant, Novec 1230, is being increasingly used worldwide. However, no published study has considered using Novec 1230 with fires involving radioactive material including actinides; here, therefore, this research note focuses on the possible interactions between Novec 1230 and its thermal degradation products (TDPs) with some actinide compounds (e.g., actinide metal and oxides) commonly present in a radiological facility in the event of a fire. Previous studies of halogenated fire suppressants used in actinide metal fires indicate a possibility for Novec 1230 or its TDPs to chemically interact with actinide compounds at elevated temperatures; however, these reactions are highly unlikely to cause either runaway exothermic reactions or gaseous actinide release.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Performance Evaluation of a High Salinity Produced Water Treatment Train: Chemical Analysis and Aryl Hydrocarbon Activation

Water scarcity and increased energy demands have put a strong focus on improving industries at the heart of the water–energy nexus. Treatment of oil and gas produced water (PW) can help reduce freshwater consumption during hydraulic fracturing, especially in arid regions, while also removing harmful contaminants from entering the environment. However, it is also difficult to treat because PW contains high concentrations of many environmentally toxic contaminants, which require complex and expensive treatment processes to achieve their removal. To demonstrate the possibility of PW treatment and reuse in the O&G industry, a comprehensive environmental toxicity and water quality analysis throughout a five-process treatment train was performed on high salinity (>120 g/L) Permian basin raw PW. Here, the concentrations of naturally occurring radioactive materials were reduced by over 99%, total organic carbon was reduced by 93%, and inorganic constituents, including total dissolved solids, were reduced by over 99%. Compounds that induced the aryl hydrocarbon receptor and caused cytotoxicity in MCF-7 cells were also removed. Overall, the results of this study show that a short treatment train (five distinct unit processes) can be effective in treating PW to a level suitable for use outside of the oil industry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Geobacter sulfurreducens Immobilized Boron-Doped Diamond Electrodes for Uranium(VI) in Water Electrochemical Bioremediation

The proliferation of nuclear science and technology has resulted in an increase in nuclear waste containing uranium, posing significant risks to both human and environmental health. This study proposes the use of Geobacter sulfurreducens (G. sulfurreducens) modified boron-doped diamond electrodes to facilitate the reduction and removal of uranium(VI) from aqueous media. The bioremediation process involves electrochemically immobilizing the bacteria on a boron-doped diamond electrode (BDD). The immobilization process requires applying reduction potentials ranging from −0.40 to −0.70 V (vs Ag/AgCl (3 M NaCl)), with −0.60 V identified as the optimal potential for effective bacterial modification. The uranium source is provided by a 2.0 mM uranyl acetate solution in G. sulfurreducens growth medium. Scanning electron microscopy (SEM) reveals a highly uniform layer of uranium on the electrode surface. Energy-dispersive X-ray fluorescence spectroscopy (EDS) and cyclic voltammetry (CV) studies confirm the presence of uranium in the system. Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) successfully elucidate the reduction process of U(VI) to predominantly U(IV) using a bacteria-electrode coupled system. Additionally, a comparison is made with the electrochemical removal of uranyl ions using the electrodeposition method on unmodified BDD. Results demonstrate the presence of three uranium oxide species (UO 2 , UO 3 , and U 3 O 8 ) on the BDD electrode after experimentation, in contrast to the G. sulfurreducens/BDD assembly, which achieves the predominant reduction of UO 2 2+ to UO 2 with a small quantity of UO 3 as the final species. This study highlights the efficient electrochemical removal of uranyl ions from aqueous media at the G. sulfurreducens/BDD interface through chronoamperometry, presenting a promising approach for remediating sites contaminated with radioactive materials. The findings contribute to the exploration of sustainable alternatives for managing nuclear waste, emphasizing the potential of this electrochemical bioremediation strategy.

Bacteria↗

Impact of ionizing radiation on superconducting qubit coherence

The practical viability of any qubit technology stands on long coherence times and high-fidelity operations with the superconducting qubit modality being an auspicious example, However, superconducting qubit coherence is impacted by broken Cooper pairs referred to as quasiparticles, with a density that is empirically observed to be orders of magnitude greater than the value predicted for thermal equilibrium by the Bardeen-Cooper-Schrieffer (BCS) theory of superconductivity. Previous work has shown that infrared photons significantly increase the quasiparticle density, yet even in the best isolated systems, it still remains higher than expected, suggesting that another generation mechanism exists. In this Letter, we provide evidence that ionizing radiation from environmental radioactive materials and cosmic rays contributes to this observed difference, leading to an elevated quasiparticle density that would ultimately limit superconducting qubits of the type measured here to coherence times in the millisecond regime. Additionally, we further demonstrate that introducing radiation shielding reduces the flux of ionizing radiation and positively correlates with increased coherence time. Albeit a small effect for today’s qubits, reducing or otherwise mitigating the impact of ionizing radiation will be critical for realizing fault-tolerant superconducting quantum computers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Expectation-propagation for weak radionuclide identification at radiation portal monitors

We propose a sparsity-promoting Bayesian algorithm capable of identifying radionuclide signatures from weak sources in the presence of a high radiation background. The proposed method is relevant to radiation identification for security applications. In such scenarios, the background typically consists of terrestrial, cosmic, and cosmogenic radiation that may cause false positive responses. We evaluate the new Bayesian approach using gamma-ray data and are able to identify weapons-grade plutonium, masked by naturally-occurring radioactive material (NORM), in a measurement time of a few seconds. We demonstrate this identification capability using organic scintillators (stilbene crystals and EJ-309 liquid scintillators), which do not provide direct, high-resolution, source spectroscopic information. Compared to the EJ-309 detector, the stilbene-based detector exhibits a lower identification error, on average, owing to its better energy resolution. Organic scintillators are used within radiation portal monitors to detect gamma rays emitted from conveyances crossing ports of entry. The described method is therefore applicable to radiation portal monitors deployed in the field and could improve their threat discrimination capability by minimizing “nuisance” alarms produced either by NORM-bearing materials found in shipped cargoes, such as ceramics and fertilizers, or radionuclides in recently treated nuclear medicine patients.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Structural study of complexes formed by acidic and neutral organophosphorus reagents

The coordination of the trivalent 4f ions, Ln = La 3+ , Dy 3+ , and Lu 3+ , with neutral and acidic organophosphorus reagents, both individually and combined, was studied by use of X-ray absorption spectroscopy. These studies provide metrical information about the interatomic interactions between these cations and the ligands tri- n -butyl phosphate (TBP) and di- n -butyl phosphoric acid (HDBP), whose behavior are of practical importance to chemical separation processes that are currently used on an industrial scale. Previous studies have suggested the existence of complexes involving a mixture of ligands, accounting for extraction synergy. Through systematic variation of the aqueous phase acidity and extractant concentration and combination, we have found that complexes with Ln and TBP : HDBP at any mixture and HDBP alone involve direct Ln–O interactions involving 6 oxygen atoms and distant Ln–P interactions involving on average 3–5 phosphorus atoms per Ln ion. It was also found that Ln complexes formed by TBP alone seem to favor eight oxygen coordination, though we were unable to obtain metrical results regarding the distant Ln–P interactions due to the low signal attributed to a lower concentration of Ln ions in the organic phases. Our study does not support the existence of mixed Ln–TBP–HDBP complexes but, rather, indicates that the lanthanides are extracted as either Ln–HDBP complexes or Ln–TBP complexes and that these complexes exist in different ratios depending on the conditions of the extraction system. Furthermore, this fundamental structural information offers insight into the solvent extraction processes that are taking place and are of particular importance to issues arising from the separation and disposal of radioactive materials from used nuclear fuel.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Preliminary analysis of loss-of-coolant accident in Fukushima nuclear accident

Loss-of-Coolant Accident (LOCA) in Boiling Water Reactor (BWR) especially on Fukushima Nuclear Accident will be discussed in this paper. The Tohoku earthquake triggered the shutdown of nuclear power reactors at Fukushima Nuclear Power station. Though shutdown process has been completely performed, cooling process, at much smaller level than in normal operation, is needed to remove decay heat from the reactor core until the reactor reach cold-shutdown condition. If LOCA happen at this condition, it will cause the increase of reactor fuel and other core temperatures and can lead to reactor core meltdown and exposure of radioactive material to the environment such as in the Fukushima Dai Ichi nuclear accident case. In this study numerical simulation has been performed to calculate pressure composition, water level and temperature distribution on reactor during this accident. There are two coolant regulating system that operational on reactor unit 1 at this accident, Isolation Condensers (IC) system and Safety Relief Valves (SRV) system. Average mass flow of steam to the IC system in this event is 10 kg/s and could keep reactor core from uncovered about 3,2 hours and fully uncovered in 4,7 hours later. There are two coolant regulating system at operational on reactor unit 2, Reactor Core Isolation Condenser (RCIC) System and Safety Relief Valves (SRV). Average mass flow of coolant that correspond this event is 20 kg/s and could keep reactor core from uncovered about 73 hours and fully uncovered in 75 hours later. There are three coolant regulating system at operational on reactor unit 3, Reactor Core Isolation Condenser (RCIC) system, High Pressure Coolant Injection (HPCI) system and Safety Relief Valves (SRV). Average mass flow of water that correspond this event is 15 kg/s and could keep reactor core from uncovered about 37 hours and fully uncovered in 40 hours later.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Accumulation of radionuclides in selected marine biota from Manjung coastal area

Distribution of radionuclides from anthropogenic activities has been intensively studied due to the accumulation of radionuclides in marine ecosystem. Manjung area is affected by rapid population growth and socio-economic development such as heavy industrial activities including coal fired power plant, iron foundries, port development and factories, agricultural runoff, waste and toxic discharge from factories.It has radiological risk and toxic effect when effluent from the industries in the area containing radioactive materials either being transported to the atmosphere and deposited back over the land or by run off to the river and flow into coastal area and being absorbed by marine biota. Radionuclides presence in the marine ecosystem can be adversely affect human health when it enters the food chain. This study is focusing on the radionuclides [thorium (Th), uranium (U), radium-226 ({sup 226}Ra), radium-228 ({sup 228}Ra) and potassium-40 ({sup 40}K)] content in marine biota and sea water from Manjung coastal area. Five species of marine biota including Johnius dussumieri (Ikan Gelama), Pseudorhombus malayanus (Ikan Sebelah), Arius maculatus (Ikan Duri), Portunus pelagicus (Ketam Renjong) and Charybdis natator (Ketam Salib) were collected during rainy and dry seasons. Measurements were carried out using Inductively Coupled Plasma Mass Spectrometer (ICPMS). The results show that the concentration of radionuclides varies depends on ecological environment of respective marine biota species. The concentrations and activity concentrations are used for the assessment of potential internal hazard index (H{sub in}), transfer factor (TF), ingestion dose rate (D) and health risk index (HRI) to monitor radiological risk for human consumption.

54 ENVIRONMENTAL SCIENCES↗

Design of a containment apparatus for synchrotron XAS measurements of radioactive fluid samples under high temperatures and pressures

The simple working principles and versatility of the hydrothermal diamond-anvil cell (HDAC) make it signifcantly useful for synchrotron x-ray studies of aqueous and fluid samples at high pressure-temperature (P-T) conditions. Yet, safety concerns need to be overcome in order to use the HDAC for synchrotron studies of aqueous radioactive samples at high temperatures and pressures. For accomplishment of such hydrothermal experiments of radioactive materials at synchrotron beamlines, the samples are required to be enclosed in a containment system employing three independent layers of airtight sealing at some synchrotron facilities while enabling access to the sample using several experimental probes, including incoming and outgoing x-rays. In this article, we report the design and implementation of a complete radiological safety enclosure system for an HDAC specialized for high P-T x-ray absorption spectroscopy (XAS) measurements of aqueous solutions containing the actinides at synchrotron beamlines. The enclosure system was successfully tested for XAS experiments using the HDAC with aqueous samples containing depleted uranium at temperatures ranging from 25 to 500 °C and pressures ranging from vapor pressure to 350 MPa.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Dose Rate Evaluation for the ES-3100 Package with HEU Content Using MCNP, ADVANTG, Monaco, and MAVRIC

Here, this paper presents a comparative study of dose rate calculations for the ES-3100 package with highly enriched uranium (HEU) content for different source configurations using computer codes: (1) MCNP; (2) Automated Variance Reduction Generator (ADVANTG)/MCNP; (3) Monaco; and (4) Monaco with Automated Variance Reduction using Importance Calculations (MAVRIC). The Model ES-3100 package was developed at the Y-12 National Security Complex for domestic and international transportation of Type B fissile radioactive material. In this study, six different source configurations (i.e., solid cylinder, cylindrical hemi-shell, cylindrical shell, rectangular plate, cylindrical rod, or cylindrical segment form) having 36 kg of HEU metal inside the package containment vessel (based on configurations in the ES-3100/HEU safety analysis report for packaging) are evaluated. Dose rates at the package surfaces and 1 m from the package surfaces are calculated for these different source configurations. MCNP and Monaco cases are run without any biasing options to accelerate the convergence. Consistent Adjoint Driven Importance Sampling (CADIS) and Forward-Weighted CADIS (FW-CADIS) methods developed at the Oak Ridge National Laboratory are implemented in ADVANTG/MCNP and MAVRIC codes to accelerate the convergence. ADVANTG generates variance reduction parameters using Denovo code, and MCNP is used with the variance reduction parameters to accelerate the convergence. MAVRIC uses Denovo code to construct an importance map and a biased source distribution that are supplied to Monaco to accelerate the Monte Carlo simulation. The FW-CADIS option in ADVANTG and MAVRIC is used to accelerate the convergence in this study. The accelerated convergence cases (ADVANTG/MCNP and MAVRIC) are about 100 times faster with 100 times less particle simulation than those cases run without biasing options (analog MCNP and analog Monaco). Lastly, the MCNP, ADVANTG/MCNP, Monaco, and MAVRIC calculated dose rates at the package surfaces and at 1 m from the package surfaces for the different source configurations are compared and are found to be in general agreement.

42 ENGINEERING↗

MASTODON: An Open-Source Software for Seismic Analysis and Risk Assessment of Critical Infrastructure

Seismic analysis and risk assessment of safety-critical infrastructure like hospitals, nuclear power plants, dams, and facilities handling radioactive materials involve computationally intensive numerical models and coupled multiphysics scenarios. They are also performed in a strict regulatory environment that requires high software quality assurance standards, and in the case of safety-related nuclear facilities, a conformance to the American Society of Mechanical Engineers Nuclear Quality Assurance (NQA-1) standard. This paper introduces the open-source finite-element software, MASTODON (Multi-hazard Analysis of Stochastic Time-Domain Phenomena), which implements state-of-the-art seismic analysis and risk assessment tools in a quality-controlled environment. MASTODON is built on MOOSE (Multi-physics Object-Oriented Simulation Environment), which is a highly parallelizable, NQA-1 conforming, coupled multiphysics, finite-element framework developed at Idaho National Laboratory. MASTODON is capable of fault rupture and source-to-site wave propagation using the domain reduction method, nonlinear site response, and soil-structure interaction analysis, implicit and explicit time integration, automated stochastic simulations, and seismic probabilistic risk assessment. When coupled with other MOOSE applications, MASTODON can also solve strongly and weakly coupled multiphysics problems. This paper presents a summary of the capabilities of MASTODON and some demonstrative examples.

42 ENGINEERING↗

Improved learning from data competitions through strategic design of training and test data sets

Leveraging the depth and breadth of solutions generated through crowdsourcing can be a powerful accelerator to method development for high consequence problems. While data science competitions have become quite popular and prevalent, particularly in supervised learning formats, their implementations by the host are highly variable. Without careful planning, a supervised learning competition is vulnerable to overfitting, where the winning solutions are so closely tuned to the particular set of provided data that they cannot generalize to the general underlying problem of interest to the host. This paper outlines important considerations for strategically designing relevant and informative data sets to maximize the learning outcome from hosting a competition. These include: precisely defining the scope of the problem, encouraging participation by competitors from diverse technical backgrounds, specifying the most interesting solution space in order to encourage improvement and distinguish between competitors, strategically generating data sets that enable testing for interpolation and extrapolation to new scenarios of interest, leveraging design of experiment principles for strategic data design while preventing unintentional artifacts in the competition data set that an algorithm could exploit without addressing the real problem of interest, and carefully designing the leaderboard scoring metric to select top solutions that exactly match the overall competition goals. The methods are illustrated with a recently completed competition in the context of urban radiological search to evaluate algorithms capable of detecting, identifying, and locating radioactive materials. Simulated data were used in the urban search competition. Ideas for using measured real data in competitions are also suggested

97 MATHEMATICS AND COMPUTING↗

Low-background temperature sensors fabricated on parylene substrates

Temperature sensors fabricated from ultra-low radioactivity materials have been developed for low-background experiments searching for neutrinoless double-beta decay and the interactions of WIMP dark matter. The sensors consist of electrical traces photolithographically-patterned onto substrates of vapor-deposited parylene. They are demonstrated to function as expected, to do so reliably and robustly, and to be highly radio-pure. This work is a proof-of-concept study of a technology that can be applied to broad class of electronic circuits used in low-background experiments.

47 OTHER INSTRUMENTATION↗

The Majorana Demonstrator readout electronics system

The M AJORANA D EMONSTRATOR comprises two arrays of high-purity germanium detectors constructed to search for neutrinoless double-beta decay in 76 Ge and other physics beyond the Standard Model. Its readout electronics were designed to have low electronic noise, and radioactive backgrounds were minimized by using low-mass components and low-radioactivity materials near the detectors. This paper provides a description of all components of the M AJORANA D EMONSTRATOR readout electronics, spanning the front-end electronics and internal cabling, back-end electronics, digitizer, and power supplies, along with the grounding scheme. The spectroscopic performance achieved with these readout electronics is also demonstrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Target development using the method of High-Intensity Vibrational Powder Plating (HIVIPP) at the Center for Accelerator Target Science (CATS) at Argonne National Laboratory (ANL)

One of the primary goals of the Center for Accelerator Target Science (CATS) is to provide targets and foils in support of the ATLAS User Facility and the Low-Energy community at large. While a wide array of target production techniques are available at CATS, new methods that must be explored invariably arise. One such technique, the High-Intensity Vibrational Powder Plating (HIVIPP), was first reported in 1997 by Isao Sugai. It was developed to produce targets and stripper foils that were difficult to make by standard methods. At Argonne National Laboratory (ANL), we have successfully constructed and tested a simple system for this purpose. We have produced targets of carbon and titanium on various metal backings using the HIVIPP method. We are currently in the exciting phase of exploring the production of other elements, including isotopically enriched and radioactive material. This work is in progress and will be further detailed with specific examples.

47 OTHER INSTRUMENTATION↗

The effect of jet–ejecta interaction on the viewing angle dependence of kilonova light curves

ABSTRACT The merger of two neutron stars produces an outflow of radioactive heavy nuclei. Within a second of merger, the central remnant is expected to also launch a relativistic jet, which shock-heats and disrupts a portion of the radioactive ejecta. Within a few hours, emission from the radioactive material gives rise to an ultraviolet, optical, and infrared transient (a kilonova). We use the endstates of a suite of 2D relativistic hydrodynamic simulations of jet–ejecta interaction as initial conditions for multidimensional Monte Carlo radiation transport simulations of the resulting viewing angle-dependent light curves and spectra starting at $1.5\, \mathrm{h}$ after merger. We find that on this time-scale, jet shock heating does not affect the kilonova emission for the jet parameters we survey. However, the jet disruption to the density structure of the ejecta does change the light curves. The jet carves a channel into the otherwise spheroidal ejecta, revealing the hot, inner regions. As seen from near (≲30°) the jet axis, the kilonova is brighter by a factor of a few and bluer. The strength of this effect depends on the jet parameters, since the light curves of more heavily disrupted ejecta are more strongly affected. The light curves and spectra are also more heavily modified in the ultraviolet than in the optical.

Klion, Hannah↗