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At least 1,099 records · Page 61

Machine learning for fundamental spectroscopic and thermodynamic data of actinides and lanthanides

Accurately modeling optical spectra with absolute radiometric intensities is vital for nuclear forensics applications that depend on characterizing optical emissions from energetic nuclear phenomena. This requires precise knowledge of the individual atomic transition probabilities, known as Einstein A-coefficients, for each emission line. Obtaining these values theoretically or experimentally is often impractical due to the complex electronic structures and the number of transitions involved in atoms relevant to nuclear applications. In this study, we explore the use of machine learning to predict the Einstein A coefficients for atomic transitions. Seven models were evaluated that ranged from deep learning to decision tree algorithms, and found that gradient boosting performed best, specifically the Extreme Gradient Boosting (XGB) architecture, achieving a precision of 86% across transitions of 36 elements. Furthermore, the model was cross-validated using published transition probabilities reported in the literature and applied to estimate Pu plasma temperatures from a previous experiment conducted at Savannah River National Laboratory.

Atomic spectroscopy↗

Real-time gross actinide monitoring in extreme (10 6 :1) beta-gamma background fluid streams using mini-ATMFDs

Real-time, trace alpha activity monitoring in extreme mixed radiation fields is a well-known challenge in fission product-rich streams containing mixtures of beta-gamma-alpha radiation-emitting isotopes, arising due to the extreme 10 6 :1 ratio of background beta-gamma vs. alpha radiation activity levels. This paper presents results from a novel approach to addressing this challenge, based on Tensioned Metastable Fluid Detector (TMFD) sensing technology. An acoustically driven technique was developed and tested at Purdue University (using dissolved Rn-Po and U-chain alpha emitters), and validated (with dissolved Pu) at Savannah River National Laboratory for real-time monitoring of alpha activity in the 100–10,000 dpm/mL range.

Environmental Monitoring↗

Nuclear Criticality Safety [Book Chapter]

Nuclear Criticality Safety is a field of nuclear engineering that involves worker and public safety during the handling, processing, transportation, and storage activities of fissile isotopes ( 233 U, 235 U, and 239 Pu) outside of nuclear reactors. Criticality accidents release energy as a result of accidentally producing a self-sustaining fission chain reaction. If these occur during hands-on operations the results can be lethal to worker within about 4.6 m (15 ft.) of the accident. There have been 22 process criticality accidents in the world between 1953 and 1999 resulting in physical injury, on and off-site dose, or death. Nuclear Criticality Safety involves work by qualified persons to preclude criticality accidents and their consequences by ensuring activities with fissionable materials remain subcritical, i.e., safe, during all normal and credible abnormal conditions. This article presents information about those nuclear fuel cycle steps presenting Nuclear Criticality Safety concerns that must be considered to ensure worker and public safety is assured.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A comprehensive diffusion mobility database comprising 23 elements for magnesium alloys

We report that reliable experimental diffusion coefficients of 10 key alloying elements in Mg obtained by the present authors together with experimental data in the literature enabled us to perform a systematic test of the reliability of diffusion coefficients obtained from DFT calculations. The computed activation energy values were found to be quite accurate (mostly within 0.2 eV) but the computed pre-factors were less reliable. Such insights allowed us to develop a practical and yet robust strategy to perform diffusion mobility assessments by adopting the computed activation energy while fitting only the pre-factor when available experimental data are limited to a narrow temperature range. The overall good agreement between the DFT data and experimental data also gave us the confidence to employ the computed data for those that were still missing or inaccessible from experimental measurements. A systematic assessment of both the measured and computed diffusion data in hcp Mg was performed using the above holistic approach to yield the most comprehensive open Mg mobility database to date, comprising 23 elements (Mg, Ag, Al, Be, Ca, Cd, Ce, Cu, Fe, Ga, Gd, In, La, Li, Mn, Nd, Ni, Pu, Sb, Sn, U, Y, Zn). This more reliable mobility database will contribute to future development of advanced Mg alloys. The holistic approach developed in this study will be very beneficial to the future establishment of reliable mobility databases for other alloy systems as well.

36 MATERIALS SCIENCE↗

Reassessing methods to close the nuclear fuel cycle

This paper presents the major takeaways from studies conducted over several years that were focused on transitioning the U.S. nuclear infrastructure from the current once-through fuel cycle to one in which fuel is continuously recycled in fast reactors. Furthermore, these studies involved simulating and analyzing numerous example scenarios of fuel cycle transition with various assumptions on technology, policy, and material utilization strategies. Among the many findings, perhaps the most important is that under certain conditions, the use of high-assay low-enriched uranium to start up a fleet of fast reactors may be more favorable compared to using recycled Pu from thermal reactors since it is less constrained by other technologies and may even be more economical.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Constrained Bayesian optimization of criticality experiments

The design of criticality experiments is typically an iterative process that employs a Monte Carlo transport code. The goal is to find a design that optimizes some variable, like the sensitivity of a response to a cross section, while simultaneously ensuring criticality. The high fidelity of the Monte Carlo code is a great asset, but it makes exploring the design space computationally expensive. Herein, we present how a constrained Bayesian optimization algorithm can be used to efficiently design a criticality experiment. It uses Gaussian processes as a surrogate model to probe the design space and to reduce the number of code executions that are needed to find the optimum. Furthermore, we demonstrate constrained Bayesian optimization with a Pu-239/polyethylene solution system and a TEX experiment that is designed for criticality safety validation of a nuclear waste model at the Hanford Site. For both systems, a global optimum was found within 75 Monte Carlo simulations.

42 ENGINEERING↗

Machine learning application to single channel design of molten salt reactor

This study proposes a robust approach to quickly design a nuclear reactor core and explores the best performing machine learning (ML) technique for predicting feature parameters of the core. Here we implemented the approach into a hypothetical channel of molten salt reactors to demonstrate the applicability of the method. We prepared a Python tool, named Plankton, which couples to a reactor physics code and an optimization tool, and imports ML methods. The tool performs three consecutive phases: reactor database generation, machine learning application, and design optimization. We identified the extra trees method as the best performing estimator. With the estimator, we found nine optimum designs in total, one for each fuel-salt pair, and estimated all the performance metrics of the designs with a <5% prediction error compared to their actual values. U-Pu-NaCl fuel-salt gave promising results with the highest conversion ratio, the most negative feedback coefficient, and the lowest fast flux.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

On silica's roles in controlling americium migration in contaminated sediments

Two studies in the early 1980s described the leaching behavior of americium (Am) disposed as part of acidic high-salt processing wastes from the Hanford Site’s Plutonium Finishing Plant to nearby ground sediments. Here these batch leach experiments showed that the Am concentrations followed a linear log [Am] versus pH relationship with a slope of –1. Column leach experiments in the second study, however, did not follow this relationship and only ~30% of the americium desorbed even after extensive column leaching. Here, the 1980s research is re-examined along with previously unpublished information and, in light of recent published work, a plausible mechanism is proposed to explain these phenomena. Amorphous silica in the contaminated sediments is postulated to be the substrate responsible for both the exchangeable Am available for leaching and the retained low-leachable Am made evident in the column leach experiments. The exchangeable Am 3+ in the contaminated sediment leach experiments behaves with pH dependence similar to that observed for uptake onto amorphous silica of sodium (Na + ), calcium (Ca 2+ ), barium (Ba 2+ ), cadmium (Cd 2+ ), uranyl (UO 2 2+ ), ferric (Fe 3+ ), chromic (Cr 3+ ), cupric (Cu 2+ ), plumbous (Pb 2+ ), uranium(IV) (U 4+ ), plutonium(IV) (Pu 4+ ), zirconium (Zr 4+ ), analogue lanthanide (gadolinium, Gd 3+ , europium, Eu 3+ , and lutetium, Lu 3+ ) and curium (Cm 3+ ) ions as well as other studies with Am 3+ . Correspondingly, the residual low-leachable Am 3+ revealed in the column leach experiments is attributed to incorporation of Am 3+ within amorphous silica by dynamic Am 3+ sorption and silica precipitation processes.

58 GEOSCIENCES↗

Comparison of active interrogation methods for source location in a scattering and absorbing medium, consisting of PGNAA, and an AmBe quasi-forward biased directional source

Source location of Special Nuclear Material (SNM) encompassing 95% 235 U and 239 Pu is identified by utilizing a directional source from Patent No: US20190013109A1 using Prompt Gamma Neutron Activation Analysis (PGNAA) and neutron spectroscopy simulated with Monte-Carlo N-Particle transport 6.2 (MCNP). BC-408, HPGe, LaBr 3 detector arrays were used to identify the location of the SNM using total counts incident on each detector, and PGNAA photopeaks from HPGe and LaBr 3 detector arrays in a polyethylene shield. The conducted simulations varied the volume and location of the SNM in the MCNP input files to observe how the source location method behaved. PGNAA photopeaks used for source identification include 61 keV from fission, 2.223 MeV prompt gamma from hydrogen, 511 keV annihilation, and a single and double escape peaks from the prompt gamma interaction from hydrogen. The capabilities of each detector systems to acquire well resolved photopeaks with a 1% relative error or less, and total relative error for F4 and F8 tallies were less than 0.015% relative error. Source predictions of the SNM with uneven amounts of polyethylene shielding between the source and detectors was observed to overpredict and give invalid source location predictions. Source locations of the SNM with even amounts of polyethylene material between the source and each detector were found to be valid. With a 1 Ci 241 Am source activity, it was determined that 1630 s were needed to obtain the results for each detector system with the quasi-forward directional AmBe source. Coupling source and material identification together would increase acquisition time but would only require one system to determine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Programmable bionanocomposite coated fertilizers for prolonged controlled release of nitrogen

Controlled-release fertilizers (CRFs) present a promising solution for alleviating food and nutrient scarcity. However, their development has been mainly hindered by both rapid and unsynchronized nutrient release and unsustainable coating materials. In this study, we address this issue by developing a new coating layer for CRFs using a programmable biopolyurethane nanocomposite. This nanocomposite is prepared from diphenylmethane diisocyanate (MDI)-functionalized bentonite nanoclay (BNT-MDI) and a biopolyol from biomass waste. The results show that the BNT-MDI-doped CRFs (BCRFs) exhibit an impressive nitrogen (N)-release longevity of approximately 120 days at a 4 wt% coating ratio, surpassing previous CRF formulations. In a 30-day snap bean cultivation study, BCRF significantly improved root length (1000%), leaf length (257%), leaf width (400%), and plant height (1400%) compared to the control. The superior performance of BCRF is attributed to the PU-nanoclay biocomposite film, with full nano-exfoliation, controllable porosity, and high crosslinking density. Furthermore, we introduce a new dynamic release mechanism and establish a quantitative relationship between the nanostructure, property, and release performance of BCRF by combining the multiplicative and diffusion models for porous materials. Finally, this study provides a theoretical framework and a straightforward methodology for designing programmable nanocomposite structures for future biobased CRFs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Properties and performance of lignin-based polyurethane foams from lignin and castor oil as synergistic bio-polyols

Lignin and castor oil with intrinsic hydroxyl groups are attractive green resources for polyurethane (PU) applications. However, lignin's heterogeneous and highly crosslinked structure, poor processability, as well as the feedstock variability, lead to inconsistent and poor performance of the final foam products. Castor oil-based polyurethane foam (PUF) has a relatively high price and density, which are big hurdles to its practical applications. Here, in this study, we hypothesized that synergistic bio-polyol mixtures composed of lignin and castor oil could balance the drawbacks from individual component. Castor oil could improve the dispersity of lignin, while lignin simultaneously addressed the issues caused by PUF prepared with castor oil, such as its high density and low thermal stability. For a comprehensive understanding of the effects of structural properties of lignin on its PUF processing and applications, various lignin fractions were isolated by co-solvent enhanced lignocellulosic fractionation (CELF) from different species, including hardwood, softwood, and herbaceous plants, and the processed lignins with different molecular weights were applied with castor oil. The lignin fractions with lower molecular weight showed good dispersity in castor oil with a high lignin content (up to 50 wt%) and completely replaced petroleum-based polyols. The produced foam with 50 wt% low-molecular-weight lignin fractions from woody biomass showed comparable/higher compressive strength (up to 20 psi) and thermal insulation performance (up to 5.69 R-value in −1 for 50 % L-Pine foam). In addition, this study revealed the relationship between lignin's structural properties and foam performance, providing insights for practical applications of lignin-based PUF.

Jeong, Soyeon [State Univ. of New York (SUNY), Syr↗

Investigation of process history and underlying phenomena associated with the synthesis of plutonium oxides using Vector Quantizing Variational Autoencoder

Accurate, high throughput, and unbiased analysis of plutonium oxide particles is needed for analysis of the phenomenology associated with process parameters in their synthesis. Compared to qualitative and taxonomic descriptors, quantitative descriptors of particle morphology through scanning electron microscopy (SEM) have shown success in analyzing process parameters of uranium oxides. Among other candidates, a neural network called a Vector Quantizing Variational Autoencoder (VQ-VAE) has shown the ability to quantitatively describe particle morphology to attain >85% accuracy in identifying uranium oxide processing routes. We utilize a VQ-VAE to quantitatively describe plutonium dioxide (PuO 2 ) particles created in a designed experiment and investigate their phenomenology and prediction of their process parameters. PuO 2 was calcined from Pu(III) oxalates that were precipitated under varying synthetic conditions that related to concentrations, temperature, addition and digestion times, precipitant feed, and strike order; the surface morphology of the resulting PuO 2 powders were analyzed by SEM. A pipeline was developed to extract and quantify useful image representations for individual particles with the VQ-VAE, then further reduce the dimensionality of the feature space using a bottlenecking neural network fit to perform multiple classification tasks simultaneously. The reduced feature space could predict process parameters with greater than 80% accuracies for some parameters with a single particle. They also showed utility for grouping particles with similar surface morphology characteristics together. Both the clustering and classification results reveal valuable information regarding which chemical process parameters chiefly influence the PuO 2 particle morphologies: strike order and oxalic acid feedstock. Doing the same analysis with multiple particles was shown to improve the classification accuracy on each process parameter over the use of a single particle, with statistically significant results generally seen with as few as four particles in a sample.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Group hexavalent actinide separation from lanthanides using sodium bismuthate chromatography

Advanced used nuclear fuel (UNF) reprocessing strategies are limited by the complex radiochemical separations and engineering required to achieve the separation of actinides (An) from neutron scavenging lanthanides (Ln). The accessibility of the hexavalent oxidation state for the actinides (U – Am) provides a pathway to achieving a group hexavalent actinide separation from the trivalent lanthanides and Cm. The solid oxidant and ion exchanger, sodium bismuthate (NaBiO 3 ), has been demonstrated to quantitatively oxidize and separate Am from trivalent Cm in a column chromatographic system. This work expands on the use of NaBiO 3 chromatography to characterize the adsorption, kinetic, and elution behavior of U, Pu, and Eu. Separation factors over 200 with rapid kinetics were observed at dilute nitric acid concentrations with a complete An/Ln separation achieved in under an hour. In conclusion, the adsorption and chromatographic behavior of key fission products present in various reprocessing raffinates was characterized which demonstrated potential application of a NaBiO 3 -based separation following a TRUEX process.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Accelerated impurity solver for DMFT and its diagrammatic extensions

Here, we present ComCTQMC, a GPU accelerated quantum impurity solver. It uses the continuous-time quantum Monte Carlo (CTQMC) algorithm wherein the partition function is expanded in terms of the hybridisation function (CT-HYB). ComCTQMC supports both partition and worm-space measurements, and it uses improved estimators and the reduced density matrix to improve observable measurements whenever possible. ComCTQMC efficiently measures all one and two-particle Green's functions, all static observables which commute with the local Hamiltonian, and the occupation of each impurity orbital. ComCTQMC can solve complex-valued impurities with crystal fields that are hybridized to both fermionic and bosonic baths. Most importantly, ComCTQMC utilizes graphical processing units (GPUs), if available, to dramatically accelerate the CTQMC algorithm when the Hilbert space is sufficiently large. We demonstrate acceleration by a factor of over 600 (100) in a simulation of δ-Pu at 600 K with (without) crystal fields. In easier problems, the GPU offers less impressive acceleration or even decelerates the CTQMC. Here we describe the theory, algorithms, and structure used by ComCTQMC in order to achieve this set of features and level of acceleration.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Radionuclide incorporation in negative thermal expansion α-Zr(WO 4 ) 2 : A density functional theory study

The incorporation of uranium, plutonium and technetium in the negative thermal expansion (NTE) α-Zr (WO 4 ) 2 has been investigated within the framework of density functional theory (DFT). It is found that the vacancy formation energies of the charged vacancies are overall larger than that of its counterpart neutral Frenkel defects and Schottky defects. DFT calculations suggest that U and Pu substitutions for the Zr site are preferred in α-Zr (WO 4 ) 2 . In case of Tc substitution, both Tc(IV) for the Zr site and Tc(VII) for the W site are considered under oxygen-poor and oxygen-rich conditions, while Tc(VII) substitution can be improved significantly by including Y 2 O 3 (charge compensation).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

From acetone fractionation to lignin-based phenolic and polyurethane resins

In this paper, acetone fractionation was used to increase the homogeneity of softwood kraft lignin for product development. The acetone soluble and insoluble fractions were analyzed in terms of elemental composition, chemical structure, and thermal properties. The phenolic hydroxyl content of the acetone soluble fraction increased by 24%. The acetone soluble fraction of kraft lignin was used to fully substitute phenol in phenolic resin formulation. The resulting formulated lignin-formaldehyde adhesive showed higher adhesion strength (4.3 MPa) compared to a lab formulated phenol-formaldehyde resin (3.4 MPa) with 100% wood failure after lap shear test. On the other hand, the acetone insoluble lignin fraction, which had 23% higher aliphatic hydroxyl content compared to the starting lignin, was used to entirely replace petroleum-based polyol in polyurethane resin formulation. Then a bio-derived solvent (dihydrolevoglucosenone, Cyrene) was used to dissolve the acetone insoluble lignin fraction to synthesize lignin-based polyurethane resin. Tailoring the structure of kraft lignin through solvent fractionation resulted in two fractions, which were used to replace 100% of two major petrochemicals (phenol and polyol) in the formulations of phenolic and PU resins, that would otherwise be challenging due to the heterogeneity of softwood kraft lignin.

36 MATERIALS SCIENCE↗

Effects of flow on uranium speciation in soils impacted by acidic waste fluids

Radioactive acidic liquid waste is a common byproduct of uranium (U) and plutonium (Pu) enrichment and recycling processes whose accidental and planned release has led to a significant input of U into soils and sediments across the world, including at the U.S. DOE's Hanford site (WA, USA). Because of the particularly hazardous nature of U, it is important to predict its speciation when introduced into soils and sediments by acidic waste fluids. Of fundamental importance are the coupled effects of acid-driven mineral transformation and reactive transport on U speciation. To evaluate the effect of waste-fluid residence time and co-associated dissolved phosphate concentrations on U speciation in impacted soils and sediments, uncontaminated surface materials (from the Hanford Site) were reacted with U-containing synthetic acidic waste fluids (pH 2) amended with dissolved phosphate concentrations in both batch (no flow) and flow-through column systems for 7–365 days. By comparing dissolved U behavior and solid phase speciation as a function of flow regimen, we found that the availability of proton-promoted dissolution products (such as Si) to sequester U into uranyl silicates was dependent on waste fluid-sediment contact time as uranyl silicates were not detected in short contact time flow-through systems but were detected in no-flow, long contact time, reactors. Moreover, the dominance of uranyl phosphate as neoprecipitate U scavenger (principally in the form of meta-ankoleite) in phosphate amended systems confirmed the importance of phosphate amendments for an efficient sequestration of U in the soils and sediments. Overall, our experiments suggest that the formation of uranyl silicates in soils impacted by acidic waste fluids is likely to be limited unless reaction products are allowed to accumulate in soil pores, highlighting the importance of investigating soil U speciation in flow-through, transport-driven systems as opposed to no-flow, batch systems. Finally, this study provides insights into uranium speciation and its potential changes under acidic conditions for better prediction of risks and subsequent development of efficient remediation strategies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗