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At least 937 records · Page 52

Quantification of UV-Visible and Laser Spectroscopic Techniques for Materials Accountability and Process Control

Ultraviolet–visible spectroscopy (UV–Visible) and time-resolved laser fluorescence spectroscopy (TRLFS) optical techniques can permit on-line analysis of actinide elements in a solvent extraction process in real time. These techniques have been used for measuring actinide speciation and concentration under laboratory conditions and are easily adaptable to multiple sampling geometries, such as dip probes, fiber-optic sample cells, and flow-through cell geometries. To fully exploit these techniques, researchers must determine the fundamental speciation of target actinides and the resulting influence on spectroscopic properties. Detection limits, process conditions, and speciation of key actinide components can be established and utilized in a range of areas, particularly those related to materials accountability and process control. Through this project, researchers will develop tools and spectroscopic techniques to evaluate solution extraction conditions and concentrations of U, Pu, and Cm in extraction processes, addressing areas of process control and materials accountability. The team will evaluate UV– Visible and TRLFS for use in solvent extraction-based separations. Ongoing research is examining efficacy of UV-Visible spectroscopy to evaluate uranium and plutonium speciation under conditions found in the UREX process and using TRLFS to evaluate Cm speciation and concentration in the TALSPEAK process. A uranyl and plutonium nitrate UV–Visible spectroscopy study met with success, which supports the utility and continued exploration of spectroscopic methods for evaluation of actinide concentrations and solution conditions for other aspects of the UREX+ solvent extraction scheme. This project will examine U and Pu absorbance in TRUEX and TALSPEAK, perform detailed examination of Cm in TRUEX and TALSPEAK, study U laser fluorescence, and apply project data to contactors. The team will also determine peak ratios as a function of solution concentrations for the UV-Visible spectroscopy studies. The use of TRLFS to examine Cm and U will provide data to evaluate lifetime, peak location, and peak ratios (mainly for U). The bases for the spectroscopic techniques have been investigated, providing fundamental evidence for the application’s utility.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tracking the Sun 10: The Installed Price of Residential and Non-Residential Photovoltaic Systems in the United States

Berkeley Lab’s Tracking the Sun report series is dedicated to summarizing trends in the installed price of grid-connected, residential and non-residential systems solar photovoltaic (PV) systems in the United States. The present report, the tenth edition in the series, focuses on systems installed through year-end 2016, with preliminary data for the first half of 2017. The report provides an overview of both long-term and more-recent trends, highlighting key drivers for installed price declines over different time horizons. The report also extensively characterizes the widespread variability in system pricing, comparing installed prices across states, market segments, installers, and various system and technology characteristics. The trends described in this report derive from project-level data collected by state agencies and utilities that administer PV incentive programs, solar renewable energy credit (SREC) registration systems, or interconnection processes. In total, data for this report were compiled and cleaned for more than 1.1 million individual PV systems, though the analysis in the report is based on a subset of that sample, consisting of roughly 630,000 systems with available installed price data. The full underlying dataset of project-level data (excluding any confidential information) is available in a public data file, for use by other researchers and analysts.

14 SOLAR ENERGY↗

Assembly and Testing of a Tritium and Iodine Removal System for Use with Advanced Tritium Pretreatment

US regulations will require the removal of iodine and tritium, along with other volatile and semivolatile radionuclides, from the off-gas streams of nuclear fuel reprocessing plants. Tritium pretreatment is a head-end operation that could be incorporated within nuclear fuel reprocessing plants for the upfront removal and trapping of these volatiles species. Quantitative, up-front removal in a single compact system is of significant advantage because otherwise tritium and iodine distributes to other unit operations, each of which have associated off-gas streams also requiring treatment. Oak Ridge National Laboratory is presently developing an advanced tritium pretreatment process based on the oxidation of used nuclear fuel at low temperature using NO 2 /O 2 mixtures, which produces a fine powder. This process can result in the quantitative volatilization of both tritium and iodine. The powder product can be selected to be U 3 O 8 , UO 3 , or a nitrate by adjusting the processing conditions and the process can be readily interfaced to either conventional aqueous-based or advanced pyrochemical–based reprocessing plants. In preparation for a planned kilogram-scale hot cell demonstration of the advanced tritium pretreatment process with used nuclear fuel (UNF), an integrated iodine and tritium capture system was designed and assembled. Three experimental runs of this system were completed successfully. All the samples were submitted for analysis. The results and data analysis will be covered in a subsequent report to be issued by the Off-Gas Sigma Team. Several additional tests should be undertaken to provide additional information on the system’s performance. The objectives for the additional tests and test conditions are presented in this report.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Demonstration of the Coating Analysis Capabilities in BISON

In order to improve the accident tolerance of light water reactor (LWR) fuel, coated cladding materials have been proposed which exhibit much slower oxidation kinetics in high-temperature steam than Zr-alloys. This behavior should decrease the energy release due to oxidation and allow the cladding to remain integral longer in the presence of high-temperature steam, making accident mitigation more likely. In order to determine how these coating materials will adjust the behavior of the Zr-alloy cladding during normal reactor operation, simulations have been performed using the Bison fuel performance code. This analysis focused on modeling and comparing the integral thermo-mechanical performance of coated and uncoated zircaloy cladding with uranium dioxide fuel under normal operating conditions. This analysis demonstrates the ability to model a discrete meshed coating bonded to the cladding exterior and provides a comparison with an uncoated fuel rod. A generic range of coating material properties are implemented given the differences and unknowns regarding the proprietary coating properties used by the vendors. A main-effects analysis was performed to identify trends and sensitivities in how coating material properties affect key fuel performance metrics. Lastly, because residual stresses are expected to form in the coating, arising from the high temperature coating application process and application techniques, an additional analysis was performed to identify the impact of these stresses on the cladding behavior. Future analysis efforts will target more comprehensive documentation of this main effects analysis by sampling the results at the beginning and middle-of-life in order to capture important behavior before and during the onset of gap closure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Arctic Mixed-Phase Cloud Base Ice Precipitation Properties During the M-PACE Field Campaign

Cloud-climate feedbacks are still the greatest source of uncertainty in current climate projections. Arctic clouds, which are predominantly stratiform and supercooled, often long-lived, and nearly-continuously precipitate ice particles, contribute roughly 10% of the uncertainty attributed to the global cloud feedback. This Arctic cloud uncertainty is driven by incomplete observational and theoretical knowledge required to estimate and explain the state and active processes occurring in those clouds. A focus on ice precipitation properties at Arctic cloud base rather than the surface deconfounds the product of cloud condensate sink processes from the influence of the atmospheric thermodynamic state below cloud base, rendering cloud-base properties a more appealing target for inference and evaluation of model simulations. This dataset provides a set of 25 samples from the M-PACE field campaign, all of which were retrieved using the synthesis of ARM radar and lidar measurements. The retrieved ice precipitation variables in this dataset include, among others, the ice number concentration, water content, PSD parameters, precipitation rate, mass-weighted fall velocity, vertical air motion, and effective radius, all of which are highly valuable for model evaluation and a general understanding of polar cloud sink processes. Each variable sample includes its mean value and associated uncertainty. Additional variables based on ARM measurements (liquid layer statistics, etc.) are included in this dataset as well. The retrieval algorithm and analysis of this dataset are described in Silber (JGR, 2023, https://doi.org/10.1029/2022JD038202).

54 ENVIRONMENTAL SCIENCES↗

A Control Chart Approach for Representing and Mining Data Streams with Shape Based Similarity

The mining of data streams for online condition monitoring is a challenging task in several domains including (electric) power grid system, intelligent manufacturing, and consumer science. Considering a power grid application in which thousands of sensors, called the phasor measurement units, are deployed on the power grid network to continuously collect streams of digital data for real-time situational awareness and system management. Depending on design, each sensor could stream between ten and sixty data samples per second. The myriad of sensory data captured could convey deeper insights about sequence of events in real-time and before major damages are done. However, the timely processing and analysis of these high-velocity and high-volume data streams is a challenge. Hence, a new data processing and transformation approach, based on the concept of control charts, for representing sequence of data streams from sensors is proposed. In addition, an application of the proposed approach for enhancing data mining tasks such as clustering using real-world power grid data streams is presented. The results indicate that the proposed approach is very efficient for data streams storage and manipulation.

big data↗

Assessment and Non-Destructive Evaluation of the Influence of Residual Solvent on a Two-Part Epoxy-Based Adhesive Using Ultrasonics

Polymers are increasingly being used in higher demanding applications due to their ability to tailor the properties of structures while allowing for a weight and cost reduction. Solvents play an important role in the manufacture of polymeric structures since they allow for a reduction in the polymer’s viscosity or assist with the dispersion of fillers into the polymer matrix. However, the incorrect removal of the solvent affects both the physical and chemical properties of polymeric materials. The presence of residual solvent can also negatively affect the curing kinetics and the final quality of polymers. Destructive testing is mainly performed to characterize the properties of these materials. However, this type of testing involves using lab-type equipment that cannot be taken in-field to perform in situ testing and requires a specific sample preparation. Here, a method is presented to non-destructively evaluate the curing process and final viscoelastic properties of polymeric materials using ultrasonics. In this study, changes in longitudinal sound speed were detected during the curing of an aerospace epoxy adhesive as a result of variations in polymer chemistry. To simulate the presence of residual solvent, samples containing different weight percentages of isopropyl alcohol were manufactured and tested using ultrasonics. Thermogravimetric analysis was used to show changes in the decomposition of the adhesive due to the presence of IPA within the polymer structure. Adding 2, 4, and 6 wt.% of IPA decreased the adhesive’s lap shear strength by 40, 58, and 71%, respectively. Ultrasonics were used to show how the solvent influenced the curing process and the final sound speed of the adhesive. Young’s modulus and Poisson’s ratio were determined using both the longitudinal and shear sound speeds of the adhesive. Using ultrasonics has the potential to non-invasively characterize the quality of polymers in both an in-field and manufacturing settings, ensuring their reliability during use in demanding applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Lower Temperature Annealing of Vapor Diffused Nb₃Sn for Accelerator Cavities

Nb₃Sn is a next-generation superconducting material for the accelerator cavities with higher critical temperature and superheating field, both twice compared to Nb. It promises superior performance and higher operating temperature than Nb, resulting in significant cost reduction. So far, the Sn vapor diffusion method is the most preferred and successful technique to coat niobium cavities with Nb₃Sn. Although several post-coating techniques (chemical, electrochemical, mechanical) have been explored to improve the surface quality of the coated surface, an effective process has yet to be found. Since there are only a few studies on the post-coating heat treatment at lower temperatures, we annealed Nb₃Sn-coated samples at 800 C - 1000 C to study the effect of heat treatments on surface properties, primarily aimed at removing surface Sn residues. This paper discusses the systematic surface analysis of coated samples after annealing at temperatures between 850 C and 950 C.

43 PARTICLE ACCELERATORS↗

Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS

The ability to directly measure uranium isotope ratios on environmental swipes has been achieved through a solution-based microextraction process and represents a significant advancement toward the development of a rapid method to analyze international nuclear safeguard samples. Here, a microextraction probe is lowered and sealed onto the swipe surface, and analytes within the sampling site (~8 mm2) are dissolved and extracted into a flowing solvent of 2% nitric acid (HNO 3 ). The mobilized species are subsequently directed into an inductively coupled plasma-mass spectrometer (ICP-MS) for accurate and precise isotope ratio determination. This work highlights the novelty of the sampling mechanism, particularly with the direct coupling of the microextraction probe to the ICP-MS and measurement of uranium isotope ratios. The preliminary method detection limit for the microextraction-ICP-MS method, utilizing a quadrupole-based MS, was determined to be ~50 pg of 238 U. Additionally, precise and accurate isotope ratio measurements were achieved on uranium reference materials for both the major ( 235 U/ 238 U) and minor ( 234 U/ 238 U and 236 U/ 238 U) ratios. While the present work is focused on directly measuring uranium isotopic systems on swipe surfaces for nuclear safeguards and verification applications, the benefits would extend across many applications in which direct solid sampling is sought for elemental and isotopic analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

CFD Analysis of RLUOB Zone 1 HEPA Filter Plenum and Testing Manifolds

The purpose of this computational fluid dynamics (CFD) analysis is to ensure that Camfil Farr’s upstream and downstream injection and sampling manifolds can meet or exceed the requirements outlined in the ASME AG-1 1997 a(2000) Code on Nuclear Air and Gas Treatment for the testing of HEPA and adsorbent filters. This paper will present a numerical simulation of airflow in the Radiological Laboratory Utility Office Building (RLUOB) zone 1 HEPA filter plenum and testing manifolds using the commercial CFD software ANSYS FLUENT 2020R1. The CFD analysis focuses on the investigation of the air flow distribution and air-aerosol mixing uniformity. The evaluation was done for all steps of the modeling process: grid generation, physics setup, simulation, and post-processing. The mass flow rate in each section of the zone 1 injection and sampling manifolds is also reported.

42 ENGINEERING↗

Tuning the Magnetic Properties of ZnFe{sub 2}O{sub 4} Nanoparticles Through Partial Doping and Annealing

The aim of this study was to investigate the effect of annealing temperature and cobalt cation (Co{sup 2+}) doping on the magnetic properties of zinc ferrite (ZFO) nanoparticles. The nanoparticles were prepared through sol-gel combustion process with citric acid as the fuel. The obtained nanoparticles were annealed at several temperatures from 300 to 1000 °C for 2 h. Spinel formation was proved by X-ray diffraction (XRD) patterns, and the average crystallite size in all samples was estimated between 22 and 32 nm. It is worthwhile to mention that Fe{sub 2}O{sub 3} and ZnO are detected as the medium phases. Meanwhile, Fe{sub 2}O{sub 3} phase transformation to the other allotropes has happened around 400 °C and was characterized via the simultaneous thermal analysis (STA) and XRD. For higher annealing temperatures, diffusion has gradually been completed and, finally, the single phase of spinel structure was prepared at 1000 °C. In addition, field-emission scanning electron microscopy (FESEM) images revealed that the nanoparticle size after annealing was between 30 and 200 nm for the whole samples. The formation of the spinel phase was considered the most important factor on the magnetic properties of ZFO. Cobalt doping, annealing temperature, and also Fe{sub 2}O{sub 3} phase were the main factors on changing magnetic properties. Paramagnetic nanoparticles with higher coercivity for doped samples rather than un-doped samples have been obtained.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Application of the Uranium–Helium Chronometer to the Analysis of Nuclear Forensic Materials

Radiochronometers are used to constrain the manufacturing and processing history of actinide materials for nuclear forensic investigations. This paper describes here U–He ages and He diffusion kinetics obtained from a metallic, highly enriched uranium sample. The average U–He age is 8% older than the known casting date, which indicates that excess He is present and is likely due to incomplete degassing of pre-existing He during the casting process. Although the U–He age is older than expected, the accuracy is comparable to other chronometers that have been applied to this material. Diffusion kinetics obtained from the uranium metal indicate that He is quantitatively retained under plausible storage conditions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Extreme-Scale Distribution-Based Data Analysis

Scientists overview and identify regions of interest by transforming data into compact information descriptors that characterize simulation results and allow detailed analysis on demand. Among many existing feature descriptors, statistical information derived from data samples is a promising approach to taming the big data avalanche because data distributionscomputed from a population can compactly describe the presence and characteristics of salient data features with minimal data movement. The ability to computationally summarize and process data using distributions also provides an efficient and representative capture of information that can adjust to size and resource constraints, with the added benefit that uncertainty associated with results can be quantified and communicated. In this project, we have developed a distribution-based data analysis and visualization framework for optimizing in situ processing and analysis of extreme-scale scientific data.

97 MATHEMATICS AND COMPUTING↗

Sensitivity analysis, surrogate modeling, and optimization of pebble-bed reactors considering normal and accident conditions

This research provides a valuable tool that streamlines the optimization process while significantly increasing its accuracy. This study creates a robust framework for reactor design optimization by incorporating comprehensive modeling using the Comprehensive Reactor Analysis Bundle, or BlueCRAB, within the Multiphysics Object-Oriented Simulation Environment (MOOSE). BlueCRAB is the United States Nuclear Regulatory Commission's code suite for non-light water reactor analysis and includes the Griffin, Pronghorn, and Bison applications. This not only improves the efficiency of the optimization process but also enhances the reliability of the results. Such a tool is essential for advancing the state-of-the-art in pebble-bed reactor technology and is critical for achieving the goals of Generation IV reactors, which aim for safe, sustainable, and economically viable nuclear energy solutions. This work presents and applies this workflow on pebble-bed reactors while considering both normal and off-normal conditions. A representative gas-cooled pebble-bed reactor at equilibrium core conditions serves as the nominal design specification for normal operation and is based on previous research. The depressurized loss-of-forced-cooling accident is deployed for off-normal conditions in this work. After defining design-related parameters and quantities of interest regarding reactor safety and performance, this multiphysics model is sampled using the MOOSE stochastic tools module. The result is a comprehensive dataset of configurations, enabling sensitivity analysis and the generation of surrogate models. Subsequently, the dataset and surrogate models are employed in two optimization studies aimed at maximizing fuel utilization and economic profit while adhering to safety and operational constraints. Performing the optimization process with fuel utilization as the metric leads to an improvement of approximately 10%, compared to engineering-judgment-based nominal conditions. The optimization on economic profit leads to an estimated increase of ~300 million USD over the lifetime of the reactor.

97 MATHEMATICS AND COMPUTING↗

Automated instant labeling chemistry workflow for real-time monitoring of monoclonal antibody N -glycosylation

With the transition toward continuous bioprocessing, process analytical technology (PAT) is becoming necessary for rapid and reliable in-process monitoring during biotherapeutics manufacturing. Bioprocess 4.0 is looking to build end-to-end bioprocesses that include PAT-enabled real-time process control. This is especially important for drug product quality attributes that can change during bioprocessing, such as protein N-glycosylation, a critical quality attribute for most monoclonal antibody (mAb) therapeutics. Glycosylation of mAbs is known to influence their efficacy as therapeutics and is regulated for a majority of mAb products on the market today. Currently, there is no method to truly measure N-glycosylation using on-line PAT, hence making it impractical to design upstream process control strategies. We recently described the N-GLYcanyzer workflow: an integrated PAT unit that measures mAb N-glycosylation within 3 hours of automated sampling from a bioreactor. Here, we integrated Agilent's Instant Procainamide (InstantPC) based chemistry workflow into the N-GLYcanyzer PAT unit to allow for nearly 10× faster near real-time analysis of mAb glycoforms. Furthermore, our methodology is explained in detail to allow for replication of the PAT workflow as well as present a case study demonstrating the use of this PAT to autonomously monitor a mammalian cell perfusion process at the bench scale to gain increased knowledge of mAb glycosylation dynamics during continuous biologics manufacturing using Chinese hamster ovary (CHO) cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Wet-chemical etching of FIB lift-out TEM lamellae for damage-free analysis of 3-D nanostructures

Reducing ion beam damage from the focused ion beam (FIB) during fabrication of cross sections is a well-known challenge for materials characterization, especially cross sectional characterization of nanostructures. To address this, a new method has been developed for cross section fabrication enabling high resolution transmission electron microscopy (TEM) analysis of 3-D nanostructures free of surrounding material and free of damage detectable by TEM analysis. Before FIB processing, nanopillars are encapsulated in a sacrificial oxide which acts as a protective layer during FIB milling. Furthermore, the cross sectional TEM lamella containing the nanopillars is then mounted and thinned with some modifications to conventional FIB sample preparation that provide stability for the lamella during the following wet-chemical dip etch. The wet-chemical etch of the TEM lamella removes the sacrificial oxide layer, freeing the nanopillars from any material that would obscure TEM imaging. Both high resolution TEM and aberration corrected scanning TEM images of Si/SiGe pillars with diameters down to 30 nm demonstrate the successful application of this approach.

3-d nanostructure analysis↗

Laser Driven Hydrothermal Processing (LDHP) for Rapid Dissolution of Glassy Nuclear Debris

Discovered in 2009 on the SLAB laser system at LLNL, Laser-Driven Hydrothermal Processing (LDHP) both spalls and transiently dissolves a wetted surface (e.g., rock, concrete, paint) when that surface is struck by a laser beam pulse under specific conditions. Previous projects have explored the application of LDHP to expediting sample dissolution for post-detonation nuclear forensics. Early results were very promising, indicating that this method could decrease material dissolution time by a factor of 10 or more. However, the large and complicated lasers previously used are impractical for this application. Under the R^3 venture we aimed to benchmark the LDHP capabilities of turn-key commercial off-the-shelf (COTS) lasers, and to establish how this process could be integrated into an analytical workflow for nuclear forensic analysis. We demonstrated that geological rock standards could be quickly processed into fine powder by LDHP followed by complete acid digestion in 15 minutes, without elemental fractionation that would skew analytical results. We determined that the COTS laser can be used for LDHP that could potentially reduce dissolution time for solid nuclear debris samples in post detonation nuclear forensics. One downside to this approach, however, is that the laser interactions are different with every material, so extensive method validation would be required for all likely material compositions. The LDHP processing rates of several materials were tested and determined to be favorable in the beginning with significant slowdown due to particulate scattering. This could be mitigated either by stopping and centrifuging the sample at specific intervals, or through design of a continuous solvent flow through mechanism.

36 MATERIALS SCIENCE↗

Evaluation of Digital Image Recognition Methods for Mass Spectrometry Imaging Data Analysis

Analyzing mass spectrometry imaging data can be laborious and time consuming, and as the size and complexity of datasets grow, so does the need for robust automated processing methods. We here present a method for comprehensive, semi-targeted discovery of molecular distributions of interest from mass spectrometry imaging data, using widely available image similarity scoring algorithms to rank images by spatial correlation. A fast and powerful batch search method using a MATLAB implementation of structural similarity (SSIM) index scoring with a pre-selected reference distribution is demonstrated for two sample imaging datasets, a plant metabolite study using Artemisia annua leaf, and a drug distribution study using maraviroc-dosed macaque tissue. .

97 MATHEMATICS AND COMPUTING↗