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At least 1,495 records · Page 83

Assessment of Flow-Enhanced Sensors for Actinide Quantification in MSRs

This report serves as the deliverable for Milestone M2RS-22AN0401062 that is part of Work Package RS-22AN040106 (Flow Enhanced Sensors for MSRs – ANL). The goal of this milestone is to assess the capabilities of flow-enhanced electrochemical sensors (FEES) to quantify actinides in molten salt reactors. Flow enhanced electrochemical sensors are a type of electroanalytical sensor that has been developed at Argonne National Laboratory to be installed directly into MSR flow conduits in order to make measurements of the salt composition. These sensors represent a significant improvement in capabilities compared to earlier electroanalytical sensors that instead can only be operated in quiescent conditions. To support this work, Argonne constructed a molten salt flow system to serve as a testbed for the development of safeguards and process monitoring-relevant sensors in challenging molten salt flow conditions. Through extensive flow testing using UCl3-bearing salts, Argonne has been able to show that the FEES are able to make good measurements of salt composition. Concentration measurements with a mean absolute error of 0.09 wt% have been achieved for representative fuel salt mixtures across a range of UCl3 loadings. Repeatability was also good, with the relative standard deviation from repeated measurements being less than 1.0%. These sensors have also been shown to be able to measure the flow rate of the salt within the flow system’s transfer line. Although the accuracy of the sensors has been good, the sensors have thus far not been able to achieve performance good enough to satisfy the nuclear material accountancy requirements in 10 CFR 74. To do so, accuracy levels of 0.1% must be achieved; the FEES when operated in Argonne’s flow system have so far only been able to achieve relative errors of approximately 5.0%. Much of the error that has been observed at this stage is due to challenges in maintaining a stable salt composition in the molten salt flow system, and it is not believed that there are any inherent flaws in the sensor design. Nonetheless, the high degree of accuracy required by 10 CFR 74 represents a significant challenge, and further design evolution and integration of the sensors into multimodal sensing frameworks will likely be needed to push the measurement accuracy to the needed level.

Moore, Colin E.↗

Fission Product Quantification and Burnup Analysis via Gamma Spectrometry of the AGR-5/6/7 TRISO Fuel Experiment

Five capsules containing varying configurations of TRISO fuel compacts were irradiated in the most recent Advanced Gas Reactor (AGR) TRISO test campaign, AGR-5/6/7. As part of the post-irradiation examination (PIE) of this work all the fuel compacts and capsule graphite holders were measured with the Precision Gamma Scanner (PGS) to determine isotopic activities and locations using gamma spectrometry. Measuring the compacts allowed for the comparison of physics model depletion calculations with the measured compact activity to validate models. These measurements also are used to find compacts of interest with low fission product retention that may be tested in subsequent PIE. Measurements of the holders can confirm fission product distribution and migration. Of the isotopes measured, Cs-137 and Cs-134 were used to estimate location of failed particles as well as determine a measured burnup estimation. Results from Capsule 1 compacts and the holder indicate many fuel particle failures occurred. There are high amounts of cesium in the holder near Stack 9 of Capsule 1 that corresponds to low fractions?measured-to-calculated (M/C) ratio?of cesium remaining in those compacts. All other capsules had cesium retention ratios near 1. The isotope 110mAg had less consistent results. Capsule 2 compacts exhibited a M/C of 0.20, much lower than anticipated for the temperatures these compacts underwent. Capsule 3 experienced much higher temperatures, >1300C and had an average M/C of 0.75. These are the opposite results than what was predicted by past AGR experiments for the relationship between temperature and isotope retention. Capsule 4 and 5 showed good fission product retention and agreement with the physics model predictions. The burnup results from the PGS measurements showed strong agreement between the physics models and the measured values. Using a ratio of Cs-134/Cs-137 to calculate the burnup match closely with the physics models. Additionally, the Cs-137 burnup results were less accurate but extremely close to the model results.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Role of Uncertainty Quantification in the Explainability of Large Language Models for the Nuclear Industry

The meteoric rise of generative artificial intelligence (AI) large language models (LLMs) has created an opportunity to utilize them to increase efficiencies in a multitude of industries. While LLMs carry great potential to revolutionize the manner in which work is performed, numerous known deficiencies limit their utility, including the black box nature of the models, the stochastic nature of the response (i.e., presenting the same prompt multiple times results in different responses), and the potential for hallucination. Widespread adoption of LLMs in safety-critical industries such as nuclear will require some form of explainability to assure end users that the LLM’s response to a given query is valid. Model uncertainty is inherently linked to the concepts of trust and explainability, and can be used to identify situations in which the model is insufficiently certain about its answer. Although uncertainty is not enough in and of itself to determine the suitability of an answer—a model can be very certain of an inaccurate answer—it still provides valuable supporting information. Practical methodologies for gauging or quantifying the uncertainty in LLM outputs are presented herein, along with examples based on nuclear-specific prompts.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗

Uncertainty quantification in MELCOR Safety analysis of ARIES reactor designs

MELCOR-TMAP is a combined thermal-hydraulics and tritium tracking code developed to simulate severe accident scenarios in fission and fusion power plants. Here, we demonstrate the results of MELCOR-TMAP analyses on historical ARIES program reference designs. By coupling MELCOR-TMAP with the open source RAVEN probabilistic risk analysis framework’s Bayesian UQ capabilities, we also demonstrate key uncertainties in material properties with the highest impact on tritium inventory and plant risk.

70 - PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Experimental Covariance Determination for Critical Integral Experiments

Integral benchmarks for criticality safety and nuclear data validation require expensive uncertainty quantification studies. In general, uncertainty quantification techniques ignore correlations between experiments and shared parts. Experiments, such as the TEX (Thermal/Epithermal eXperiments) campaigns, consist of many shared parts, such as the ‘Jemima’ HEU fuel plates, which create a strong correlation in their uncertainties. While these correlations are known to exist, they are often not estimated due to the complexity of such calculations. This paper describes an intuitive method of determining the covariance for each of the experimental components, providing a correlation for each family of parts across the multiple cases examined within a benchmark. A proof-of-principle study using the TEX-HEU experimental campaign was performed and verified that the correlations can be calculated with information commonly found in the ICSBEP (International Criticality Safety Benchmark Evaluation Project) benchmarks. This study showed that the introduction of model and experimental covariances reduces the χ 2 per degree of freedom from 2.203 to 1.179, indicating that the omission causes overly pessimistic bias quantifications. This technique can be seamlessly integrated to current benchmark evaluations as well as reevaluations of legacy benchmarks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Block Design with Common Reference Samples Enables Robust Large-Scale Label-Free Quantitative Proteome Profiling

Label-free quantitative proteomics has become an increasingly popular tool for profiling global protein abundances. However, one major weakness is the potential performance drift of the LC-MS platform over time, which in turn limits its utility for analyzing large-scale sample sets. To address this, in this work we introduce an experimental and data analysis scheme based on a block-design with common controls within each block for enabling LC-MS-based large-scale label-free quantification. In this scheme, a large number of samples (e.g., >100 samples) are analyzed in smaller, and more manageable blocks, minimizing instrument drift and variability within a block. Furthermore, each designated block also contains common controls (or reference) samples for normalization within and across blocks. We demonstrated the effectiveness of this method by profiling the proteome response of human macrophage THP-1 cells to 11 engineered nanomaterials (ENMs) at two different doses. A total of 116 samples were analyzed in six blocks, yielding an average coverage of 4500 proteins per sample. The data revealed consistent quantification of proteins across all six blocks, as shown by highly stable quantification of house-keeping proteins in all samples and high levels of quantification correlation among samples from different blocks. The data also demonstrated that label-free quantification is robust and accurate enough to quantify even very subtle abundance changes as well as large fold-changes without potential ratio compression as often encountered with isobaric labeling. Our streamlined workflow is easy to implement and can be readily adapted to other large cohort studies for reproducible label-free proteome quantification.

59 BASIC BIOLOGICAL SCIENCES↗

Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements

Hot carriers in plasmonic nanostructures, generated via plasmon decay, play key roles in applications such as photocatalysis and in photodetectors that circumvent bandgap limitations. However, direct experimental quantification of steady-state energy distributions of hot carriers in nanostructures has so far been lacking. We present transport measurements from single-molecule junctions, created by trapping suitably chosen single molecules between an ultrathin gold film supporting surface plasmon polaritons and a scanning probe tip, that can provide quantification of plasmonic hot-carrier distributions. Our results show that Landau damping is the dominant physical mechanism of hot-carrier generation in nanoscale systems with strong confinement. The technique developed in this work will enable quantification of plasmonic hot-carrier distributions in nanophotonic and plasmonic devices.

Science & Technology - Other Topics↗