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At least 91 records · Page 5

Compaction of crushed salt for safe containment – a summary of the KOMPASS projects

Abstract. For the underground disposal of high-level nuclear waste in rock salt formations, the safety concept includes the backfilling of open cavities with crushed salt. For the prognosis of the sealing function of the backfill for the safe containment of the radioactive waste, it is crucial to have a comprehensive process understanding of the crushed-salt compaction behavior. The crushed-salt compaction process is influenced by internal properties (e.g., grain size, mineralogy, and moisture content) and boundary conditions (e.g., temperature, stress state, and compaction rate) and, therefore, involves several coupled thermal–hydro–mechanical (THM) processes (Hansen et al., 2014; Kröhn et al., 2017). With the paradigm shift from the limited release of radionuclides to safe containment due to the German Repository Site Selection Act passed in 2017, the importance of crushed salt as geotechnical barrier has increased, with a focus on the evolution of its hydraulic properties. Based on the knowledge gaps in the current process understanding, the “Compaction of crushed salt for safe containment” (KOMPASS) projects were initiated to improve the scientific basis behind using crushed salt for the long-term isolation of high-level nuclear waste within rock salt repositories. The efforts to improve the prediction of crushed-salt compaction begun during the first phase of the KOMPASS projects (Czaikowski et al., 2020) and were followed up in a second phase ending in June 2023. The primary achievements of the projects are as follows (Czaikowski et al., 2020; Friedenberg et al., 2022): specification of the KOMPASS reference material, an easily available and reproducible synthetic crushed-salt material, for generic investigations; development of pre-compaction methods and successful production of samples in the short term and under in situ loading conditions; formulation of an extended laboratory program addressing the isolated investigation of known relevant factors influencing the compaction behavior of crushed salt (Düsterloh et al., 2022); execution of long-term compaction tests addressing isotropic and deviatoric load changes, temperature, and compaction state; construction of a backfill body using the KOMPASS reference material in the Sondershausen mine through collaboration with the SAVER (Entwicklung eines salzgrusbasierten Versatzkonzepts unter der Option Rückholbarkeit) project (Schaarschmidt and Friedenberg, 2022); advancement of the tools for microstructure investigation methods (Svensson and Laurich, 2022); generation (first stages) of a microphysical process list combining literature research with our own findings; benchmarking of long-term compaction test for model development and optimization of various existing models as well as the development of new models; application of a virtual demonstrator (2D model representing a backfilled drift in rock salt) for the visualization of developments and the quantification of the models (Rabbel, 2022). In summary, the KOMPASS projects contributed to the reduction of uncertainties and the strengthening of the safety case for using crushed salt within rock salt repositories.

Friedenberg, Larissa↗

In situ microstructural evolution in face-centered and body-centered cubic complex concentrated solid-solution alloys under heavy ion irradiation

This study characterizes the microstructural evolution of single-phase complex concentrated solid-solution alloy (CSA) compositions under heavy ion irradiation with the goal of evaluating mechanisms for CSA radiation tolerance in advanced fission systems. Three such alloys, Cr 18 Fe 27 Mn 27 Ni 28 , Cr 15 Fe 35 Mn 15 Ni 35 , and equimolar NbTaTiV, along with reference materials (pure Ni and E90 for the Cr-FeMnNi family and pure V for NbTaTiV) were irradiated at 50 K and 773 K with 1 MeV Kr ++ ions to various levels of displacements per atom (dpa) using in-situ transmission electron microscopy. Cryogenic irradiation resulted in small defect clusters and faulted dislocation loops as large as 12 nm in face-centered cubic (FCC) CSAs. With thermal diffusion suppressed at cryogenic temperatures, defect densities were lower in all CSAs than in their less compositionally complex reference materials indicating that point defect production is reduced during the displacement cascade stage. High temperature irradiation of the two FCC CSA resulted in the formation of interstitial dislocation loops which by 2 dpa grew to an average size of 27 nm in Cr 18 Fe 27 Mn 27 Ni 28 and 10 nm in Cr 15 Fe 35 Mn 15 Ni 35 . This difference in loop growth kinetics was attributed to the difference in Mn-content due to its effect on the nucleation rate by increasing vacancy mobility or reducing the stacking-fault energy.

36 MATERIALS SCIENCE↗

Total metals, carbon, nitrogen & anion concentration data; Slate River & East River floodplains, Crested Butte, CO; May 2022-October 2022

This data package includes processed and undiluted measurements for metal, total carbon, total nitrogen, and anion concentrations from pore water (groundwater) and surface water samples from the Slate River and East River floodplains of Crested Butte, CO, focus field sites for the SLAC Floodplain Hydro-Biogeochemistry SFA. The data was generated as part of the work targeting the overarching research question for the SLAC SFA: How do ubiquitous subsurface interfaces mediate molecular-scale biogeochemical processes and groundwater quality in floodplains and watersheds? Samples were collected between May and October of 2022. These measurements were all recorded at the Arizona Laboratory for Emerging Contaminants (ALEC) at the University of Arizona located in Tucson, AZ. Groundwater samples were extracted from a network of installed rhizon (Rhizosphere Research Products, part no. 19.60.21F, 0.6 micrometer mesh size) and piezometer wells within the river floodplain. All water samples were shaded from sun exposure during extraction from the subsurface and preserved at 4C until measured at ALEC.Analysis by ICP-MS (metals):Measurements for total metals were made on the Agilent 7700x ICP-MS (for total metals) – Agilent Technologies, Santa Clara, CA. The analytical QA/QC protocol was adapted from US EPA Method 200.8 for analysis by ICP-MS. Calibration standards were prepared from multi-element stock solutions (SPEX Certiprep, Metuchen, NJ). Calibration curves include at least 7 points with correlation coefficients > 0.995. The QC protocol includes a continuing calibration blank (CCB), a continuing calibration verification (CCV) solution and at least one quality control sample (QCS) to be analyzed just after calibration and again after every 12 samples and at the completion of the run. The QCS solutions are from an independent source, such as NIST SRM 1643e - Trace elements in water, or QCS solutions from High Purity Standards (Charleston, SC). Acceptable QC responses must be between 90 and 110% of the certified value. Lastly, a suitable internal standard (usually Rh, In, Ga or Ge) is added using on-line addition into the sample line and mixing tee.Analysis by Shimadzu TOC-L (TOC/TN):The TOC-L system is a combustion technique where liquid samples are injected and combusted into CO2 for carbon detection by non-dispersive infrared (NDIR) and NO for detection by chemiluminescence. A calibration curve using five standard solutions between 0.1 and 7 ppm for carbon and 0.05 and 3.5 ppm for nitrogen is made for each type of measurement with a linearity >0.99. All samples, standards, and QC’s are prepared in 24mL scintillation vials that have been baked for 4hrs at 475 Cº and made using RO water (18.2mΩ). QC’s include a calibration blank check (CCB), continuing calibration check (CCC), and a certified reference material check (CRM). All QC’s are within ±10% error and are run before and after each batch of samples. Samples are diluted and rerun if any measurement concentrations are above the highest standard.Analysis by Ion Chromatography (Anions):The instrument used is the Thermo Scientific Dionex ICS-6000 using AS+AG22 column set for anion analysis with sodium carbonate eluent. A calibration curve using five standard solutions between 5 and 250 umol/L is made with a linearity >0.99. Standards and QC’s are prepared in 15mL polypropylene conical tubes, pipetted along with the samples into 1.5mL polypropylene vials. Dilutions are made using RO water (18.2mΩ). QC’s include a calibration blank check (CCB), continuing calibration check (CCC), and a certified reference material check (CRM). All QC’s are within ±10% error and are run before and after each batch of samples. Samples are diluted and rerun if any measurement concentrations are above the highest standard.All files are in csv format.

54 ENVIRONMENTAL SCIENCES↗

Faraday detector uranium isotope ratio measurement: Insights from solution- and laser ablation-based sampling methodologies on the Neoma MC-ICP-MS

In this study we utilize an all-faraday cup detector configuration on the Neoma MC-ICP-MS to perform uranium isotope ratio determinations from certified reference materials and a nuclear fuel precursor material via solution and laser ablation based sampling methodologies. The goal in performing these measurements is primarily to demonstrate that the all-faraday cup method can produce highly precise and accurate isotope ratios even at relatively low signal intensity levels while also developing a preliminary understanding of how the complex interplay between different amplifier resistor levels (e.g. 10 11 vs 10 13 Ω) and integration times impacts the precision and accuracy of different types of measurements. Our results show that the faraday cups with 1013 Ω resistors in their amplifier feedback loops can be used to produce accurate and relatively precise isotope ratios for ion beams down to ~5 K cps. However, at the lower end of the signal intensities observed in this study, longer integration times are necessary to mitigate the impact of ion beam instability that can occur during laser ablation based sampling. Despite this potential limitation, the all-faraday cup method is highly versatile as exemplified by the analysis of a collection of uranium reference materials with highly variable uranium isotopic compositions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Model ages of three uranium metal CRMs and implications for radiochronometry data interpretation

In this study, we report 230 Th/ 234 U and 231 Pa/ 235 U model ages in three uranium metal certified reference materials with distinct production histories and isotopic compositions ranging from depleted to highly enriched (CRMs 112-A, 115, and 116-A). Here, our results provide the first model age values for these materials using multiple radiochronometers, which can be used as reference values for quality control of radiochronometry measurements performed during nuclear forensic investigations. Furthermore, we evaluate the model ages in the context of available production records for the materials, which provides insight into the processes that may impact radiochronometry systems during uranium metal production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

R&D Outcomes of Surrogate Environmental Swipe Manufacturing Technique Method Development for Arms Control and Treaty Verification Applications

The analysis of environmental samples is a critical component of nuclear compliance verification and safeguards activities. While the associated particle analyses have benefitted from recent advances in the production of actinide-bearing particulates with uniform and well-characterized particle size, material phase, and isotopic ratios to serve as reference materials for calibration and interlaboratory comparisons, there is an outstanding need for surrogate environmental samples, which resemble field-collected samples, with the aforementioned reference particulates to support future nuclear compliance verification exercises and method development. This effort seeks to leverage the recent advances in tailored reference particle production to generate surrogate environmental swipe samples via parallel production techniques (direct and indirect) which are uniquely suited to the hydrothermal and aerosol-based synthesis routes developed at PNNL and SRNL, respectively. PNNL’s hydrothermal particle production method was used to generate surrogate reference particles for the indirect production of test swipes.

54 ENVIRONMENTAL SCIENCES↗

A new algae technical standards focus group: Summarizing and guiding the algae state of the art

The value proposition of algae technical metrics was the subject of a recent, industry-led, Focus Group interactive discussion. The interactive platform allowed for real time capturing and priority ranking of the topics that are deemed critical challenges for a future successful algae-based bioeconomy. This work ultimately sets the stage for providing guidance, methods, and standard reference materials tailored to respective algae industry segments for the cultivation, processing and marketing of high-quality and safe algae-based products. The group solicits input from the broader algae community on the value proposition and presents a case here to build a consensus around algae-specific metrics. The value proposition of technical standards to the industry is that guidance obtained through these collaborations builds producers' and consumers' trust that algae and algae-derived products are safe, reliable, and may allow for expanded market access, and increased competitiveness and international trade.

59 BASIC BIOLOGICAL SCIENCES↗

C136A and C138A Report of Analysis

In this work the isotopic ratios and weight percentages of 238 Pu, 239 Pu, 240 Pu, 241 Pu and 242 Pu were determined using Isotope Dilution Mass Spectrometry. Two samples of C136A and C138A were sent to the Analytical Research laboratories by the National Nuclear Security Administration Nuclear Reference Material Program. The four samples were dissolved in concentrated hydrochloric acid. From the parent solutions, eight aliquots were taken, diluted, spiked with 244 Pu and submitted to separations. After the samples were separated, they were analyzed using Multicollector Inductively Coupled Plasma Mass Spectrometry. Along with the samples, two C126A Quality Control Samples were analyzed each day. Mass bias standards were also analyzed at the beginning, during and at the end of the analysis. GUM Workbench Pro software Version 2.4.1.406 was used to calculate the isotopic ratios relative to 239 Pu, and total Pu mass and the correlated expanded uncertainties.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

International interlaboratory compilation of trace element concentrations in the CUP-2 uranium ore concentrate standard

Herein, a nuclear forensics investigation involving a uranium ore concentrate relies on accurate and precise analysis of impurities. Analytical data defensibility requires the use of reference materials as part of quality control. This study presents a compilation of trace element concentration results of the CUP-2 Uranium Ore Concentrate Standard measured by 11 different laboratories. The laboratories employed various dissolution methods, analytical preparation methods, and instrumental platforms. The data presented here contain concentrations of 66 impurities with up to 138 individual data points for each impurity. Consensus values have been assigned to each impurity following a statistical analysis of the data set.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Collaborative Study for Certification of Trace Elements in Uranium Ore Concentrate CRMs UCLO-1, UCHI-1, and UPER-1

Trace impurity patterns are important nuclear forensic signatures in uranium ore concentrates (UOCs) and Certified Reference Materials (CRMs) are used to validate the analysis methods employed by end users. Herein, we discuss the certification campaign for three new UOC CRMs from the National Research Council Canada: UCLO-1 (https://doi.org/10.4224/crm.2020.uclo-1), UCHI-1 (https://doi.org/10.4224/crm.2020.uchi-1), and UPER-1 (https://doi.org/10.4224/crm.2020.uper-1). This study involved 15 laboratories from 10 countries, using sector-field and (triple) quadrupole inductively-coupled plasma mass spectrometry to analyze 64 trace element impurities. We discuss the importance of the acids used for sample digestion, difficulties analyzing in a high uranium matrix, and data combination and uncertainty evaluation for this large dataset.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Assessment of Low-Level Pu Isotope Ratio Measurements Using Multicollector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS/MS) Equipped with a Pre-Mass Filter

We present an initial investigation into the performance of a multicollector inductively coupled plasmamass spectrometer equipped with a pre-mass filter (Neoma MC-ICP-MS/MS) for making plutonium (Pu) isotope ratio measurements on solutions containing low level (i.e., pg mL –1 ) Pu concentrations. This assessment was achieved by comparison of the 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu ratios attained over a one month period on the MC-ICP-MS/MS with the long-term (∼1 year) performance observed on the predecessor MC-ICP-MS (Neptune Plus) instrument each equipped with an equipped with an APEXΩ desolvating nebulizer for repeated measurements of certified reference materials from New Brunswick Program Office (NBL PO) CRM 136a and CRM 137. The MC-ICP-MS/MS performance of repeated measurement of CRM 136a (n = 20) resulted in mean values of 240 Pu/ 239 Pu = 0.1448 ± 0.0006, 241 Pu/ 239 Pu = 0.00371 ± 0.00006, and 242 Pu/ 239 Pu = 0.00682 ± 0.00006 (k = 2). The CRM 137 (n = 20), analyzed during the same analytical sessions, produced mean values for 240 Pu/ 239 Pu = 0.2414 ± 0.0006, 241 Pu/ 239 Pu = 0.00464 ± 0.00007, and 242 Pu/ 239 Pu = 0.0157 ± 0.0001 (k = 2). These results closely align with the certificate values for CRM 136a and CRM 137 and are within the k = 2 envelopes defined by the long-term performance of the traditional MC-ICP-MS approach (Neptune Plus). Examination of the performance of the various Pu isotope ratios as a function of total Pu content revealed accurate results (<3% relative difference, or RD) above ∼50 fg total Pu. The results presented here demonstrate the capability of the MC-ICP-MS/MS making accurate and precise low level Pu isotopic measurements. While the intent of this work was not to investigate the functionality of the collision cell, the pre-mass filter was employed. Future studies are warranted to investigate the entire capability of the MC-ICP-MS/MS collision cell and pre-cell mass filter optimization for performing low level Pu isotope measurements, even in mixed matrix samples.

CRM↗

Thermal conductivity of RHIC superconducting magnet insulation materials at low temperatures

The Electron-Ion Collider (EIC) is planned to be built upon the Relativistic Heavy Ion Collider (RHIC), which vacuum chamber will need to be upgraded to host the EIC hadron beams. For the beam pipe section running through the RHIC superconducting (SC) magnets, the baseline is to insert a screen that will get cooled by thermal contact to the 4.55 K beam pipe of RHIC. Knowing the material properties of the cold mass is thus crucial to understand which is the final temperature that the screen and the superconducting coils in the magnets will reach during the passage of the EIC beams. The thermal conductivities of two insulation materials in the RHIC superconducting magnets and a reference material were measured at cryogenic temperatures at the Magnet Science and Technology division of the National High Magnetic Field Laboratory (NHMFL). The measurements were performed in a Quantum Design physical property measurement system. This report explains the motivation behind this work and summarizes the measurement method and results.

43 PARTICLE ACCELERATORS↗

Additive Friction Stir Deposition of a Tantalum–Tungsten Refractory Alloy

Additive friction stir deposition (AFSD) is a solid-state metal additive manufacturing technique, which utilizes frictional heating and plastic deformation to create large deposits and parts. Much like its cousin processes, friction stir welding and friction stir processing, AFSD has seen the most compatibility and use with lower-temperature metals, such as aluminum; however, there is growing interest in higher-temperature materials, such as titanium and steel alloys. In this work, we explore the deposition of an ultrahigh-temperature refractory material, specifically, a tantalum–tungsten (TaW) alloy. The solid-state nature of AFSD means refractory process temperatures are significantly lower than those for melt-based additive manufacturing techniques; however, they still pose difficult challenges, especially in regards to AFSD tooling. In this study, we perform initial deposition trials of TaW using twin-rod-style AFSD with a high-temperature tungsten–rhenium-based tool. Many challenges arise because of the high temperatures of the process and high mechanical demand on AFSD machine hardware to process the strong refractory alloy. Despite these challenges, successful deposits of the material were produced and characterized. Mechanical testing of the deposited material shows improved yield strength over that of the annealed reference material, and this strengthening is mostly attributed to the refined recrystallized microstructure typical of AFSD. These findings highlight the opportunities and challenges associated with ultrahigh-temperature AFSD, as well as provide some of the first published insights into twin-rod-style AFSD process behaviors.

36 MATERIALS SCIENCE↗

Versailles Project on Advanced Materials and Standards interlaboratory study on intensity calibration for x-ray photoelectron spectroscopy instruments using low-density polyethylene

We report the results of a Versailles Project on Advanced Materials and Standards interlaboratory study on the intensity scale calibration of x-ray photoelectron spectrometers using low-density polyethylene (LDPE) as an alternative material to gold, silver, and copper. An improved set of LDPE reference spectra, corrected for different instrument geometries using a quartz-monochromated Al Kα x-ray source, was developed using data provided by participants in this study. Using these new reference spectra, a transmission function was calculated for each dataset that participants provided. When compared to a similar calibration procedure using the NPL reference spectra for gold, the LDPE intensity calibration method achieves an absolute offset of ~3.0% and a systematic deviation of ±6.5% on average across all participants. For spectra recorded at high pass energies (≥90 eV), values of absolute offset and systematic deviation are ~5.8% and ±5.7%, respectively, whereas for spectra collected at lower pass energies (<90 eV), values of absolute offset and systematic deviation are ~4.9% and ±8.8%, respectively; low pass energy spectra perform worse than the global average, in terms of systematic deviations, due to diminished count rates and signal-to-noise ratio. Differences in absolute offset are attributed to the surface roughness of the LDPE induced by sample preparation. We further assess the usability of LDPE as a secondary reference material and comment on its performance in the presence of issues such as variable dark noise, x-ray warm up times, inaccuracy at low count rates, and underlying spectrometer problems. In response to participant feedback and the results of the study, we provide an updated LDPE intensity calibration protocol to address the issues highlighted in the interlaboratory study. Finally, we also comment on the lack of implementation of a consistent and traceable intensity calibration method across the community of x-ray photoelectron spectroscopy (XPS) users and, therefore, propose a route to achieving this with the assistance of instrument manufacturers, metrology laboratories, and experts leading to an international standard for XPS intensity scale calibration.

36 MATERIALS SCIENCE↗

Similarity Downselection: Finding the n Most Dissimilar Molecular Conformers for Reference-Free Metabolomics

Computational methods for creating in silico libraries of molecular descriptors (e.g., collision cross sections) are becoming increasingly prevalent due to the limited number of authentic reference materials available for traditional library building. These so-called “reference-free metabolomics” methods require sampling sets of molecular conformers in order to produce high accuracy property predictions. Due to the computational cost of the subsequent calculations for each conformer, there is a need to sample the most relevant subset and avoid repeating calculations on conformers that are nearly identical. The goal of this study is to introduce a heuristic method of finding the most dissimilar conformers from a larger population in order to help speed up reference-free calculation methods and maintain a high property prediction accuracy. Finding the set of the n items most dissimilar from each other out of a larger population becomes increasingly difficult and computationally expensive as either n or the population size grows large. Because there exists a pairwise relationship between each item and all other items in the population, finding the set of the n most dissimilar items is different than simply sorting an array of numbers. For instance, if you have a set of the most dissimilar n = 4 items, one or more of the items from n = 4 might not be in the set n = 5. An exact solution would have to search all possible combinations of size n in the population exhaustively. We present an open-source software called similarity downselection (SDS), written in Python and freely available on GitHub. SDS implements a heuristic algorithm for quickly finding the approximate set(s) of the n most dissimilar items. We benchmark SDS against a Monte Carlo method, which attempts to find the exact solution through repeated random sampling. We show that for SDS to find the set of n most dissimilar conformers, our method is not only orders of magnitude faster, but it is also more accurate than running Monte Carlo for 1,000,000 iterations, each searching for set sizes n = 3–7 out of a population of 50,000. We also benchmark SDS against the exact solution for example small populations, showing that SDS produces a solution close to the exact solution in these instances. Using theoretical approaches, we also demonstrate the constraints of the greedy algorithm and its efficacy as a ratio to the exact solution.

97 MATHEMATICS AND COMPUTING↗

Application of ATONA Amplifiers to the Measurement of Uranium Isotopic Ratios by Thermal Ionization Mass Spectrometry

Uranium isotopic composition can provide valuable information about the history and provenance of a nuclear material; therefore, uranium isotopic analyses are frequently made in the nuclear forensics, safeguards, and environmental monitoring communities. These measurements have always presented challenges due to the extreme variability in the relative abundance between the major ( 235 U, 238 U) and minor ( 233 U, 234 U, 236 U) isotopes of uranium. Here, the recently developed ATONA (Atto- to Nano-Amp) amplification system paired with Faraday cup detectors has a large dynamic range and low noise floor making it ideal for measuring uranium isotopic ratios in materials of both natural and anthropogenic origin. A wide variety of certified reference materials were analyzed to investigate the utility of the ATONA amplification system for determining uranium isotopic composition in samples ranging from depleted to highly enriched. The ATONA amplifiers provide nearly an order of magnitude improvement in external reproducibility over 10 11 Ω amplifiers when measuring the minor 234 U/ 238 U ratio in isotopically natural and depleted samples and when paired with a secondary electron multiplier can measure very low relative abundance uranium isotopes (i.e., 236 U).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Progress in development of characterization capabilities to evaluate candidate materials for direct air capture applications

As part of U.S. national efforts to combat the detrimental effect of global climate change, the National Institute of Standards and Technology (NIST) was recently tasked to support efforts in direct air capture (DAC) of carbon dioxide research and deployment. In order to develop test procedures, materials, and documentary standards, key characterization methods relevant to DAC materials have been investigated and used to identify desirable properties for a potential Standard Reference Material (SRM). Select amine-supported materials that previously showed potential for DAC applications have been characterized using commonly available laboratory methods. Further insights into the adsorption characteristics have been gained from developing and applying more specialized characterization tools ideal for probing low concentrations of carbon dioxide. A broad suite of capabilities that examine relevant properties under appropriate conditions gives the most profound insights into a material's specific performance. We advocate for even more specialized capabilities to be developed and standardized to quantitatively monitor the interactions of CO 2 with molecular species in complex and often disordered systems to advance DAC and support carbon dioxide reduction (CDR) in general.

carbon dioxide↗