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At least 667 records · Page 37

Graphene SHDMC Data

The data used to produce all of the figures and tables in the manuscript titled "Highly Accurate Many-Body Theory Reaches 2D Materials" can be found here. This data set includes: -SHDMC results for graphene -selected CI with and without re-normalized second-order perturbation (rPT2) theory corrections for graphene -data demonstrating that SHDMC displays an exponential rate of convergence -data used for sCI + rPT2 complete basis set extrapolation -data used to extrapolate SHDMC energies to the infinite basis limit -data used to demonstrate compactness of SHDMC wavefunction

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Two-stage formation-energy correction (NbZr, TaZr, VZr)

This bundle contains the scripts, the raw and corrected per-structure data, and the manuscript plots for the NbZr / TaZr / VZr BCC binary formation energies and the associated RMSDs. Why a two-stage correction is necessary: The "raw" formation energy of every relaxed VASP configuration is computed in the usual way, FE_raw(c) = E_alloy(c) - sum_i x_i * E_pure_i , where E_pure_i are the per-atom total energies of the pure-element reference structures (Nb, Ta, V, Zr in the same BCC supercell, with identical INCAR / KPOINTS / PAW choices). With perfectly consistent reference runs the raw FE should vanish at the two pure-element endpoints (x = 0 and x = 1) by construction. In practice this does not hold for two reasons that are present in our dataset: 1. Reference-energy inconsistency (composition-dependent bias). Even with identical input parameters, the pure-element runs (stored in `corrected_DFT_pure_element_runs/`) differ slightly from the values that would be implied by the alloy runs at near-pure compositions (a few meV/atom). This bias is approximately linear in concentration, because the residual error in E_pure_Nb (or E_pure_Ta / E_pure_V) propagates into FE_raw(c) as (1 - x) * dE_pure_1, and the corresponding error in E_pure_Zr propagates as x * dE_pure_2. Left uncorrected, this produces a non-physical "tilt" of FE_raw(x) and shifts the entire FE-vs-x cloud away from zero at the endpoints. 2. Endpoint anchoring against the audited true endpoints. The strict endpoint values (FE_x0_meVatom, FE_x1_meVatom in `corrected_fe_strict_endpoints_20260518/strict_endpoint_check_20260518.csv`) were re-derived from an independent cross-check of the pure-element runs. After stage 1 removes the linear bias, the near-pure compositions in the alloy dataset still extrapolate to values that differ slightly from these audited endpoints — because stage 1 is fit from a few near-end alloy bins, not from the audited pure-element references themselves. The README.txt file discusses how these issues are addressed by the two-stage correction, and describes folder layout, pipeline summary, and how to re-run.

36 MATERIALS SCIENCE↗

Learning genetic perturbation effects with variational causal inference

Advances in sequencing technologies have enhanced the understanding of gene regulation in cells. In particular, Perturb-seq has enabled high-resolution profiling of the transcriptomic response to genetic perturbations at the single-cell level. This understanding has implications in functional genomics and potentially for identifying therapeutic targets. Various computational models have been developed to predict perturbational effects. While deep learning models excel at interpolating observed perturbational data, they tend to overfit in the lack of enough data and may not generalize well to unseen perturbations. In contrast, mechanistic models, such as linear causal models based on gene regulatory networks, hold greater potential for extrapolation, as they encapsulate regulatory information that can predict responses to unseen perturbations. However, their application has been limited to small studies due to overly simplistic assumptions, making them less effective in handling noisy, large-scale single-cell data. We propose a hybrid approach that combines a mechanistic causal model with variational deep learning, termed Single Cell Causal Variational Autoencoder (SCCVAE). The mechanistic model employs a learned regulatory network to represent perturbational changes as shift interventions that propagate through the learned network. SCCVAE integrates this mechanistic causal model into a variational autoencoder, generating rich, comprehensive transcriptomic responses. Our results indicate that SCCVAE exhibits superior performance over current state-of-the-art baselines for extrapolating to predict unseen perturbational responses. Additionally, for the observed perturbations, the latent space learned by SCCVAE allows for the identification of functional perturbation modules and simulation of single-gene knockdown experiments of varying penetrance, presenting a robust tool for interpreting and interpolating perturbational responses at the single-cell level.

59 BASIC BIOLOGICAL SCIENCES↗

West Flank Coso FORGE: 3D Temperature Model

x,y,z data of the 3D temperature model for the West Flank Coso FORGE site. Model grid spacing is 250m. The temperature model for the Coso geothermal field used over 100 geothermal production sized wells and intermediate-depth temperature holes. At the near surface of this model, two boundary temperatures were assumed: (1) areas with surface manifestations, including fumaroles along the northeast striking normal faults and northwest striking dextral faults with the hydrothermal field, a temperature of ~104 deg C was applied to datum at +1066 meters above sea level elevation, and (2) a near-surface temperature at about 10 meters depth, of 20 deg C was applied below the diurnal and annual conductive temperature perturbations. These assumptions were based on heat flow studies conducted at the CVF and for the Mojave Desert. On the edges of the hydrothermal system, a 73 deg C/km temperature gradient contour was established using conductive gradient data from shallow and intermediate-depth temperature holes. This contour was continued to all elevation datums between the 20 deg C surface and -1520 meters below mean sea level. Because the West Flank is outside of the geothermal field footprint, during Phase 1, the three wells inside the FORGE site were incorporated into the preexisting temperature model. To ensure a complete model was built based on all the available data sets, measured bottom-hole temperature gradients in certain wells were downward extrapolated to the next deepest elevation datum (or a maximum of about 25% of the well depth where conductive gradients are evident in the lower portions of the wells). After assuring that the margins of the geothermal field were going to be adequately modelled, the data was contoured using the Kriging method algorithm. Although the extrapolated temperatures and boundary conditions are not rigorous, the calculated temperatures are anticipated to be within ~6 deg C (20 deg F), or one contour interval, of the observed data within the Coso geothermal field. Based on a lack of temperature data west of 74-2TCH, the edges of this model still seem to have an effect on West Flank modeled temperatures.

15 GEOTHERMAL ENERGY↗

Utah FORGE: Temperature Contours at 200 m

The individual shapefiles in this dataset delineate estimated temperature contours (20, 40, 60, and 80 deg C) at a depth of 200 m in the Milford, Utah FORGE area. Contours were derived from 86 geothermal, gradient, and other wells drilled in the area since the mid-1970s with depths greater than 50 m. Conductive temperature profiles for wells less than 200 m were extrapolated to determine the temperature at the desired depth. Because 11 wells in the eastern section of the study area (in and around the Mineral Mountains) are at higher elevations compared to those closer to the center of the basin, temperature profiles were extrapolated to a constant elevation of 200 m below the 1830 m (6000 ft) a.s.l. datum (approximate elevation of alluvial fans at the base of the Mineral Mountains) to smooth the contours across the ridges and valleys.

15 GEOTHERMAL ENERGY↗

Scripts and data associated with a manuscript linking soil and sediment elemental composition with dissolved organic matter chemistry across CONUS

This data package provides scripts and geochemical data for a manuscript titled “Linkages between mineral element composition of soils and sediments with hyporheic zone dissolved organic matter chemistry across the contiguous United States” (preprint: doi: 10.22541/essoar.169447343.31694990/v1). This data is associated with the Worldwide Hydrobiogeochemistry Observation Network for Dynamic River Systems (WHONDRS, https://whondrs.pnnl.gov) and is an extension of the Summer 2019 Sampling campaign which crowdsourced samples from rivers and sediment across the continental United States. Data from this study can be found at https://data.ess-dive.lbl.gov/datasets/doi:10.15485/1603775 and https://data.ess-dive.lbl.gov/datasets/doi:10.15485/1729719. The main objective of this manuscript was to couple sediment water extractable dissolved organic matter chemistry, defined by ultra-high resolution mass spectrometry, with localized sediment elemental composition and watershed scale soil elemental characteristics. This data package contains one main folder with four subfolders. The main data folder contains (1) readme; (2) data dictionary (dd); (3) file-level metadata (flmd); (4) an R markdown to reproduce manuscript figures and analyses; (5) a pdf of instructions to reproduce NGS interpolations with ArcGIS software; and (6) a python script to reproduce NGS extrapolations with python. The four subfolders contain files required to reproduce NGS extrapolations include (1) ‘CONUS_boundaries’ containing boundary layers (.shp) for the Continental United States; (2) ‘ngs_project’ containing files (.shp) with point level NGS soil elemental data (Grossman et al., 2004); (3) ‘raster_outputs’ containing the interpolated raster output files for various soil elements; and (4) ‘NGS_Chemistry_Final’ contain final extracted soil elemental data.

54 ENVIRONMENTAL SCIENCES↗

Status of permanent magnet radiation resiliency studies at CEBAF

An ongoing investigation for the future of Jefferson Lab’s Continuous Electron Beam Accelerator Facility (CEBAF) lies in upgrading its maximum nominal energy using Fixed-Field Alternating-gradient (FFA) technology for its recirculating arcs, using permanent magnets for the FFA arcs. A common concern among the community is the degradation of these permanent magnets during operation due to the radiation environment in which they will be present. This work, funded by a Laboratory Directed R&D grant, aims to measure the permanent magnet degradation in the CEBAF tunnel enclosure, and extrapolate to the energies expected from the upgrade. We present the latest results of this study, as well as plans moving forward.

Accelerator Physics↗

Bridging the PSI Knowledge Gap: A Multi-Scale Approach

Plasma-surface interactions (PSI) pose an immense scientific hurdle in magnetic confinement fusion and our present understanding of PSI in confinement environments is highly inadequate; indeed, a recent Fusion Energy Sciences Advisory Committee report found that 4 out of the 5 top five fusion knowledge gaps were related to PSI. The time is appropriate to develop a concentrated and synergistic science effort that would expand, exploit and integrate the wealth of laboratory ion-beam and plasma research, as well as exciting new computational tools, towards the goal of bridging the PSI knowledge gap. This effort would broadly advance plasma and material sciences, while providing critical knowledge towards progress in fusion PSI. This project involves the development of a Science Center focused on a new approach to PSI science; an approach that both exploits access to state-of-the-art PSI experiments and modeling, as well as confinement devices. The organizing principle is to develop synergistic experimental and modeling tools that treat the truly coupled multi-scale aspect of the PSI issues in confinement devices. This is motivated by the simple observation that while typical lab experiments and models allow independent manipulation of controlling variables, the confinement PSI environment is essentially self-determined with few outside controls. This means that processes that may be treated independently in laboratory experiments, because they involve vastly different physical and time scales, will now affect one another in the confinement environment. Also, lab experiments cannot simultaneously match all exposure conditions found in confinement devices typically forcing a linear extrapolation of lab results. At the same time programmatic limitations prevent confinement experiments alone from answering many key PSI questions. The resolution to this problem is to usefully exploit access to PSI science in lab devices, while retooling our thinking from a linear and de-coupled extrapolation to a multi-scale, coupled approach. The PSI Plasma Center consisted of three equal co-centers; one located at the MIT Plasma Science and Fusion Center, one at UC San Diego Center for Energy Research and one at the UC Berkeley Department of Nuclear Engineering, which moved to the University of Tennessee, Knoxville (UTK) with Professor Brian Wirth in July 2010. The Center had three co-directors: Prof. Dennis Whyte led the MIT co-center, the UCSD co-center was led by Dr. Russell Doerner, and Prof. Brian Wirth led the UCB/UTK center. The directors have extensive experience in PSI and material research, and have been internationally recognized in the magnetic fusion, materials and plasma research fields. The co-centers feature keystone PSI experimental and modeling facilities dedicated to PSI science: the DIONISOS/CLASS facility at MIT, the PISCES facility at UCSD, and the state-of-the-art numerical modeling capabilities at UCB/UTK. A collaborative partner in the center is Sandia National Laboratory at Livermore (SNL/CA), which has extensive capabilities with low energy ion beams and surface diagnostics, as well as supporting plasma facilities, including the Tritium Plasma Experiment, all of which significantly augment the Center. Interpretive, continuum material models are available through SNL/CA, UCSD and MIT. The participating institutions of MIT, UCSD, UCB/UTK, SNL/CA and LLNL brought a formidable array of experimental tools and personnel abilities into the PSI Plasma Center. Our work has focused on modeling activities associated with plasma surface interactions that are involved in effects of He and H plasma bombardment on tungsten surfaces. This involved performing computational material modeling of the surface evolution during plasma bombardment using molecular dynamics modeling. The principal outcomes of the research efforts within the combined experimental – modeling PSI center are to provide a knowledgebase of the mechanisms of surface degradation, and the influence of the surface on plasma conditions.

36 MATERIALS SCIENCE↗

Aging Behavior and Performance Projections for a Polysulfide Elastomer

The accelerated aging behavior and aging state of a 30 year old field retrieved polysulfide elastomer was examined. The material is used as an environmental thread sealant for a stainless steel bolt in a steel threaded insert in an aluminum assembly. It is a two component curable polysulfide elastomer that is commercially available in a similar formulation as was applied 30 years ago. The primary goal of this study was to establish if aging over 30 years under moderate aging conditions (mostly ambient temperature and humidity) resulted in significant property changes, or if accelerated aging could identify developing aging pathways which would prevent the extended use of this material. The aging behavior of this material was examined in three ways: A traditional accelerated thermo-oxidative aging study between 95 to 140°C which focused on physical and chemical properties changes, an evaluation of the underlying oxidation rates between RT and 125°C, and an assessment of the aging state of a small 30 year old sample. All three data sets were used to establish aging characteristics, their time evolution, and to extrapolate the observed behavior to predict performance limits at RT. The accelerated aging study revealed a relatively high average activation energy of ~130 kJ/mol which gives overconfident performance predictions. Oxidation rates showed a decreasing behavior with aging time and a lower E a of ~84 kJ/mol from time - temperature superposition , but also predicted sufficient additional performance at RT. Consistent with these projections for extended RT performance, only small changes were observed for the 30 year old material. Extrapolations using this partially aged material also predict ongoing use as a viable option. Unexpected RT degradation could only develop into a concern should the oxidation rate not trend lower over time as was observed at elevated temperature. Considering all data acquired in this limited aging study , there are no immediately apparent concerns with this material for ongoing use. ACKNOWLEDGEMENTS We thank Lisa Deibler for providing us with a small sample of field aged and new commercial material.

Celina, Mathias C.↗

Detailed Characterization of Nuclear Recoil Pulse Shape Discrimination in the DarkSide-50 Direct Dark Matter Experiment

While evidence of non-baryonic dark matter has been accumulating for decades, its exact nature continues to remain a mystery. Weakly Interacting Massive Particles (WIMPs) are a well motivated candidate which appear in certain extensions of the Standard Model, independently of dark matter theory. If such particles exist, they should occasionally interact with particles of normal matter, producing a signal which may be detected. The DarkSide-50 direct dark matter experiment aims to detect the energy of recoiling argon atoms due to the elastic scattering of postulated WIMPs. In order to make such a discovery, a clear understanding of both the background and signal region is essential. This understanding requires a careful study of the detector's response to radioactive sources, which in turn requires such sources may be safely introduced into or near the detector volume and reliably removed. The CALibration Insertaion System (CALIS) was designed and built for this purpose in a j oint effort between Fermi National Laboratory and the University of Hawaii. This work describes the design and testing of CALIS, its installation and commissioning at the Laboratori Nazionali del Gran Sasso (LNGS) and the multiple calibration campaigns which have successfully employed it. As nuclear recoils produced by WIMPs are indistinguishable from those produced by neutrons, radiogenic neutrons are both the most dangerous class of background and a vital calibration source for the study of the potential WIMP signal. Prior to the calibration of DarkSide-50 with radioactive neutron sources, the acceptance region was determined by the extrapolation of nuclear recoil data from a separate, dedicated experiment, ScENE, which measured the distribution of the pulse shape discrimination parameter, $f_{90}$, for nuclear recoils of known energies. This work demonstrates the validity of the extrapolation of ScENE values to DarkSide-50, by direct comparison of the $f_{90}$ distributio n of nuclear recoils from ScENE and an AmBe calibration sour! ce. The combined acceptance as defined by ScENE and the \textit{in-situ} AmBe calibration were used to establish the best WIMP exclusion limit on an argon target. Unfortunately, radioactive sources used for the calibration of DarkSide-50 are universally accompanied by gamma decays, which obscure the low energy region where most WIMP interactions are expected to occur and seem to make continuing dependence on an external measurement such as ScENE inevitable. However, this work presents a novel method of nuclear recoil calibration employing event selection, unique to the design of DarkSide-50, which produces a nearly pure sample of nuclear recoils. Further, it describes the execution of a neutron calibration campaign, from planning to analysis, which yielded a valuable data set for defining the acceptance region. Together with the event selection techniques, this allows for the definition of the acceptance region independent of ScENE values. Two analytical models of the $f_{90 }$ distribution are described and their results for nuclear recoils are compared. Finally, a detailed study of integrated noise in nuclear and electron recoil

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

An Investigation into Solution Verification for CFD-DEM

This report presents the study of the convergence behavior of the computational fluid dynamicsdiscrete element method (CFD-DEM) method, specifically National Energy Technology Laboratory’s (NETL) open source MFiX code (MFiX-DEM) with a diffusion based particle-tocontinuum filtering scheme. In particular, this study focused on determining if the numerical method had a solution in the high-resolution limit where the grid size is smaller than the particle size. To address this uncertainty, fixed particle beds of two primary configurations were studied: i) fictitious beds where the particles are seeded with a random particle generator, and ii) instantaneous snapshots from a transient simulation of an experimentally relevant problem. Both problems considered a uniform inlet boundary and a pressure outflow. The CFD grid was refined from a few particle diameters down to 1/6 th of a particle diameter. The pressure drop between two vertical elevations, averaged across the bed cross-section was considered as the system response quantity of interest. A least-squares regression method was used to extrapolate the grid-dependent results to an approximate “grid-free” solution in the limit of infinite resolution. The results show that the diffusion based scheme does yield a converging solution. However, the convergence is more complicated than encountered in simpler, single-phase flow problems showing strong oscillations and, at times, oscillations superimposed on top of globally non-monotonic behavior. The challenging convergence behavior highlights the importance of using at least four grid resolutions in solution verification problems so that (over-determined) regression-based extrapolation methods may be applied to approximate the grid-free solution. The grid-free solution is very important in solution verification and VVUQ exercise in general as the difference between it and the reference solution largely determines the numerical uncertainty. By testing different randomized particle configurations of the same general problem (for the fictitious case) or different instances of freezing a transient simulation, the numerical uncertainties appeared to be on the same order of magnitude as ensemble or time averaging uncertainties. By testing different drag laws, almost all cases studied show that model form uncertainty in this one, very important closure relation was larger than the numerical uncertainty, at least with a reasonable CFD grid, roughly five particle diameters. In this study, the diffusion width (filtering length scale) was mostly set at a constant of six particle diameters. A few exploratory tests were performed to show that similar convergence behavior was observed for diffusion widths greater than approximately two particle diameters. However, this subject was not investigated in great detail because determining an appropriate filter size is really a validation question which must be determined by comparison to experimental or highly accurate numerical data. Future studies are being considered targeting solution verification of transient simulations as well as validation of the filter size with direct numerical simulation data.

97 MATHEMATICS AND COMPUTING↗

Creep Analysis of Poly(ester urethane) Copolymer by Dynamic Mechanical Analysis (DMA): Melt Determination

An experiment is presented utilizing film tension, creep test dynamic mechanical analysis (DMA) to characterize the physical properties of a poly(ester urethane) block copolymer, Estane ® 5703. The polymer was pressed into a sheet from pellet form and cut into strips for analysis utilizing the TA Q800 DMA with film tension clamp. The strips were tested under five constant stress analyses from 0.125 to 0.625, at 0.125 MPa increments. Each analysis was run stepwise through a temperature gradient from 25 °C to 67 .5 °C with 2.5 °C increments, the material reached the instrument maximum displacement at different temperature steps dependent on the constant applied stress. At each of the 18 temperature steps the material was held at constant stress for 10 minutes and allowed to recover under stress-less conditions for 20 minutes. With data analysis recoverable strain data was produced and ultimately a curve of Modulus at temperature, the regression extrapolated to modulus = 0 M Pa. The extrapolated point correlated with data the weighted average melt point of the polymer measured by MDSC, within the regressive least squares fit of the measured moduli. Thereby measuring the melt temperature of a polymer by DMA. This is the third in a series of three reports 4,5 on the physical properties and degradation processes of materials used in polymer bonded explosive 9501 written for submission to the University of Oregon, Masters Industrial Internship Program.

36 MATERIALS SCIENCE↗

Dead-End Filtration and Crystalline Silicotitanate Cesium Ion Exchange with Hanford Tank Waste AW-102

The Direct Feed Low-Activity Waste (DFLAW) flowsheet provides for the initial production of immobilized low-activity waste (ILAW) by feeding low-activity waste (LAW) directly from tank farms to the Hanford Tank Waste Treatment and Immobilization Plant (WTP) LAW facility for immobilization. Prior to the transfer of feed to the WTP LAW facility, tank supernatant waste will be pretreated by the Tank Side Cesium Removal (TSCR) system to meet the WTP LAW waste acceptance criteria (<3.18E-5 Ci 137Cs/mole of Na). This pretreatment facility will filter the waste to remove suspended solids and remove cesium from the waste stream through ion exchange. Bench-scale filtration testing of 7.4 liters of diluted of AW-102 supernate was conducted using dead-end filtration in the hot cells of the Radiochemical Processing Laboratory at Pacific Northwest National Laboratory. A Mott 70-mm disc filter (media grade 5) was used to capture solids. The filter area was adjusted to 2.2 in2 to match the planned TSCR supernate process volume to surface area ratio. There was no indication of filter fouling and no recoverable solids were observed on the filter. Ion exchange testing with the filtered, diluted AW-102 supernatant was conducted using crystalline silicotitanate (CST) ion exchange media. The IONSIV R9140-B CST was provided by Honeywell UOP, LLC in 2018 (Lot number 8056202-999). The column testing operations were prototypic to the intended Low-Activity Waste Pretreatment System operations in a lead-lag column format, although on a small-scale basis with 10-mL CST beds. The feed was processed downflow through the lead column and then through the lag column at ~1.8 bed volumes per hour (BV/h). After 88.6 BVs of feed processing, the volume in the feed bottle dropped below the inlet tube and the lead column fluid headspace was displaced with air. Feed processing was suspended while a new column was prepared and installed into the lead position. A total of 450 BVs of diluted AW-102 feed were processed through the new lead column; only 4.3% Cs breakthrough was achieved. This volume of feed was insufficient to generate useful Cs loading information without extrapolation. A straight-line extrapolation was used to determine the 50% breakthrough of the lead column and contract limit breakthrough from the lag. The values were found to be 1200 BVs and 930 BVs, respectively.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Initial Development of an Improved Creep-Fatigue Design Method that Avoids the Separate Evaluation of Creep and Fatigue Damage and Eliminates the Requirement for Stress Classification

This report describes a method for capturing the effect of strain range, temperature, hold time, and elastic follow up on the cyclic life of a material undergoing uniaxial load. Developing design correlations of this type requires methods for extrapolating experimental data as a function of hold time and follow up factor. Various extrapolation methods are developed and discussed here and recommendations are developed for the final approaches to be adopted for design use. The report also describes comparisons between the new creep-fatigue design method, described here, and current creep-fatigue design methods in the ASME Boiler and Pressure Vessel Code and associated nuclear Code Cases. These comparisons demonstrate several advantages of the new method: it is easier to execute and is less over conservative than many current approaches. This report, along with a companion on extending these results to multiaxial load and on combining load cycles, represents the accumulation of several years of work on the development of this new approach to creep-fatigue design, combining an elastic perfectly plastic analysis method with simplified model tests measuring the effect of elastic follow up on creep-fatigue cyclic life. The conclusions to this report describe a path forward to developing the required design data for high temperature advanced reactor structural materials and guiding the adoption of the new method in the ASME Boiler and Pressure Vessel Code and related standards.

36 MATERIALS SCIENCE↗

Cesium Ion Exchange Testing Using a Three-Column System with Crystalline Silicotitanate and Hanford Tank Waste 241-AP-107

Washington River Protection Solutions (WRPS) is working to support early production of immobilized low-activity waste by feeding Hanford tank supernate from tank farms to the Hanford Waste Treatment and Immobilization Plant (WTP) Low-Activity Waste (LAW) facility. This goal incorporates the design of a Tank-Side Cesium Removal (TSCR) system, which in effect filters tank waste supernate and processes it through a cesium ion exchange medium to remove 137Cs. The 137Cs-depleted product is sent to the WTP for vitrification. Rovira et al. (2018) reported the successful Cs removal from Hanford tank 241-AP-107 waste (hereafter called AP-107) using crystalline silicotitanate (CST) ion exchange media manufactured by Honeywell UOP, LLC (product IONSIVTM R9140-B, Batch 2081000057) in a lead-lag column system. Since that testing, WRPS has changed the column design to a three-column system. WRPS requested a repeated study with AP-107 tank waste using a different batch of IONSIVTM R9140-B, Lot 2002009604, in a three-column format. A small-scale test platform was constructed to demonstrate solids filtration, Cs removal, and LAW vitrification and installed at Pacific Northwest National Laboratory. This report describes the small-scale ion exchange testing system component of the test platform and the processing of approximately 8.55 L of filtered AP-107 supernate using CST, Lot 8056262-999, that passed through a 25-mesh filter. This report also describes the Cs ion exchange batch contact testing to determine the Cs distribution coefficient and the maximum Cs loading capacity in the AP-107 tank waste matrix. Batch contact testing helps to evaluate CST performance on tank waste supernate and is often used prior to processing tank waste through ion exchange columns to assess some performance metrics (e.g., 50% Cs breakthrough). Batch contact tests were performed with the filtered AP-107 tank waste at four Cs concentrations at a phase ratio of 200 (liquid volume to exchanger mass). The distribution coefficient (K d ) at the equilibrium condition of 9.2 µg Cs/mL (AP-107 feed condition) was determined to be 806 mL AP 107/g CST. With a CST bed density of 1.01 g/mL (<25 mesh CST), this K d corresponded to a predicted 50% Cs breakthrough of 814 bed volumes (BVs). The Cs load capacity at the equilibrium feed condition was determined to be 8.3 mg Cs/g dry CST. The three-column format testing was prototypic to the intended TSCR operations, albeit on a small scale with 10-mL CST beds. Flowrate was adjusted to match the CST contact time expected for the full-scale operation, i.e., matched bed volumes per hour (BV/h) flow rate. The feed was processed downflow through the lead column, then through the middle column, and then through the polish column. Loading continued at an average of 1.88 BV/h (1.83 to 2.04 BV/h range) until the entire available AP-107 feed was processed. The Cs-decontaminated product will be provided for vitrification testing. The lead column only reached 45% Cs breakthrough after processing 855 BVs of feed. The 50% Cs breakthrough was extrapolated to occur at ~900 BVs. This extrapolated 50% Cs breakthrough value differed from the batch contact estimate (814 BVs) by 13%. The waste acceptance criteria (WAC) or contract limit for the WTP LAW vitrification facility is 3.18E-5 Ci 137 Cs per mole Na. For the AP-107 tank waste, only 0.127% of the influent 137 Cs concentration may be delivered to the WTP; this required a Cs decontamination factor of 787. The Cs effluent from the middle column reached the WAC after processing 590 BVs. Cs breakthrough from the polish column began at 590 BVs, reaching 6.3E-3 µCi/mL or 4.3E-3% Cs breakthrough after processing 844 BVs of feed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Progression to Compatibility Evaluations in Flowing Molten Salts

Molten salt compatibility with structural alloys has been identified as a key issue for the development of Generation 3 concentrating solar power (CSP) systems with thermal storage. To accelerate this evaluation to pumped systems, the goal of this project was to conduct thermal convection loop (TCL) experiments with a peak temperature of ≥700°C and a typical temperature gradient of ~100°C. The experiments indicated that conventional ~16wt.%Cr Ni-based alloys are compatible up to 700°C with purified (i.e. low O) or dried (low H₂O) industrial-sourced Mg-K-Na chloride salt with <10 μm/yr loss. This two-year project was conducted based on the experimental and mechanistic understanding developed more than 60 years ago at Oak Ridge National Laboratory (ORNL). The first TCL experiment met the <15 μm/yr corrosion metric for this project with specimens of Ni-based alloy 600 exposed at 580°-700°C for 1000 h and post-exposure room temperature tensile tests showed minimal degradation. The second TCL experiment successfully deployed an electrochemical sensor from Argonne National Laboratory and had a peak temperature of 750°C but only ran for ~110 h due to a furnace failure. Both experiments used highly purified industrial-sourced salt with an O content of ~3 μg O/g salt and a Mg addition of 0.04 wt.%. In the second year, the Chloride Collective developed a more economical drying procedure such that the O content was much higher (>20,000 μg O/g salt). A third TCL experiment was conducted with a sensor and a peak temperature of 700°C using dried salt from the same industrial source and increased NaCl content (~20 wt.%). In addition to a 0.05% Mg addition to the salt, a Mg coupon was added in the coldest part of the loop which dissolved during the experiment. Again, small mass changes were noted for specimens of alloys 600 and C276 but the values were slightly higher than those measured in purified salt with Mg. A thin non-continuous and non-adherent oxide layer was deposited on most specimens containing Mg, Si and Al but Cr depletion also was observed. Both years included facilities qualification crucible experiments and then capsule experiments to confirm a baseline isothermal reaction rate. The first year capsule experiment led to the conclusion that the two-stage ORNL purification process using NH₄Cl and CCl₄ left the salt with a high Cl potential and a Mg addition (~0.05wt.%) was needed to lower the potential. The second year capsule experiments at 600° and 700°C found little difference in depth of attack for 0-0.25%Mg additions. In general, the complex reactions where salt can be trapped in the porous surface layer of metal indicated that mass change is an unreliable metric and average depth of Cr depletion is a better metric for assessing the extent of attack. These results have created a new baseline that is contrary to the recent published literature for chloride salts where mass losses have been reported that can be extrapolated to very significant annual metal loss rates. Chloride salt corrosion can be controlled and the results also indicate that salt purification to low O levels may not be necessary. However, additional TCL experiments are needed at different times and temperatures to generate important engineering information such as temperature dependent corrosion rates and reaction rate laws for extrapolation to long-term behavior and isolate the effect of salt additives and impurities.

36 MATERIALS SCIENCE↗

Model 9975 O-Ring Fixture Long-Term Leak Performance (FY2020 Status Report)

Leak testing experiments to monitor the aging performance of Viton GLT and GLT-S O-rings used in the model 9975 shipping package has been ongoing since 2004 at Savannah River National Laboratory. Seventy tests using mock-up 9975 primary containment vessels (PCVs) with GLT O-rings were assembled and heated to temperatures ranging from 200 to 450 °F. In addition, fourteen tests with GLT-S O-rings were initiated in 2008 and heated to temperatures ranging from 200 to 400 °F. The conditioning temperatures are elevated compared to the calculated maximum O-ring temperature in a 9975 package in storage, 158 °F, to accelerate aging and enable observations of O-ring failures in a reasonable time frame. The fixtures are leak tested periodically and all GLT O-ring fixtures aging at 350 °F or above have failed to maintain a leak-tight seal. Eight GLT O-ring fixtures aging at 300 °F have failed after 2.8 to 5.7 years at temperature while the remaining fixtures at 300 °F were retired from testing following more than five years without failure. No failures have yet been observed in GLT O-ring fixtures aging at 200 °F for 12 to 14 years or aging at 270 °F for 8.5 years. All GLT-S O-ring fixtures aging at 300 °F or above have failed their leak test. No failures have yet been observed in GLT-S O-ring fixtures aging at 200 and 250 °F for 10 to 10.5 years. Data from the O-ring fixtures are generally consistent with results from compression stress-relaxation testing, and provide confidence in the predictive models based on those results. However, uncertainty exists in extrapolating these elevated temperature results to the lower temperatures of interest for normal storage in K-Area Complex (KAC). Oxygen consumption testing, which includes results from temperatures near KAC normal storage temperatures, is ongoing to provide further confidence and corroborate these extrapolations. The collective data from these test efforts suggest the minimum O-ring service life at KAC normal storage conditions should be at least 34 years for GLT and GLT-S O-rings. Measurement of compression set in O-rings removed from failed fixtures, compared to that from KAC surveillance O-rings, indicates margin remains for O-rings still in service. Aging and periodic leak testing will continue for the remaining PCV fixtures.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

National Ignition Campaign Data Analysis by an ICF Outsider

A simple DT burn model, with no alpha-particle warming feedback, using a combination of ICF inputs and the measured ion temperature, T, volume compression, C, ablator velocity, v, and burn width time, Δt, can reproduce the national-ignition campaign (NIC) fusion yields with a rms percent difference of ~40%. Analysis suggestion the fusion-yield reproducibility of NIC events with nominally identically measured T, C, v, and Δt is <30%. The highest fusion yields, at a fixed laser energy are obtained with depleted-uranium (DU) hohlraums and high-density carbon (HDC) ablators. Small diameter fit tubes (≤5 μm) enhance fusion yields by an average of 26±15% relative to 10-μm diameter fit tubes. A dependence of fusion yield on the diameter of the capsule relative to the diameter of the hohlraum is inferred for fixed T, C, v, and Δt. No evidence of conditions close to ignition, or alpha-particle warming is found in the existing NIC data with LEH< 2MJ. To obtain a predictive model for extrapolation proposes we map the T, C, and v into power laws as a function of LEH. The above mentioned extrapolatable model has a rms percent difference from the yields of the second half of the NIC of (56 ± 4)%. Higher (and significantly lower) DT temperatures are obtained with HDC ablators (and low-foot drives). The highest compressions are obtained via low-foot drives, but this does not compensate for the corresponding lower temperatures. An extrapolation of the presented model suggests significant alpha-particle heating at an LEH of ~5 MJ. It is hoped that others more familiar it the conditions needed for ignition will use to presented model to estimate the LEH required for ignition.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗