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DOE OSTI2023

Integral Experiment Request 554: CED-2 Summary Report

This report summarizes the critical experiment design 2 (CED-2) or final design study for Integral Experiment Request 554 (IER-554). This experiment describes the effects and importance of adding a commercially available neutron absorber material to a known light-water low-enriched uranium assembly. The assembly in question is the Seven Percent Critical Experiments (7uPCX) at Sandia National Laboratories. The neutron absorber plates considered for the experiment are known as Boralcan and are made of boron carbide (B 4 C) particles embedded in 1100 aluminum alloy. The concentrations of B 4 C and 1100 aluminum were changed as well as the thickness and the positions of the plates, and the fuel rod configuration was adapted to ensure that the assembly would be critical in each case studied. A total of 6 critical configurations, each with a neutron absorber plate inserted, are described in this report. No results of high-quality integral experiments involving neutron absorbers made with B 4 C and 1100 aluminum plates are currently publicly available. Sensitivity to the neutron absorber plate material definition, isotopes, and cross sections of specific regions and configurations are also analyzed. As part of the final design of the experiment, a safe plate holder made of 3003 aluminum was designed. The study results indicate that these experiments are achievable with sufficiently low uncertainties and minimal modification to the assembly, and the CED-3 phase can start when funding allows.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

AMICE2 measurements of lab-generated and ambient aerosols at BNL from 2025-07-21 to 2025-08-22

From July 21 through August 22, 2025 the Absorption Measurement Inter-Comparison Experiment phase 2 (AMICE2) was conducted at Brookhaven National Laboratory. The experiment included concurrent operation of several filter-based instruments and in situ instruments sampling from a common sample line. The common sample line provided all instruments with either lab-generated aerosols composed of external mixtures of nigrosin, cabojet, and ammonium sulfate, or with ambient aerosol drawn through an external stack. This data set contains measurements from the CAPS PMssa instrument taken as a reference instrument at 532 nm and against which the effectiveness of the filter corrections may be assessed. It also contains attenuation coefficients from all filter-based instruments and filter transmittances in order to permit correction for filter loading, and the SSA and COA to permit corrections for aerosol darkness. Finally, two sets of multiplicative corrections are provided for the AE-33, TAP, and MA-350 instruments: the first one, Corr1, corrects for filter amplification factor and loading, the second one, Corr2, corrects for the aerosol darkness in terms of the natural log of COA.

Aerosol Extinction↗

DOE OSTI2025

Modeled sensitivity of multi-MA accelerator performance to electrode contaminant inventory

Significant particle-in-cell code development has enabled simulations of power flow in multi-MA accelerators to include the desorption of surface contaminants, their ionization into surface plasmas, and the impact of these plasmas on efficiency. The simulations base desorption on an Arrhenius equation, whose most significant unknown is the surface contaminant inventory. The sensitivity of power-flow simulations to this inventory is studied here using Sandia National Laboratories' Z accelerator with a 7-nH MagLIF load [Phys. Plasmas 17, 056303 (2010)]. Simulations are conducted in 3D cylindrical coordinates for the current-adder, or “convolute,” region of Z and in 2D for the final feed only. Simulated contaminant inventories are varied from 1 to 32 monolayers (MLs) in 2D, and 2 to 4 ML in 3D. The results reveal sensitivities to the local ratio of E/B⁠. The high B-field, low E-field region near the short-circuit load is insensitive to the contaminant inventory, where assumed values of 4–32 ML change the load current by ≤ 2%, and agree with experiment to within 2% at peak current. A 1-ML value is the outlier, increasing the load current by 5%, but still within measurement uncertainty. In contrast, the relatively higher E-field, lower B-field convolute region has slower contaminant desorption and higher-magnitude E-field penetration of the surface plasmas. The current loss in the convolute region does increase with contaminant inventory. The loss assuming 4 ML is 12% larger than for 2 ML, with 4 ML being the better match to experiment.

Arrhenius equation↗

DOE OSTI2024

Perennializing marginal croplands: going back to the future to mitigate climate change with resilient biobased feedstocks

Managing annual row crops on marginally productive croplands can be environmentally unsustainable and result in variable economic returns. Incorporating perennial bioenergy feedstocks into marginally productive cropland can engender ecosystem services and enhance climate resiliency while also diversifying farm incomes. We use one of the oldest bioenergy-specific field experiments in North America to evaluate economically and environmentally sustainable management practices for growing perennial grasses on marginal cropland. This long-term field trial called 9804 was established in 1998 in eastern Nebraska and compared the productivity and sustainability of corn (Zea mays L.)—both corn grain and corn stover—and switchgrass (Panicum virgatum L.) bioenergy systems under different harvest strategies and nitrogen (N) fertilizer rates. This experiment demonstrated that switchgrass, compared to corn, is a reliable and sustainable bioenergy feedstock. This experiment has been a catalyst for other bioenergy projects which have also expanded our understanding of growing and managing bioenergy feedstocks on marginal cropland. We (1) synthesize research from this long-term experiment and (2) provide perspective concerning both the knowledge gained from this experiment and knowledge gaps and how to fill them as well as the role switchgrass will play in the future of bioenergy.

09 BIOMASS FUELS↗

DOE OSTI2023

Charge state transition levels of Ni in $β$-Ga 2 O 3 crystals from experiment and theory: An attractive candidate for compensation doping

Nickel-doped β-Ga 2 O 3 crystals were investigated by optical absorption and photoconductivity, revealing Ni-related deep levels. Here, the photoconductivity spectra were fitted using the phenomenological Kopylov and Pikhtin model to identify the energy of the zero-phonon transition (thermal ionization), Franck–Condon shift, and effective phonon energy. The resulting values are compared with the predicted ones by first-principle calculations based on the density functional theory (DFT). An acceptor level (0/-) of 1.9 eV and a donor level (+/0) of 1.1 eV above the valence band minimum are consistently determined for Ni Ga , which preferentially incorporates on the octahedrally coordinated Ga site. Temperature-dependent resistivity measurements yield a thermal activation energy of ~2.0 eV that agrees well with the determined Ni acceptor level. Conclusively, Ni is an eminently suitable candidate for compensation doping for producing semi-insulating β-Ga 2 O 3 substrates due to the position of the acceptor level (below and close to the mid-bandgap).

36 MATERIALS SCIENCE↗

DOE OSTI2022

Elucidating structure and dynamics of crystalline α-zirconium phosphates intercalated with water and methanol by multinuclear solid-state MAS NMR: A comprehensive NMR approach

Solid-state NMR experiments on 2 H, 31 P, 13 C, and 1 H nuclei, including 31 P T 1 , 1 H T 1 , and 1 H T 1ρ measurements, as well as on the kinetics of proton-phosphorus cross-polarization have been performed to characterize the crystalline and amorphous α-zirconium phosphates, which were intercalated with D 2 O and/or CD 3 OD. The 13 C{ 1 H} CP MAS NMR experiment performed for compound 1-CD 3 OD (Zr (HPO 4 ) 2 .0.2CD 3 OD) with carbon cross-polarization via protons of phosphate groups has provided a prove that the methanol was intercalated into the interlayer spaces of this compound. The variable-temperature 2 H solid-echo MAS NMR spectra of intercalated compounds demonstrated that the methanol molecules, in contrast to the mobile water, were immobile, keeping, however, free CD 3 rotations around the C 3 -axis. It has been demonstrated that the intercalated species, D 2 O and CD 3 OD, do not affect the high-frequency motions of the phosphate groups. By utilizing local structural models that satisfy the constraints of the experimental data, it has been suggested that the immobile methanol molecules are located in the cavity between two neighboring layers of the zirconium phosphates. Here, the present work illustrates the reliable criteria in a comprehensive NMR approach to structural and dynamic studies of such systems.

1H↗

DOE OSTI2022

High-temperature compressive creep tests of U 3 Si 2 with spark plasma sintering: Experiments and finite element modeling

This paper reports a systematic high-temperature creep behavior of dense U 3 Si 2 pellets using a spark plasma sintering (SPS) apparatus at elevated temperatures and pressures under vacuum conditions. The stress exponent was subsequently derived to be 3.21 at 1173 K and 2.17 at 1223 K, respectively, indicating a grain boundary sliding creep mechanism. The creep activation energy was determined to be 203.6 ± 19.0 kJ/mol, which agrees well with the literature. Finite element modeling was performed using the creep parameters fitted from the strain-time plot. Additionally, the results suggest an excellent match with the experimental data, confirming the validity of the experiments. Microstructure characterizations indicate that the main phase of the specimens after creep tests remains to be U 3 Si 2 , with a 4 μm thick layer of nano-sized particles induced from the diffusion between U 3 Si 2 and alumina disc used to avoid electric current passing through the sample. The successful conduct of creep experiments demonstrates the great potential of SPS to perform high-temperature mechanical testing of nuclear fuels under vacuum conditions. The subsequent finite element modeling exhibits excellent capabilities for accurately predicting material performance in the creep tests and provides a practical tool in evaluating nuclear fuels’ performance for a much-extended time scale.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Broadband Solenoidal Haloscope for Terahertz Axion Detection

We introduce the Broadband Reflector Experiment for Axion Detection (BREAD) conceptual design and science program. This haloscope plans to search for bosonic dark matter across the [ 10 - 3 , 1 ] eV ([0.24, 240] THz) mass range. BREAD proposes a cylindrical metal barrel to convert dark matter into photons, which a novel parabolic reflector design focuses onto a photosensor. This unique geometry enables enclosure in standard cryostats and high-field solenoids, overcoming limitations of current dish antennas. A pilot 0.7 m 2 barrel experiment planned at Fermilab is projected to surpass existing dark photon coupling constraints by over a decade with one-day runtime. Axion sensitivity requires < 10 - 20 W / Hz sensor noise equivalent power with a 10 T solenoid and 10 m 2 barrel. We project BREAD sensitivity for various sensor technologies and discuss future prospects.

Liu, Jesse↗

DOE OSTI2020

Transformation of Ferrihydrite to Goethite and the Fate of Plutonium

Understanding the interactions between plutonium and iron (oxy)hydroxide minerals is necessary to gain a predictive understanding of plutonium environmental mobility and to evaluate long-term performance of nuclear waste repositories. We investigated the fate of plutonium during the formation of ferrihydrite and its subsequent transformation into goethite. Ferrihydrite was synthesized with varying quantities of Pu(IV) following either a sorption or coprecipitation process; the ferrihydrite was then aged hydrothermally to yield goethite. Additionally, the synthesized materials were characterized via extended X-ray absorption fine structure spectroscopy, transmission electron microscopy, and acid leaching to elucidate the nature of plutonium association with ferrihydrite and goethite. In samples prepared following the sorption method, plutonium was identified in two different forms: a PuO 2 precipitate and a surface-sorbed plutonium complex. For the samples prepared via coprecipitation, no PuO 2 formation occurs in the ferrihydrite precursor and in the goethite experiments where plutonium concentration is ≤1000 ppm (mg kg –1 ). In these coprecipitation products, plutonium is strongly bound to the minerals either via formation of an inner sphere complex, or via an incorporation process. In the coprecipitation experiments, PuO 2 formation only occurs at the highest plutonium concentration (3000 ppm), suggesting that during ferrihydrite transformation into goethite, part of the plutonium can be remobilized to form PuO 2 nanoparticles. Collectively, our results demonstrate that the nature of plutonium associated with the precursor ferrihydrite (adsorbed vs coprecipitated) will have a direct impact on the association of plutonium with its alteration product (goethite). Furthermore, the data illustrate that some properties of plutonium association with the precursor ferrihydrite are retained through the transformation into goethite. These findings show that plutonium strongly associates with iron (oxy)hydroxides formed through coprecipitation processes and in these materials, plutonium can be strongly retained by the iron minerals.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Fe- and Ru-H-Mordenites for Polyethylene Upcycling: Insights from Thermo-Catalytic Pyrolysis and DFT Studies

Catalytic pyrolysis of polyethylene (PE) was performed using Fe- and Ru-impregnated H-mordenite (HM) catalysts to produce lighter hydrocarbons. Catalyst surface areas were analyzed by N 2 adsorption−desorption and acidity by NH 3 - TPD studies. Reducibility of metal from H 2 -TPR, experiments indicate multiple oxidation states of Fe due to higher H 2 consumption. The catalyst activity studies monitored by GC− MS analysis highlight the importance of temperature and PE: catalyst ratio in optimizing hydrocarbon selectivity to C 1 −C 4 alkanes and C 2 −C 5 olefins. Studies with polymer-to-catalyst ratios of 1:1 and 1:2 at higher temperature increased PE conversion with stronger acid sites favoring conversion and moderate acid sites improving selectivity toward lighter olefins. While propane dominated at lower temperatures, propene was the main product at 500 °C. Both catalysts exhibited overall similar conversion, while Ru-HM yielded >40% propene selectivity compared to <40% for Fe-HM. Ethylene selectivity exceeded 10% in both cases. Density functional theory simulations using a C 4 surrogate on Ru-HM confirmed that late-stage cracking dominates dehydrogenation, validating the proposed reaction mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

NCSP Integral Experiments at Sandia in FY21 [Slides]

This presentation provides details regarding integral experiments at Sandia National Laboratory for fiscal year 2021. The experiments discussed are as follows: IER 230: Characterize the Thermal Capabilities of the 7uPCX; IER 304: Temperature Dependent Critical Benchmarks; IER 305: Critical Experiments with UO 2 Rods and Molybdenum Foils; IER 306: Critical Experiments with UO 2 Rods and Rhodium Foils ; IER 441: Epithermal HEX Lattices with SNL 7uPCX Fuel for Testing Nuclear Data; IER 452: Inversion Point of the Isothermal Reactivity Coefficient; and IER 523: Critical Experiments with ACRR UO 2 -BeO Fuel.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

A proposal for reconciling diverse experiments on the superconducting state in Sr 2 RuO 4

A variety of precise experiments have been carried out to establish the character of the superconducting state in Sr 2 RuO 4 . Many of these appear to imply contradictory conclusions concerning the symmetries of this state. Here we propose that these results can be reconciled if we assume that there is a near-degeneracy between a ${d}_{{x}^{2}-{y}^{2}}$ (B 1g in group theory nomenclature) and a ${g}_{xy({x}^{2}-{y}^{2})}$ (A 2g ) superconducting state. From a weak-coupling perspective, such an accidental degeneracy can occur at a point at which a balance between the on-site and nearest-neighbor repulsions triggers a d-wave to g-wave transition.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Platform Of Optimal Experiment Management

The platform of optimal experiment management, POEM, powered with automated machine learning to accelerate the discovery of optimal solutions, and automatically guide the design of experiments to be evaluated. POEM currently supports 1) random model explorations for experiment design, 2) sparse grid model explorations with Gaussian Polynomial Chaos surrogate model to accelerate experiment design ,3) time-dependent model sensitivity and uncertainty analysis to identify the importance features for experiment design, 4) model calibrations via Bayesian inference to integrate experiments to improve model performance, and 5) Bayesian optimization for optimal experimental design. In addition, POEM aims to simplify the process of experimental design for users, enabling them to analyze the data with minimal human intervention, and improving the technological output from research activities.

Wang, Congjian [Idaho National Laboratory (INL), I↗

DOE OSTI2023

Characterization of Mk-IV and EBR-II X441A Metallic Fuel Pins for the THOR-C-2 and THOR-M-TOP-1 Experiments: Results from Post-Transient Neutron Tomography of THOR-C-2 Capsule and Pre-transient Non-Destructive and Destructive Examination of DP 36 and DP 40 (Rev.1)

Current interest in sodium-cooled fast reactor designs, such as TerraPower’s Natrium Reactor, has highlighted the need for advanced-reactor fuel technology development. A Fuel Safety Research and Development (FSRD) program for metallic fast reactor fuels has been created to achieve comprehensive safety testing within the re-commissioned Transient Reactor Test (TREAT) facility at the Idaho National Laboratory. Despite over 60 years of metallic fuel irradiation, uncertainties exist in the performance of the fuel system, particularly under anticipated operational occurrences and severe accident scenarios. Throughout historical testing within the Experimental Breeder Reactor (EBR)-II and the Fast Flux Test Facility, fuel behavior has demonstrated benign response to transient reactor conditions; however, accurate predictions of failure thresholds rely heavily on fuel composition and irradiation history. In advancing the FSRD program, two planned transient heating experiments are at various stages of completion. The Temperature Heat sink Overpower Response (THOR)-C-2, fueled with an unirradiated Mk IV U-10Zr pin, has undergone transient irradiation in TREAT and post-transient three-dimensional neutron tomography. Additionally, pre-transient characterization of test and sibling U-19Pu-10Zr pins for THOR-M-TOP-1 was evaluated by both non-destructive and destructive methods. The test and sibling pins were selected from previously irradiated EBR-II experiment X441A. Both pins underwent visual examination, precise gamma spectrometry, two-dimensional neutron radiography, and element contact profilometry while the sibling pin was additionally subjected to sectioning and optical microscopy. THOR-C-2 radiography captured the fuel and cladding relocation during the intermediate transient at the top and bottom of the THOR capsule, allowing key features to be linked to the pin’s measured thermal response. For THOR M TOP 1, a solid baseline for steady-state behavior has been established. No anomalous features were identified in either the test or sibling pin. Defining characteristics and features were recorded for further comparisons.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Hunga Tonga–Hunga Ha′apai Volcano Impact Model Observation Comparison (HTHH-MOC) project: experiment protocol and model descriptions

The 2022 Hunga volcanic eruption injected a significant amount of water vapor and a moderate amount of sulfur dioxide into the stratosphere, causing observable responses in the climate system. We have developed a model–observation comparison project to investigate the evolution of volcanic water and aerosols and their impacts on atmospheric dynamics, chemistry, and climate, using several state-of-the-art chemistry climate models. The project goals are (1) to evaluate the current chemistry–climate models to quantify their performance in comparison to observations and (2) to understand atmospheric responses in the Earth system after this exceptional event and investigate the potential impacts in the projected future. To achieve these goals, we designed specific experiments for direct comparisons to observations, for example from balloons and the Microwave Limb Sounder satellite instrument. Experiment 1 consists of two sets of free-running ensemble experiments from 2022 to 2031: one with fixed sea-surface temperatures and sea ice and one with coupled ocean. These experiments will help to understand the long-term evolution of water vapor and aerosols; quantify HTHH effects on stratospheric and mesospheric temperatures, dynamics, and transport; understand the impact of dynamic changes on ozone chemistry; quantify the net radiative forcings; and evaluate any surface climate impact. Experiment 2 is a nudged-run experiment from 2022 to 2023 using observed meteorology. To allow participation of more climate models with varying complexities of aerosol simulation, we include two sets of simulations in Experiment 2: Experiment 2a is designed for models with internally generated aerosol, while Experiment 2b is designed for models using prescribed aerosol surface area density. This experiment will help to analyze H 2 O and aerosol evolution, quantify the net radiative forcings, understand the impacts on mid-latitude and polar O 3 chemistry, and allow close comparisons with observations.

Zhu, Yunqian [Univ. of Colorado, Boulder, CO (Unit↗

DOE OSTI2022

Creating Frustrated Lewis Pairs in Defective Boron Carbon Nitride for Electrocatalytic Nitrogen Reduction to Ammonia

Abstract The electrocatalytic nitrogen reduction reaction (NRR) on metal‐free catalysts is an attractive alternative to the industrial Haber–Bosch process. However, the state‐of‐the‐art metal‐free electrocatalysts still suffer from low Faraday efficiencies and low ammonia yields. Herein, we present a molecular design strategy to develop a defective boron carbon nitride (BCN) catalyst with the abundant unsaturated B and N atoms as Lewis acid and base sites, which upgrades the catalyst from a single “Lewis acid catalysis” to “frustrated Lewis pairs (FLPs) catalysis.” 14 N 2 / 15 N 2 exchange experiments and density functional theory (DFT) calculations reveal that FLPs can adsorb an N 2 molecule to form a six‐membered ring intermediate, which enables the cleavage of N 2 via a pull–pull effect, thereby significantly reducing the energy barrier to −0.28 eV. Impressively, BCN achieves a high Faraday efficiency of 18.9 %, an ammonia yield of 20.9 μg h −1 mg −1 cat. , and long‐term durability.

Lin, Wenwen↗

DOE OSTI2022

Creating Frustrated Lewis Pairs in Defective Boron Carbon Nitride for Electrocatalytic Nitrogen Reduction to Ammonia

Lin, Wenwen↗

DOE OSTI2022

Two-Phase Flow Mechanisms Controlling CO2 Intrusion into Shaly Caprock

Abstract Geologic carbon storage in deep saline aquifers has emerged as a promising technique to mitigate climate change. CO 2 is buoyant at the storage conditions and tends to float over the resident brine jeopardizing long-term containment goals. Therefore, the caprock sealing capacity is of great importance and requires detailed assessment. We perform supercritical CO 2 injection experiments on shaly caprock samples (intact caprock and fault zone) under representative subsurface conditions. We numerically simulate the experiments, satisfactorily reproducing the observed evolution trends. Simulation results highlight the dynamics of CO 2 flow through the specimens with implications to CO 2 leakage risk assessment in field practices. The large injection-induced overpressure drives CO 2 in free phase into the caprock specimens. However, the relative permeability increase following the drainage path is insufficient to provoke an effective advancement of the free-phase CO 2 . As a result, the bulk CO 2 front becomes almost immobile. This implies that the caprock sealing capacity is unlikely to be compromised by a rapid capillary breakthrough and the injected CO 2 does not penetrate deep into the caprock. In the long term, the intrinsically slow molecular diffusion appears to dominate the migration of CO 2 dissolved into brine. Nonetheless, the inherently tortuous nature of shaly caprock further holds back the diffusive flow, favoring safe underground storage of CO 2 over geological time scales.

58 GEOSCIENCES↗