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DOE OSTI2021

Surface chemistry models for GaAs epitaxial growth and hydride cracking using reacting flow simulations

Hydride vapor phase epitaxy (HVPE) is a promising technology that can aid in the cost reduction of III-V materials and devices manufacturing, particularly high-efficiency solar cells for space and terrestrial applications. However, recent demonstrations of ultrafast growth rates (~500 µm/h) via uncracked hydrides are not well described by present models for the growth. Therefore, it is necessary to understand the kinetics of the growth process and its coupling with transport phenomena, so as to enable fast and uniform epitaxial growth. In this work, we derive a kinetic model using experimental data and integrate it into a computational fluid dynamics simulation of an HVPE growth reactor. We also modify an existing hydride cracking model that we validate against numerical simulations and experimental data. Here, we show that the developed growth model and the improved cracking model are able to reproduce experimental growth measurements of GaAs in an existing HVPE system.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS↗

DOE OSTI2026

Cluster Dynamics Simulations of Intra-Granular Fission Gas Bubble Size and Pressure Evolution in UO 2

Fission gases such as xenon (Xe) play a critical role in determining the behavior and response of nuclear fuel. Given that Xe has little solubility in UO 2 , it accumulates and forms bubbles, which significantly impact fuel performance. Intra- and inter-granular bubble nucleation and growth can lead to fuel swelling, and once bubbles interconnect at grain boundaries, fission gas can be released into the plenum. At low temperatures, limited uranium vacancy mobility can restrict swelling, therefore causing the bubbles to become highly pressurized. Consequently, this can induce micro-cracking, promote fission gas release (increasing the likelihood of cladding failure), and even lead to fuel pulverization under accident conditions such as a loss of coolant accident. As bubble evolution is strongly influenced by local temperature and fission rate, markedly different behavior occurs across the radial profile of the fuel pellet. Capturing the mechanisms that underpin bubble evolution is therefore important to predict these behaviors in the fuel. Previous models describing important mechanisms informed by lower length scale simulations have been developed under the NEAMS program. These can describe the evolution of a single bubble type (i.e., single value for radius and pressure) at each position in the pellet, for instance using the Centipede cluster dynamic code. However, in reality, a full distribution in bubble sizes and pressures exists within the microstructure at a given position in the pellet. To address this the cluster dynamics code Xolotl, which can predict Xe and vacancy phase space (i.e., bubble distributions) for intra-granular bubbles, has been used before. Prior work benchmarked the Xolotl code against the Centipede cluster dynamics code to ensure compatibility and to verify that mobile defect properties are adequately transferred between the two codes, along with some physics improvements. In this work, we go further by introducing a physics-based set of improvements that will allow us to accurately predict bubble size distributions and internal bubble pressures under representative UO 2 irradiation conditions. The improvements include (i) coupling bubble-defect reaction energies to a virial equation of state (EOS), (ii) including a bubble surface tension contribution, (iii) incorporating radiation-induced re-solution of Xe and vacancies, (iv) enabling pressure-driven dislocation loop punching through an effective emission of interstitial clusters informed by interstitial loop energetics, (v) accounting for radiation induced athermal diffusion of Xe, and (vi) implementing a Booth-type grain boundary sink representation for all mobile defects and defect clusters. After these modifications, we observe good agreement of Xolotl fission gas bubble size and concentration predictions with legacy experimental measurements. Additionally, it allows the distribution of Xe bubble pressures and radius to also be predicted and compared to data produced through the Advanced Fuels Campaign (AFC) program. Here, we have done this by running simulations under conditions similar to the AFC post-irradiation examination (PIE) samples irradiated at North Anna 2 light water reactor (LWR). Our results shows excellent agreement with these experimental measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1985

Initial development and performance evaluation of a process for formation of dense carbon by pyrolysis of methane

The three steps in pyrolytic carbon formation are: (1) gaseous hydrocarbon polymerization and aromatic formation; (2) gas-phase condensation and surface adsorption/impingement of polyaromatic hydrocarbon; and (3) final dehydration to carbon. The structure of the carbon in the various stages of formation is examined. The apparatuses and experimental procedures for the pyrolysis of methane in a 60 cm long quartz reactor tube at temperatures ranging from 1400-1600 K are described. The percentage of carbon converted and its density are calculated and tabularly presented. The results reveal that dense carbon formation is maximized and soot eliminated by this procedure. It is observed that conversion efficiency depends on the composition of the inlet gas and conversion increases with increasing temperature. Based on the experimental data a three-man carbon reactor subsystem (CRS) is developed; the functions of the Sabatier Methanation Reactor, two carbon formation reactors and fluid handling components of the CRS are analyzed. The CRS forms 16 kg of carbon at a rate of 0.8 kg/day for 20 days in a two percent volume density quartz wool packing at temperature of 1500-1600 K.

Noyes, G. P.↗

DOE OSTI2023

Large Eddy Simulation of Convective Heat Transfer in a Random Pebble Bed Using the Spectral Element Method

The development of fluoride-cooled high-temperature reactors has drastically increased the demand for an in-depth understanding of the heat transfer (HT) in packed beds cooled by liquid salts. The complex flow fields and space-dependent porosity found in a pebble bed require a detailed understanding to ensure the proper cooling of the reactor core during normal and accident conditions. As detailed experimental data are complicated to obtain for these configurations, high-fidelity simulation such as large eddy simulation and direct numerical simulation (DNS) can be employed to create a high-resolution heat transfer numerical database that can assist in addressing industrial-driven issues associated with the heat transfer behavior of fluoride-cooled high-temperature reactors. In this paper, we performed a series of large eddy simulation using computational fluid dynamics (CFD) code NekRS to investigate the heat transfer for a bed of 1741 pebbles. Further, the characteristics of the flow, such as average, rms, and time series of velocity and temperature, have been analyzed. Porous media averages have also been performed. The simulation results show a good agreement between non-conjugate heat transfer and conjugate heat transfer. The generated data will be used to benchmark heat transfer modeling methods and local maxima/minima of heat transfer parameters. It will also be used for supporting convective heat transfer quantification for Kairos Power and benchmarking lower fidelity models.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2024

An Assessment of the Safeguards Implications of Particle and Alloy Formation in MSRs

Molten salt reactors (MSRs) present unique challenges for applying safeguards measures and differ significantly from traditional nuclear reactors. Although the special fissionable materials within MSRs principally exist as dissolved species within the fuel salt, key actinides of interest may also be converted to solid phases including alloys and precipitated oxides via chemical and electrochemical reactions. These solid-phase components will complicate the nuclear material accounting and control (NMAC) approaches that have, so far, primarily targeted measurements of the liquid salt itself. For example, most of the proposed monitoring and characterization methods for MSRs are reliant on homogeneity of the salt and the ability to maintain accountable materials in solution. Solid deposits and particulates could invalidate the assumption of homogeneity and necessitate the use of new models and measurement tools to permit a full accounting of all nuclear material in an MSR. To address this, the likelihood of solids formation in MSRs, estimated the rate at which these solids could form, and assessed the monitoring tools that are available to account for the presence of these materials were examined. Specifically, three solid forming mechanisms were investigated, including (1) the accumulation of actinides within the MSR’s structural materials due to alloying, (2) the accumulation of actinides within noble metal fission product particulates, and (3) the generation of actinide oxides from interactions with salt impurities. These modeling-informed studies were completed with considerations to both fluoride- and chloride-containing salts. It was determined that, although measurable amounts of special fissionable material were expected to alloy with the structural elements and fission products, the predicted amounts were below levels considered as significant quantities (SQ) by the International Atomic Energy Agency (IAEA). However, it was determined that sufficiently large oxygen concentrations could potentially lead to significant quantities of special fissionable material being converted to solid oxide phases. As such, a comparative study of technologies that are commercially available to assist in monitoring and accountancy of this material was presented. Policy implications, design recommendations, and suggestions for follow-on experimental work were also presented to further assist reactor vendors in designing and controlling the fuel salt chemistry to address potential safeguards considerations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Aided Active Learning (AAL) for Enhanced Critical Heat Flux Prediction

Accurate prediction of critical heat flux (CHF) is crucial for the safe and efficient operation of nuclear reactors. Traditional CHF modeling methods often require extensive experimental data, which are hard to obtain. This study introduces the Aided Active Learning (AAL) framework, which strategically minimizes data requirements without sacrificing model accuracy. Unlike conventional Active Learning (AL), AAL introduces an additional step of randomly selecting a subset from the sample pool before applying the query strategy. To evaluate the performance of AAL, two query strategies—uncertainty-based sampling and error-reduction sampling—were evaluated across the following models: random forest (RF), feedforward neural network (FNN), and variational feedforward neural network (vFNN). The proposed framework demonstrated that AAL effectively reduces the number of training samples needed to achieve comparable predictive accuracy. For the RF model, AL required only 710 samples to achieve an R2 score of 0.98, as compared to the 4,785 samples needed by random sampling. Similarly, the FNN model achieved the same R2 score with just 355 samples when using AL, a significant improvement over the 825 samples required by random sampling. In case of uncertainty-based sampling strategy, vFNN attained an R2 of 0.98 with 3,420 samples, reducing the sample requirement by 47% relative to the 6,440 samples needed for random sampling. Its performance suggests that larger training data are required to fully leverage its uncertainty quantification capabilities.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Carbon dioxide capture with aqueous amino acids: Mechanistic study of amino acid regeneration by guanidine crystallization and process intensification

CO 2 capture from powerplant-generated flue gas via a phase-changing process involving absorption with aqueous amino acids (e.g., glycine or sarcosine) and bicarbonate crystallization with bis-iminoguanidines (e.g., glyoxal-bis-iminoguanidine or GBIG) is investigated in this paper. This process is of high interest due to its potential to decrease the energy penalty for CO 2 capture by significantly reducing the solvent regeneration energy typically associated with aqueous amine solvents. A critical step in the proposed CO 2 capture mechanism is the regeneration of the amino acid by removal of protons and bicarbonate ions from solution through crystallization of GBIGH 2 2+ bicarbonate salt. Here, we investigated the thermodynamics and kinetics of glycine regeneration by crystallization of GBIGH 2 2+ (HCO 3 – ) 2 (H 2 O) 2 . A theoretical model was developed and compared to experimental data to simulate and predict the glycine regeneration and determine its reaction mechanism. This combined experimental and theoretical study led to the conclusion that, while the GBIGH 2 2+ bicarbonate crystallization step provides most of the thermodynamic driving force for the glycine regeneration, the rate-limiting step is the protonation of GBIG prior to crystallization. The CO 2 loading and amino acid regeneration steps were combined into a single, intensified process using a bubble column reactor. The CO 2 loading capacity of GBIG was experimentally determined to be roughly 1.36 mol CO 2 per mol GBIG. These results provide the fundamental basis for developing an effective carbon capture technology with phase-changing amino acid/guanidine absorbents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Autoignition of cyclohexane at low-to-intermediate temperatures: Rapid compression machine experiments and improved comprehensive chemical kinetic model

Cycloalkanes are an important class of hydrocarbons found in conventional and alternative transportation fuels. Being one of the simplest practical cycloalkanes, cyclohexane is often used as a surrogate in studies to understand the oxidation, ignition, and sooting characteristics of cycloalkanes more broadly. Although cyclohexane has been extensively studied, very limited datasets for cyclohexane oxidation at low-to-intermediate temperatures are available in the literature. Moreover, the literature autoignition data from rapid compression machines (RCMs) did not provide information on volume histories or experimental heat transfer characteristics which can significantly impact model predictions, thereby hindering the detailed validation of chemical kinetic models. It has also been observed that the cyclohexane kinetic models developed so far are not able to predict the literature data across a wide range of operating and mixture conditions. Hence, further studies are recommended to understand and improve model predictions for cyclohexane oxidation. In this study, RCM experiments were conducted using cyclohexane/air mixtures at varying compressed pressures (P C =15, 20, and 30 bar), equivalence ratios (ϕ=0.5, 1.0, and 2.0), and compressed temperatures (T C =670–960 K). The current RCM results of cyclohexane were found to complement well with the literature data, with the first-stage IDTs at high pressures and volume histories at all test conditions being first reported for better development and validation of chemical kinetic models. Additionally, a detailed chemical kinetic model for the cyclohexane oxidation has been developed and validated using both newly acquired experimental IDTs in this study and literature experimental studies (IDTs in RCMs and STs, species profiles in jet-stirred reactors, and laminar burning velocities). Unlike literature models, the proposed model was observed to provide an overall better prediction for experimental results over a wide range of conditions. Chemical kinetic analysis of the developed model was further conducted to identify the reaction pathways controlling the autoignition of cyclohexane.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Conduct weld campaign (FY-21-1) on irradiated materials provided by the Canadian Nuclear Laboratory (CNL), including baseline post-weld evaluation and testing

A collaborative research on developing advanced welding technologies for irradiated stainless steel 304 materials between CNL and ORNL has been established to support both U.S. and Canadian interests in evaluation of weld repair techniques on irradiated materials to support continuous operation of commercial nuclear power. The work utilizes unique material from the National Research Universal (NRU) reactor and the specialized welding hot cell facility at ORNL. The objective is to explore suitable welding technique and parameters and to determine the helium concentration limitation in terms of irradiated stainless-steel weldability. An additional objective is to develop the knowledge and understanding of cracking mechanisms induced by high concentration of helium in the process of weld repair of the irradiated structural alloys. This report summarizes the experimental welding evaluation on irradiated material from the NRU reactor containing helium concentrations ranging from 12 to 45 atomic parts per million (appm).

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2023

Collaborative Study on Weldability of Irradiated Stainless Steel 304 Materials Removed from The NRU Reactor

36 MATERIALS SCIENCE↗

DOE OSTI2023

Establishing the accuracy of position–specific carbon isotope analysis of propane by GC–pyrolysis–GC–IRMS

Rationale: Position-specific (PS) δ 13 C values of propane have proven their ability to provide valuable information on the evolution history of natural gases. Two major approaches to measure PS δ 13 C values of propane are isotopic 13 C nuclear magnetic resonance (NMR) and gas chromatography-pyrolysis-gas chromatography-isotope ratio mass spectrometry (GC-Py-GC-IRMS). Measurement accuracy of the isotopic 13 C NMR has been verified, but the requirements of large sample size and long experimental time limit its applications. GC-Py-GC-IRMS is a more versatile method with a small sample size, but its accuracy has not been demonstrated. Methods: We measured the PS δ 13 C values of propane from nine natural gases using both 13 C NMR and GC-Py-GC-IRMS, then evaluated the accuracy of the GC-Py-GC-IRMS method. Results: The results show that large carbon isotope fractionations occurred for both terminal and central carbons within propane during pyrolysis. The isotope fractionations during the pyrolysis are reproducible at optimum conditions, but vary between the two GC-Py-GC-IRMS systems tested, affected by experimental conditions (e.g., pyrolysis temperature, flow rate, and reactor conditions). Conclusions: It is necessary to evaluate and calibrate each GC-Py-GC-IRMS system using propane gases with accurately determined PS δ 13 C values. Finally, this study also highlights a need for PS isotope standards for propane and other molecules (e.g., butane and acetic acid).

03 NATURAL GAS↗

DOE OSTI2025

Advancing nuclear forensics competencies at the National Nuclear Center of the Republic of Kazakhstan and conceptual development of a National Nuclear Forensics Library

Since 2021, the National Nuclear Center (NNC) of the Republic of Kazakhstan has been successfully developing a project dedicated to nuclear forensics. The relevance of this project is underscored by Kazakhstan’s leading position in the global uranium mining and export market. The country operates research reactors and is involved in the production of experimental nuclear fuel. The nuclear forensics project is being implemented in several key areas: the project will develop competencies in laboratory research of samples, interpretation of results, and develop a prototype concept for the National Nuclear Forensics Library. In implementing these challenges, the NNC experts draw on the experience of colleagues from world-leading scientific and research centers. Designing a prototype National Nuclear Forensics Library (NNFL) is a challenging project. In conclusion, the solution to this task is based on the IAEA’s approaches, recommendations, and the experience gained from the construction of similar systems in other countries.

and nuclear chemistry↗

DOE OSTI2023

Experimental investigation of residence time and axial velocity of 6.0 cm graphite pebbles in a cold-flow pebble bed reactor using radioisotope-based technique

Not provided.

Nuclear Science & Technology↗

DOE OSTI2023

Understanding flow dynamics in membrane distillation: Effects of reactor design on polarization

Optimization and design of full-scale membrane distillation (MD) systems usually require Sherwood and Nusselt correlations that are developed from lab-scale systems. However, entrance effects in lab-scale systems can significantly impact heat, mass and momentum transfer in the reactor, therefore affect the accuracy of the developed experimental Sherwood and Nusselt correlations. Here, Computational Fluid Dynamics (CFD) simulations using OpenFOAM are performed to understand the effects of right-angled bends and inlet design on flow dynamics, temperature and concentration polarization in MD systems. Simulation results show that the presence of right-angled bends and inlets with sudden expansions lead to the formation of Dean vortices. Dean vortices enhance perpendicular mixing in MD systems and reduce both temperature and concentration polarization. Temperature and concentration polarization coefficients in MD systems with right-angled bends and inlets with sudden expansions vary significantly for the same volumetric flow rate. Our studies show that lab-scale systems with the same volumetric flow rate but different designs lead to significantly different Nusselt and Sherwood correlations. Here, this study demonstrates the importance of CFD-informed design of lab-scale systems to minimize entrance effects and suppress Dean vortices for consistent model development and calibration across multiple scales.

42 ENGINEERING↗

DOE OSTI2024

Monte Carlo Perturbation Analysis of Fuel Temperature Variations in the MCNP Model of the Annular Core Research Reactor

The Annular Core Research Reactor (ACRR) Monte Carlo N-Particle (MCNP) model is used by ACRR reactor operators and experiment designers at Sandia National Laboratories for a variety of computational calculations ranging from reactor kinetics parameter estimates and safety analyses to experimental planning. To understand the dominant source of uncertainty within the MCNP model, perturbations in temperature were applied to individual ACRR MCNP fuel rods. Fuel rod temperatures were randomly sampled from a uniform distribution from operational temperatures to quantify temperature-related uncertainty effects. Stochastic mixing was used to blend the cross sections of the desired temperatures using the MCNP continuous and Thermal Neutron Scattering Treatment [S(α,β)] libraries in ENDF/B-VII.1. Furthermore, this uncertainty analysis produced a 640 row × 640 column correlation and covariance matrix of the neutron energy spectra. Positive covariance was produced around the 1-MeV region and the 0.2-eV region. Correlation was found in the thermal and fast energy regions, but no correlation was observed in the slowing-down energy region because interactions in this region are not dominated by fuel.

ACRR↗

DOE OSTI2025

The new ITER baseline, research plan and open R&D issues

A new baseline (NB) has been proposed by the ITER Project to ensure a robust achievement of the Projects’ goals, in view of past challenges including delays incurred due to the Covid-19 pandemic, technical challenges in completing first-of-a-kind components and in nuclear licensing. The NB includes modifications to the configuration of the ITER device and its ancillaries (e.g. change from beryllium to tungsten as first wall material, modification of the heating and current drive mix, etc.) as well as additional testing of components (e.g. toroidal field coils) or phased installation (start with inertially cooled first wall before later installation of the final actively water-cooled components) to minimise operational risks. In the NB, the ITER research plan (IRP) will be divided into three main phases: (a) start of research operation, with 40 MW of ECH and 10 MW of ICH, which will focus on the demonstration of 15 MA operation in L-mode, commissioning of all required systems, including disruption mitigation, and the demonstration of H-mode plasma operation in deuterium; (b) DT-1, with 60–67 MW of ECH, 33 MW of neutral beam injection (NBI) and 10–20 MW of ICH, which will demonstrate robust operation in high confinement H-mode plasmas in DT up to Q ⩾ 10 and for burn durations of 300–500 s within an accumulated neutron fluence of ∼1% of the ITER machine’s lifetime total, and; (c) DT-2, with up to 67 MW of ECH, up to 49.5 MW of NBI and up to 20 MW of ICH, with the ITER tokamak and ancillaries in their final configuration to demonstrate routine operation in DT plasmas at high Q and the Q ⩾ 5 long-pulse and steady-state scenarios to the final neutron fluence and to perform R&D on nuclear fusion reactor issues. The logic, physics basis, modelling and experimental evaluations carried out to support the NB and the associated IRP are described. These include the impact of the tungsten wall on plasma scenarios and associated risk mitigation measures, as well as the optimisation of the tokamak components and ancillaries to minimise Project risks. Open R&D issues related to these evaluations and mitigation measures are also described together with experimental, modelling and validation activities required to address them.

ITER↗

DOE OSTI2021

Passive deconfinement of runaway electrons using an in-vessel helical coil

A helical coil designed to passively generate non-axisymmetric fields during a plasma disruption is shown (via electromagnetic analysis, linear MHD modeling, and relativistic drift orbit tracing) to be effective at deconfining runaway electrons (REs) on a time scale significantly faster than the plasma current quench. Magnetic equilibria from DIII-D RE-producing scenarios are used to calculate the toroidal electric field generated during the current quench phase of a disruption, which in turn drives current in the proposed n = 1 in-vessel helical coil, without the need for any external power supplies or disruption detection or prediction techniques. Simulations of the plasma evolution using the TokSys GS Evolve code predict the inductive coupling of coil currents up to 12% of the pre-disruption plasma current into the helical coil. The coil geometry is parametrically varied to maximize both the non-resonant and resonant components of the 3D magnetic perturbation, resulting in δB/B ≈ 10 –2 and a vacuumisland overlapwidth of up to 0.7ψ N . The REORBIT module of the MARS-F code is used to model the full non-axisymmetric magnetic field and trace RE drift orbits to determine the effect on RE deconfinement, with up to 70% of the RE orbits lost after 0.2 ms. A two-stage evolution of the RE orbit loss fraction is observed to be caused by resonant trapping between multiple magnetic island chains. Finally, electromagnetic and thermal stresses on the coil are calculated to be within operational limits for installation in DIII-D, and scale favorably to a reactor-size device. Furthermore, these findings motivate future experimental study of the helical coil concept in DIII-D or other tokamaks.

3D coil↗

DOE OSTI2023

Autonomous Controls For Reactor Technologies (acorn)

ACORN (Autonomous Controls fOr Reactor techNologies) software utilizes data, obtained from an experimental test bed and/or simulation, to implement a control command for microreactor operation. Command examples include a change to the temperature profile, power profiles, heat fluxes, etc. The control command recommended by the code is derived based on future predicted states of a microreactor, allowing proactive optimal and autonomous microreactor operation. The software is written in Python languages. The current software supports autonomous temperature controls of heat pipe simulator and autonomous heat flux controls of a 37 heat pipe non-nuclear testbed simulator (or its surrogate models).

Lin, Linyu [Idaho National Laboratory (INL), Idaho↗