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At least 199 records · Page 11

Yet Another Hauser-Feshbach Code

Code framework to perform simulations of nuclear reactions with incident particles including gammas, protons, neutrons, deuterons, tritons, helium-3, and alphas to develop nuclear data libraries and study nuclear reaction phenomona. The code can model nuclear reactions or initial populations specified by the user. The decays principally follow the compound-nucleus hypothesis and the statistical decay of Hauser and Feshbach. The code models nuclear decays with a Monte Carlo process that tracks the decay of each state. Data libraries are produced that can be translated into GNDS (generalized Nuclear Data Structure). YAHFC can also be used as an event generator, with individual decays written to disk for offline analysis. Both serial and MPI versions are provided. YAHFC does NOT perform transport of nuclear reactions through materials, only the primary reaction with a target material.

Ormand, WilliamE.↗

Tritiated Sulfur Hexafluoride Disposition Strategies

Tritium (T 2 ) is a radioactive isotope of hydrogen that is produced in nuclear fission reactions and is often used in nuclear fusion reactions and accelerator-based applications for medical isotope production. As a hydrogen isotope, tritium can readily bind to hydroxyl radicals (OH), forming tritiated water (HTO or T 2 0), and to carbon atoms. Tritium decays to helium-3 ( 3 He) via beta-decay with max decay energy of 18.6 keV. While it is not an external radiation hazard, it can be an internal radiation hazard if tritium is inhaled, ingested, or absorbed through the skin. In applications where tritium is handled, tritium confinement is performed using different barriers to minimize releases to the environment. For gaseous (elemental), liquid (oxide), and metal (hydride) tritium, process piping and components provide the primary confinement function. Secondary tritium confinement is typically provided by inert (i.e. non-flammable gases such as nitrogen, argon, or helium) gloveboxes which are connected to a tritium stripper system. Primary tritium confinement barriers typically produce low volumes of high tritium concentrations of tritiated methane from carbon in steels or organic materials along with tritiated water/tritium oxide (e.g. HTO) and tritiated ammonia from reactions with oxygen and nitrogen. Tritium escaping primary confinement into secondary confinement atmospheres (e.g. gloveboxes) produce higher volumes of lower activity contamination than found in process piping. Tritium contamination also occurs by leaks or tritium permeation/diffusion through confinement materials. Tritium from inside primary confinement barriers will diffuse or leak out of the primary confinement barrier and usually into the air, if the system is inside an air hood or ventilated hot cell, or into the secondary confinement (e.g. glovebox) atmosphere which is either exhausted or stripped based on the function of the secondary confinement (glovebox) system. Accelerator based processes for medical isotope production represent an atypical tritium contamination challenge. In medical isotope production, deuterium supply gas is ionized and accelerated to a tritium gas target to produce neutrons that are then used to produce the medical isotopes through additional nuclear fission reactions. To create large voltage differentials for accelerator operations, an electrical insulation medium is needed to prevent or rapidly quench electric discharges. A common electrical insulation medium utilized in accelerator applications is sulfur hexafluoride (SF 6 ) gas. SF 6 has a high dielectric strength and allows for the construction of smaller accelerator systems compared to other electrical insulation mediums such as air or dry nitrogen. Due to tritium permeation/diffusion through accelerator process and confinement materials, there is the possibility that tritium can contaminate the electrical insulation medium of the accelerator. Tritium contaminated SF 6 creates a material without any obvious processes for managing the contamination, reuse, or disposal of the used SF 6 . This document will discuss possible management strategies for tritium contaminated SF 6 for accelerator-based processes for Molybdenum-99 (Mo-99) production.

07 ISOTOPE AND RADIATION SOURCES↗

Nuclear Fusion Reactions in Deuterated Metals

Nuclear fusion reactions of D-D are examined in an environment comprised of high density cold fuel embedded in metal lattices in which a small fuel portion is activated by hot neutrons. Such an environment provides for enhanced screening of the Coulomb barrier due to conduction and shell electrons of the metal lattice, or by plasma induced by ionizing radiation (γ quanta). We show that neutrons are far more efficient than energetic charged particles, such as light particles (e−, e+) or heavy particles (p, d, α) in transferring kinetic energy to fuel nuclei (D) to initiate fusion processes. It is well-known that screening increases the probability of tunneling through the Coulomb barrier. Electron screening also significantly increases the probability of large- versus small-angle Coulomb scattering of the reacting nuclei to enable subsequent nuclear reactions via tunneling. This probability is incorporated into the astrophysical factor S(E). Aspects of screening effects to enable calculation of nuclear reaction rates are also evaluated, including Coulomb scattering and localized heating of the cold fuel, primary D-D reactions, and subsequent reactions with both the fuel and the lattice nuclei. The effect of screening for enhancement of the total nuclear reaction rate is a function of multiple parameters including fuel temperature and the relative scattering probability between the fuel and lattice metal nuclei. Screening also significantly increases the probability of interaction between hot fuel and lattice nuclei increasing the likelilhood of Oppenheimer-Phillips processes opening a potential route to reaction multiplication. We demonstrate that the screened Coulomb potential of the target ion is determined by the nonlinear Vlasov potential and not by the Debye potential. In general, the effect of screening becomes important at low kinetic energy of the projectile. We examine the range of applicability of both the analytical and asymptotic expressions for the well-known electron screening lattice potential energy Ue, which is valid only for E >> Ue (E is the energy in the center of mass reference frame). We demonstrate that for E ≤ Ue, a direct calculation of Gamow factor for screened Coulomb potential is required to avoid unreasonably high values of the enhancement factor f (E) by the analytical—and more so by the asymptotic—formulas.

Vladimir Pines↗

Experimental test of the ratio method for nuclear-reaction analysis

Nuclear halos are exotic quantal structures observed far from stability. They are mostly studied through reactions. The ratio of angular cross sections for breakup and scattering is predicted to be independent of the reaction process and to be very sensitive to the halo structure. We test this new observable experimentally for the first time on the collision of 11 Be on C at 22.8 MeV/nucleon and using existing data on Pb at 19.1 MeV/nucleon. The theoretical predictions are verified, which offers the possibility to develop a new spectroscopic tool to study nuclear structure far from stability.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Experimental Test of the Ratio Method for Nuclear-Reaction Analysis

Nuclear halos are exotic quantal structures observed far from stability. They are mostly studied through reactions. The ratio of angular cross sections for breakup and scattering is predicted to be independent of the reaction process and to be very sensitive to the halo structure. Here, we test this new observable experimentally for the first time on the collision of 11 Be on C at 22.8 MeV/nucleon and using existing data on Pb at 19.1 MeV/nucleon. The theoretical predictions are verified, which offers the possibility of developing a new spectroscopic tool to study nuclear structure far from stability.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Energetics of oxidation and formation of uranium mononitride

Uranium mononitride (UN) is an advanced nuclear fuel currently being considered for use in several generation IV fast and thermal neutron spectrum core designs, with additional applications to thermal and electric nuclear propulsion reactors. Here, to better understand the thermal behavior and thermodynamic stability of UN, we investigated the bulk thermal oxidation process and thermochemical reactions, including the enthalpy of oxidation and standard enthalpy of formation, by conducting thermalgravimetric analysis – differential scanning calorimetry coupled with mass spectrometry (TGA-DSC-MS), and high temperature transposed temperature drop and oxide melt drop solution calorimetry. The bulk oxidation of UN (containing a small amount of α-UN 1.5+x ) in air was found to follow a step-wise process characterized by consecutive oxidative reactions UN-UN 1.5+x -UO 2 → UO 2 -UO 3 —N k → UO 3 —N k → UO 3 → U 3 O 8 . TGA results support that the UO 2 – U 2 N 3+x passivating layer delays the onset of rapid bulk oxidation of UN in air up to 662 K. Synchrotron X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS) analyses were performed to characterize UN and its final oxidized product. The standard enthalpy of formation (ΔH° f ) of UN was determined to be –144.4 ± 5.9 kJ/mol·atom, in good agreement with previously determined values from Pt encapsulation and bomb calorimetric experiments. Lastly, a negative linear correlation between ΔH° f and the N/U molar ratio was established based on the thermochemical data obtained in this work and previously reported enthalpies of formations of β-UN 1.5-x and α-UN 1.5+x .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fusion of 12 C+ 24 Mg far below the barrier: Evidence for the hindrance effect

Background: The phenomenon of fusion hindrance may have important consequences on the nuclear processes occurring in astrophysical scenarios, if it is a general behavior of heavy-ion fusion at extreme subbarrier energies, including reactions involving lighter systems, e.g., reactions in the carbon and oxygen burning stages of heavy stars. The hindrance is generally identified by the observation of a maximum of the S-factor vs energy. Whether there is an S-factor maximum at very low energies for systems with a positive fusion Q value is an experimentally challenging question. Purpose: Our aim has been to search for evidence of fusion hindrance in 12 C+ 24 Mg which is a medium-light m system with positive Q value for fusion, besides the heavier cases where hindrance is recognized to be a general phenomenon. 12 C+ 24 Mg is very close to the 16 O + 16 O and 12 C + 12 C systems that are important for the late evolution of heavy stars. Methods: The experiment has been performed in inverse kinematics using the 24 Mg beam from the XTU Tandem accelerator of LNL in the energy range 26-52 MeV with an intensity of 4-8 pnA. The targets were 12 C evaporations 50 mu g/cm 2 thick, isotopically enriched to 99.9%. The fusion-evaporation residues were detected at small angles by a E-Delta E-ToF detector telescope following an electrostatic beam deflector. Results: Previous measurements of fusion cross section for 12 C+ 24 Mg were limited to above-barrier energies. In the present experiment the excitation function has been extended down to similar or equal to 15 mu b and it appears that the S factor develops a clear maximum vs energy, indicating the presence of hindrance. This is the first convincing evidence of an S factor maximum in a medium-light system with a positive fusion Q value. These results have been fitted following a recently suggested method and a detailed analysis within the coupled-channels model that has been performed using a Woods-Saxon potential and including the ground state rotational band of 24 Mg. The coupled-channels calculations give a good account of the data near and above the barrier but overpredict the cross sections at very low energies. Conclusions: The hindrance phenomenon is clearly observed in 12 C+ 24 Mg, and its energy threshold is in reasonable agreement with the systematics observed for several medium-light systems. The fusion cross sections at the hindrance threshold show that the highest value (sigma(s) = 1.6 mb) is indeed found for this system. Therefore it may even be possible to extend the measurements further down in energy to better establish the position of the S-factor maximum.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nuclear pumped gas laser research

Nuclear pumping of lasers by fission-fragments from nuclear chain reactions is discussed. Application of the newly developed lasers to spacecraft propulsion or onboard power, to lunar bases for industrial processing, and to earth for utilization of power without pollution and hazards is envisioned. Emphasis is placed on the process by which the fission-fragement kinetic energy is converted into laser light.

Thom, K.↗

Chemical and Radiological Compatibility Testing of 3D Printed Materials

To dramatically increase the adaptability, performance, and safety of processes in support of the Defense Waste Processing Facility (DWPF), Savannah River National Lab (SRNL) plans to perform chemical and radiological compatibility testing on a wide variety of 3D printed materials of interest. The 3D printing process provides numerous strategic operational benefits such as rapid prototyping of complex designs and geometry specific to the needs of the nuclear waste disposition process, as well as on-demand rapid prototyping and iteration with materials that aren’t as accessible through traditional manufacturing methods. Reaction chemistry in simulated waste batches can be matched closely to its radioactive counterpart, but glass reactor vessels have limitations. Vessel geometry can play a big factor in mixing transport limitations, process chemistry, and degradation reaction kinetics. In addition, additive manufacturing allows for much more detailed vessel design than traditional alternatives. Waste processing techniques in DWPF also encounter extreme chemical environments including high pH, strong acids, abrasive slurries, and significant irradiation. To meet these challenges, a matrix of various polymer, ceramic, and metal additive manufacturing materials have been exposed to a suite of chemical environments of interest as well as radioactive dose (such as gamma radiation from 60 Co) to properly test their durability under these conditions. Mass change has been monitored over a period of up to a week in these conditions, as well as added characterization for surface modification through Scanning Electron Microscopy/Electron Dispersive X-ray analysis (SEM/EDX). Further chemical characterization has been monitored through Fourier-Transform InfraRed Spectroscopy (FTIR), with planned investigation via thermal and tensile strength degradation. While the direct product of this research is identification of material(s) that can withstand specific hazardous environments encountered by the mercury water wash tank in DWPF process simulation experiments, the reference base of materials will be used for many other nuclear processes in the pursuit of rapidly developed, cost-efficient, and highly specific devices for environmental remediation and much more.

Wilson, Nathan W. [Savannah River National Laborat↗

Spectroscopy of Resonances in the Astrophysical r p –Process Path. Final Technical report

This report describes the results of a project to study the spectrum of proton-resonances which determine the energy release and timescale for the astrophysical rp-process path. Steps to achieve successful experiments include the commissioning of a the in-flight radioactive-beam facility RESOLUT , development of instrumentation and analysis techniques for experiments performed with it. Radioactive-beam experiments performed in the context of the grant included the reactions 25 Al(d,n) 26 Si, 19 O(d,p) 20 O, 19 Ne(d,n) 20 Na and 17 F(d,n) 18 Ne. The experimental program developed experiments and methods to characterize aspects of proton-capture reactions with respect to the in the context of the astrophysical rp-process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Hydrochlorination of Uranium Dioxide in a Molten Salt Mixture- Phase 2: Sparged Benchtop Reaction Vessel Experiment

In 2023, Metatomic® Inc., a South Carolina based company, was awarded a Gateway for Advanced Innovation in Nuclear (GAIN) research voucher for a proposed series of experiments aimed at demonstrating the viability of a spent nuclear fuel (SNF) recycling process patented by Metatomic Inc. For the GAIN voucher, Metatomic Inc. selected Savannah River National Laboratory (SRNL) as a partner in executing the proposed proof-of-concept experiments. This report outlines the proof-of-concept experiments performed by SRNL for Metatomic Inc. during Phase 2 (of 2) experimentation. Though Phase 1 provided evidence of successful hydrochlorination, Phase 2 highlighted the nuances and challenges associated with scaling the reaction. The target UCl 4 species generated by the hydrochlorination of UO 2 generates water, which consumes UCl 4 . Compared to the single datapoint obtained at the end of the Phase 1 experiments, data collected at multiple timepoints during Phase 2 experiments indicated a presumed maximum percent conversion of 23% for this system that is likely influenced by water generation. Engineering improvements might be able to increase the percent conversion, but not likely to the degree needed for successful implementation of the technology. Moisture also presents an issue for the Hastelloy C276 reaction vessel. Eventually, corrosion will compromise the integrity of the reaction vessel, and the corrosion products could potentially affect the hydrochlorination chemistry. The presence of corrosion products, which were not produced in the Phase 1 alumina crucible, can and have created challenges when analyzing samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Uncertainties in the production of iron-group nuclides in core-collapse supernovae from Monte Carlo variations of reaction rates

Core-collapse supernovae, occurring at the end of massive star evolution, produce heavy elements, including those in the iron peak. Although the explosion mechanism is not yet fully understood, theoretical models can reproduce optical observations and observed elemental abundances. However, many nuclear reaction rates involved in explosive nucleosynthesis have large uncertainties, impacting the reliability of abundance predictions. To address this, we have previously developed a Monte Carlo-based nucleosynthesis code that accounts for reaction rate uncertainties and has been applied to nucleosynthesis processes beyond iron. Our framework is also well suited for studying explosive nucleosynthesis in supernovae. In this paper, we investigate 1D explosion models using the ‘PUSH method’ , focusing on progenitors with varying metallicities and initial masses around $M_{\rm ZAMS} = 16\, {\rm M}_{\odot }$. Detailed post-process nucleosynthesis calculations and Monte Carlo analyses are used to explore the effects of reaction rate uncertainties and to identify key reaction rates in explosive nucleosynthesis. We find that many reactions have little impact on the production of iron-group nuclei, as these elements are primarily synthesized in the nuclear statistical equilibrium. However, we identify a few ‘key reactions’ that significantly influence the production of radioactive nuclei, which may affect astrophysical observables. In particular, for the production of ${}^{44}{\rm Ti}$, we confirm that several traditionally studied nuclear reactions have a strong impact. However, determining a single reaction rate is insufficient to draw a definitive conclusion.

79 ASTRONOMY AND ASTROPHYSICS↗

Single-Step Conversion of Ethanol to n-Butene over Ag-ZrO2/SiO2 Catalysts

Ethanol is a promising platform molecule for production of a variety of fuels and chemicals. Of particular interest is producing middle distillate fuels (i.e., jet and diesel blendstock) from renewable ethanol feedstock. State-of-the-art alcohol-to-jet technology requires multiple process steps based on catalytic dehydration of ethanol to form ethylene, followed by sometimes a multi-step oligomerization, and then hydrotreatment and distillation. Here we report on a new catalytic route in which ethanol is directly converted to n-butene (1- and 2-butene mixtures) over Ag-ZrO2/SBA-16, thus offering the potential for a reduction in the number of required processing steps versus conventional alcohol-to-jet technology. This catalyst system provides the balanced metal and Lewis acid sites required to selectively facilitate a cascading sequence of reactions that includes dehydrogenation, aldol condensation, Meerwein–Ponndorf–Verley reduction, dehydration, and hydrogenation. High conversion and selectivity toward either n-butene or 1,3-butadiene is achieved by tuning the hydrogen feed partial pressure and other process/catalyst parameters. With sufficient hydrogen partial pressure 1,3-butadiene is completely and selectively hydrogenated to form n-butene. The reaction mechanism was elucidated through operando-nuclear magnetic resonance investigations coupled with reactivity measurements. Combined experimental-computational investigation reveals how changes in silver and zirconium composition and the silver oxidation state affects reactivity under controlled hydrogen partial pressures and after prolonged run times. Finally, catalyst effectiveness also was demonstrated when using wet ethanol feed, thus highlighting process flexibility in terms of feedstock purity requirements. This work was financially supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office, and was performed at the Pacific Northwest National Laboratory (PNNL) under Contract No. DE-AC05-76RL01830 and the National Renewable Energy Laboratory under Contract No. DE-AC36- 08GO28308. Part of the work conducted by S. A. Akhade was performed under the auspices of the U.S. DOE at Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. This work was partly supported through the PNNL-WSU Distinguished Graduate Research Program for ADW. NMR and XPS experiments were performed using EMSL (grid.436923.9), a DOE Office of Science User Facility sponsored by the Office of Biological and Environmental Research

Dagle, Vanessa↗

Multimessengers from the Radioactive Decay of r -process Nuclei

The radioactive β-decay of nuclei synthesized in the rapid neutron capture process (r-process) releases a variety of particles, including electrons, γ-rays, neutrinos, and neutrons. These particles provide a rich set of multimessenger signals that carry information about the astrophysical environments where neutron-rich nucleosynthesis occurs. In this work, we calculate from first principles the emission spectra resulting from the β-decay of r-process nuclei. Our approach incorporates detailed nuclear structure and decay data to model the energy distributions of each particle species. We couple the spectra with a nuclear reaction network simulation to obtain the temporal evolution of these distributions. We find that the emission distributions vary significantly in time and are nonthermal, with substantial average energies. We investigate these nuclear signals as a direct probe of heavy element formation and show that they are complementary observables to kilonova.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The abundances of nuclei in the cosmic radiation

The relative abundances are treated as a consequence of processes in cosmic ray transport occurring during passage of the radiation through interstellar material at high velocity. Some of the subjects mentioned are nuclear fragmentation and the production of secondary nuclei, nuclear reactions, energy loss and nuclear decay, ionization, the range-energy relation and propagation variables, capture and loss of electrons, the propagation of nuclei, the transport equation, equilibrium solutions, energy-dependent path length distribution, exponential path length distributions, discrete spectra, sources, supernovae, and the origin of the abundances. The connection between the space-time features of the sources, the material traversed, and the effects of magnetic fields is established by describing the particle-field interaction as a diffusive or random-walk process.

Reames, D. V.↗

Understanding the Reaction of Nuclear Graphite with Molecular Oxygen

A thorough understanding of oxidation is important when considering the health and integrity of graphite components in graphite reactors. For the next generation of graphite reactors, HTGRs specifically, an unlikely air ingress has been deemed significant enough to have made its way into the licensing applications of many international licensing bodies. While a substantial body of literature exists on nuclear graphite oxidation in the presence of molecular oxygen and significant efforts have been made to characterize oxidation kinetics of various grades, the value of existing information is somewhat limited. Often, multiple competing processes, including reaction kinetics, mass transfer, and microstructural evolution, are lumped together into a single rate expression that limits the ability to translate this information to different conditions. This article reviews the reaction of graphite with molecular oxygen in terms of the reaction kinetics, gas transport, and microstructural evolution of graphite. It also presents the foundations of a model for the graphite-molecular oxygen reaction system that is kinetically independent of graphite grade, and is capable of describing both the bulk and local oxidation rates under a wide range of conditions applicable to air-ingress.

J. Kane, Joshua↗