Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “induced fission”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 235 records · Page 13

Mass-asymmetric fission of 205,207,209 Bi at energies close to the fission barrier using proton bombardment of 204,206,208 Pb

Background: Recent observation of mass-asymmetric fission in neutron-deficient Hg and Pt nuclei has reignited interest in fission fragment mass distributions close to Pb. Investigations at energies close to the fission barrier, where mass-asymmetric fission is expected to be most obvious and the sensitivity to shell effects is maximized, are limited in this mass region. Purpose: To measure fission mass distributions for 205,207,209 Bi nuclei at the lowest possible excitation energies to determine how the mass distributions change with excitation energy and the neutron number of the compound nucleus. Method: Proton beams bombarding targets of 204,206,208 Pb were used to study the fission of 205,207,209 Bi at energies from just above to 10 MeV above their fission barriers. Fission fragments were measured using the CUBE fission spectrometer. Fission fragment mass distributions were determined using a newly developed time difference analysis method. Mass distributions were characterized by triple-Gaussian fits to determine the systematic trends across each isotope with excitation energy. Results: Measured mass distributions of all three Bi isotopes exhibit a component of mass-asymmetric fission at all energies studied. The probability of mass-asymmetric fission decreases significantly with increasing excitation energy, from ≈70 to ≈40% over a 10-MeV range. Comparisons between the three Bi isotopes hint at an increase in the mass-symmetric fission yield with increasing neutron number, which could be due to a decrease in the difference between the symmetric and asymmetric fission barriers. The centroids of the mass-asymmetric peaks suggest that several deformed shell gaps in the fission fragments could be contributing to the presence of the mass-asymmetric fission mode with Z light ≃ 38, Z heavy ≃ 45, and N light ≃ 56 all present in the fission fragments. Conclusions: Measurements of fission mass distributions at the lowest possible excitation energies above the fission barrier provide an excellent platform to investigate the origins of the mass-asymmetric fission mode. Finally, further systematic measurements at these energies offer an opportunity to rigorously test new models of fission in this mass region.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Quantitative Analysis of Fission-Product Surrogates in Molten Salt Chloride Aerosols

This work demonstrates laser-induced breakdown spectroscopy (LIBS) applied to a stream of aerosolized salt from molten eutectic LiCl-KCl. We demonstrate analytical capabilities to track fission-product surrogates of Cs, Sr, Pr, and Nd simultaneously, with application to monitor salts in pyroprocessing schemes and molten salt reactors. This work demonstrates limits of detection using LIBS on the order of 100 μg/g, which proves potentially applicable to monitoring fission-product concentrations in pyroprocessing applications. Additionally, this work explores fundamental aspects of plasma temperature and plasma electron density of the aerosolized species during LIBS with a specific focus on potential non-uniform plasma conditions in the aerosol.

74 - ATOMIC AND MOLECULAR PHYSICS↗

Effects of Radiation-Induced Defects on Corrosion

The next generation of nuclear reactors will expose materials to conditions that, in some cases, are even more extreme than those in current fission reactors, inevitably leading to new materials science challenges. Radiation-induced damage and corrosion are two key phenomena that must be understood both independently and synergistically, but their interactions are often convoluted. In the light water reactor community, a tremendous amount of work has been done to illuminate irradiation-corrosion effects, and similar efforts are under way for heavy liquid metal and molten salt environments. While certain effects, such as radiolysis and irradiation-assisted stress corrosion cracking, are reasonably well established, the basic science of how irradiation-induced defects in the base material and the corrosion layer influence the corrosion process still presents many unanswered questions. In this review, we summarize the work that has been done to understand these coupled extremes, highlight the complex nature of this problem, and identify key knowledge gaps.

36 MATERIALS SCIENCE↗

Refinement and demonstration of a coupled BISON-Griffin workflow for designing targeted TRISO transient experiments in TREAT

The U.S. nuclear industry is expected to deploy tristructural isotropic (TRISO) particle fuel technologies for commercial reactors within the next decade. In previous work, we defined a preliminary transient design space for TRISO fuels, identified potential gaps in the available data, and began to develop multiphysics modeling tools that could be applied to design targeted Transient Reactor Test Facility (TREAT) experiments to fill these gaps. Here, this work builds on that foundation by (1) updating BISON fuel performance and Griffin reactor physics models to reflect the current TREAT experiment tube and capsule designs, (2) coupling the codes to improve the accuracy and usability of the transient design analyses, and (3) demonstrating their use over an expanded design space that includes fuel burnup. The simulated mechanical responses of the TRISO particles were complex functions of fission product accumulation, fission gas release, and irradiation-induced dimensional change in the pyrolytic carbon layers. The predicted tangential stresses in the particles' silicon carbide layers were least compressive for preheated tests involving fresh fuels but remained compressive throughout the ranges of temperature, heat rate, and burnup considered in this work. Finally, comparisons between the potential TREAT transients and historical test reactor irradiations showed that the TREAT tests would produce significantly lower average energy deposition rates, yielding less severe transients with greater relevance to near-term commercial applications. The use of these predictive capabilities has the potential to increase the value of each test, improving the overall efficiency and cost-effectiveness of transient testing for TRISO and other advanced fuels.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Passive and active neutron signatures of 233 U for nondestructive assay

The thorium fuel cycle is emerging as an attractive alternative to conventional nuclear fuel cycles, as it does not require the enrichment of uranium for long-term sustainability. The operating principle of this fuel cycle is the irradiation of 232 Th to produce 233 U, which is fissile and sustains the fission chain reaction. 233 U poses unique challenges for nuclear safeguards, as it is associated with a uniquely extreme γ-ray environment from 232 U contamination, which limits the feasibility of the γ-ray-based assay, as well as more conservative accountability requirements than for 235 U set by the International Atomic Energy Agency. Consequently, instrumentation used for safeguarding 235 U in traditional fuel cycles may be inapplicable. It is essential that the nondestructive signatures of 233 U be characterized so that nuclear safeguards can be applied to thorium fuel-cycle facilities as they come online. In this work, a set of 233 U 3 O 8 plates, containing 984 g 233 U, was measured at the National Criticality Experiments Research Center. A high-pressure 4 He gaseous scintillation detector, which is insensitive to γ-rays, was used to perform a passive fast neutron spectral signature measurement of 233 U 3 O 8 , and was used in conjunction with a pulsed deuterium-tritium neutron generator to demonstrate the differential die-away signature of this material. Furthermore, an array of 3 He detectors was used in conjunction with the same neutron generator to measure the delayed neutron time profile of 233 U, which is unique to this nuclide. These measurements provide a benchmark for future nondestructive assay instrumentation development, and demonstrate a set of key neutron signatures to be leveraged for nuclear safeguards in the thorium fuel cycle.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Shapes of rotating normal fluid He-3 versus superfluid He-4 droplets in molecular beams

Previous single-pulse extreme ultraviolet and X-ray coherent diffraction studies revealed that superfluid 4He droplets obtained in free jet expansion acquire sizable angular momentum, resulting in significant centrifugal distortion. Similar experiments with normal fluid 3He droplets may help elucidating the origin of the of the large degree of rotational excitation and highlight similarities and differences of dynamics in normal and superfluid droplets. Here, we present the first comparison of the shapes of isolated 3He and 4He droplets following expansion of the corresponding fluids in vacuum at temperatures as low as ~ 2 K. Large 3He and 4He droplets with average radii of ~160 nm and ~350 nm, respectively, were produced. We find that the majority of the 3He droplets in the beam correspond to rotating oblate spheroids with reduced average angular momentum ($\Lambda$) and reduced angular velocities ($\Omega$) similar to that of 4He droplets. Given the different physical nature of 3He and 4He, this similarity in $\Lambda$ and $\Omega$ may be surprising and suggest that similar mechanisms induce rotation regardless of the isotope. We hypothesized that the observed distribution of droplet sizes and angular momenta stem from processes in the dense region close to the nozzle. In this region, the significant velocity spread and collisions between the droplets induce excessive rotation followed by droplet fission. The process may repeat itself several times before the droplets enter the collision-fee high vacuum region further downstream.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Excitation energy dependence of prompt fission γ-ray emission from 241 Pu*

Prompt fission γ rays (PFGs) resulting from the 240 Pu(d,pf) reaction have been measured as a function of fissioning nucleus excitation energy E x at the Oslo Cyclotron Laboratory. We study the average total PFG multiplicity per fission, the average total PFG energy released per fission, and the average PFG energy. No significant changes in these characteristics are observed over the range 5.75 < E x < 8.25 MeV. The physical implications of this result are discussed. The experimental results are compared to simulations conducted using the computational fission model FREYA. We find that FREYA reproduces the experimental PFG characteristics within 8% deviation across the E x range studied. Furthermore, previous excitation energy-dependent PFG measurements conducted below the second-chance fission threshold have large uncertainties, but are generally in agreement with our results within a 2σ confidence interval. However, both a published parametrization of the PFG energy dependence and the most recent PFG evaluation included in ENDF/B-VIII.0 were found to poorly describe the PFG excitation-energy dependence observed in this and previous experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Employing ternary fission of Pu 242 as a probe of very neutron-rich matter

Detailed assessments of the ability of recent theoretical approaches to modeling existing experimental data for ternary fission confirm earlier indications that the dominant mode of cluster formation in ternary fission is clusterization in very neutron rich, very low density, essentially chemically equilibrated, nucleonic matter. An extended study and comparison of these approaches applied to ternary fission yields in the thermal neutron induced reaction 241 Pu(n th ,f) has been undertaken to refine the characterization of the source matter. Here, the resonance gas approximation has been improved taking in-medium effects on the binding energies into account. A temperature of 1.29 MeV, density of 6.7 × 10 -5 nucleons/fm 3 and proton fraction Y p = 0.035 are found to provide a good representation of yields of the ternary emitted light particles and clusters. In particular, results for Z = 1 and 2 isotopes are presented. Isotopes with larger Z are discussed, and the roles of medium and continuum effects, even at very low density are illustrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Data Assimilation using Non-invasive Monte Carlo Sensitivity Analysis of Reactor Kinetics Parameters [Slides]

Sensitivity coefficients of prompt neutron decay constant (α) and effective delayed neutron fraction (β eff ) to Pu-239 nuclear data were calculated using a newly available tool (ACEtk). Uncertainty calculations showed the following trends: (1) The prompt neutron decay constant can be used to reduce nuclear data-induced uncertainty in Pu-239(n,f) and (2) the effective delayed neutron fraction can be used to effectively reduce nuclear data-induced uncertainty in Pu-239 total fission $\tilde{v}$. Sensitivity/uncertainty analysis can be used to determine optimal experiment/detector setup to identify compensating errors in nuclear data. Upcoming work includes investigating other nuclide-reaction pairs and response sensitivities, such as Δ$\rho$, neutron leakage spectra, and reaction rate measurements to constrain nuclear data of interest.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Mo-99 Concentration and processing by Solvent Extraction and Ion Exchange

Normally derived from its transient-equilibrium parent molybdenum-99 ( 99 Mo) (t½ = 66 h), the short-lived isotope technetium-99m ( 99m Tc) (t ½ = 6.0 h) is the most widely used medical isotope in diagnostic imaging today. The National Nuclear Security Administration’s (NNSA’s) Material Management and Minimization (M3) program—established under the auspices of the American Medical Isotope Production Act—has been tasked with facilitating the work of domestic 99 Mo suppliers that do not use highly enriched uranium (HEU). Superconducting electron linear accelerators that employ high-Z converter targets can generate bremsstrahlung photons and neutron fluxes that can induce photonuclear reactions and uranium (U) fission. Argonne, in collaboration with industrial partners, has been developing the process chemistry for superconducting linear accelerator (LINAC)-irradiated triuranium octoxide (U 3 O 8 ) targets to produce 99 Mo. In short, the process involves dissolving the irradiated targets in nitric acid, which simultaneously releases valuable fission products (xenon and iodine). After adjusting the acid concentration, producers process the feed using tri-n-butyl phosphate (TBP), then mix the raffinate derived from this extraction cycle with a phosphinic acid such as Cyanex 272 or di(2-ethylhexyl) phosphoric acid (HDEHP), which is selective for Mo (molybdenum liquid liquid extraction [MoLLE]). In the next step, a concentration column comprising an anion exchange platform is used to decontaminate the remaining fission products, generating a pure 99 Mo stream in sodium hydroxide (NaOH)/sodium chloride (NaCl).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

MESOSCALE THERMAL TRANSPORT MEASUREMENTS OF MULTI-PHASE AND POROUS NUCLEAR FUELS USING A SQUARE-WAVE PULSE THERMOREFLECTANCE TECHNIQUE

The safe and efficient operation of nuclear reactors require accurate knowledge of peak temperatures in the fuel assemblies. The temperature profiles are governed by the thermal transport properties of the fuel, namely the thermal conductivities (k) and thermal diffusivities (D). These values can be very difficult to measure as they are known to vary considerably from the measured bulk values of the fresh fuel, and quickly degrade with increasing burnup [1 -3] . Laser-based techniques have been effectively used for non-destructive and non-contact thermal transport measurements of a wide variety of materials, including nuclear materials [4-6] that would otherwise prove too hazardous or difficult to measure otherwise. In this study, a new thermoreflectance technique known as square-pulse transient thermoreflectance (SPTR) is described and used to determine the mesoscale thermal diffusivity of both uranium sesquisilicide (U3Si2) and uranium nitride (UN) phases in a composite fuel with micron level spatial resolution [7]. This technique employs a rapid train of square-wave pulses from an excitation laser to create a periodic heat flux on a gold coated sample surface. Surface adsorption results in transient film temperatures and hence rapid fluctuations in thermoreflectance that can be measured via a detection laser coupled with a digital oscilloscope. The lasers are coaxially focused on the sample surface, allowing for a sample measurement area of a single convolved laser spot size (~2 µm). A sensitivity analysis was conducted to identify key measurement parameters of this technique using reference materials with a range of thermal conductivities comparable to those of both ceramic, composite, and metal nuclear fuel types (1.4 – 27.2 W/m-K). The reference materials were measured using the new technique as well as a spatial-domain thermoreflectance technique (SDTR) previously reported for a comparison [8]. Additionally, measurements of several U3Si2 and UN phase regions of a polished UN/U3Si2 (70/30 vol.%) sample were taken, and the resulting calculated D values are reported, with both techniques showing excellent agreement between samples. This technique was used to scan a multiphase region at 5 micron increments to generate a local diffusivity map, demonstrating the utility of the techniques for measuring thermal transport properties in specimens with precipitates and secondary phases. Furthermore, the technique is currently being applied to measure thermal properties of Fast Flux Test Reactor (FFTR) irradiated metal fuel specimens whose porous microstructure make it very difficult to measure using other techniques. Comparison of the local scale measurements are compared with the pre-irradiated fuel samples to show the degradation of thermal transport in fuels due to pores from fission gas bubbles and other irradiation induced defects.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Refined BISON-Griffin Workflow For Designing Targeted TRISO Transient Experiments In The Transient Reactor Test Facility

U.S. industry is expected to deploy tristructural isotropic (TRISO) particle fuel technologies for commercial reactors within the next decade. In our previous work, we defined a preliminary transient design space for TRISO fuels, identified potential gaps in the available data, and began to develop multiphysics modeling tools that could be applied to design targeted Transient Reactor Test Facility (TREAT) experiments to fill these gaps. This work builds on that foundation by (1) updating BISON fuel performance and Griffin reactor physics models to reflect the current TREAT experiment tube and capsule designs,(2) coupling the codes to improve the accuracy and usability of the transient design analyses, and (3) demonstrating their use over an expanded design space that includes fuel burnup. The simulated mechanical responses of the TRISO particles were complex functions of fission product accumulation, fission gas release, and irradiation-induced dimensional change in the pyrolytic carbon layers. Predicted tangential stresses in particle silicon carbide layers were least compressive for preheated tests involving fresh fuels but remained compressive throughout the ranges of temperature, heat rate, and burnup considered in this work. Finally, comparisons between the potential TREAT transients and historical test reactor irradiations showed that the TREAT tests would produce significantly lower average energy deposition rates, yielding less severe transients with greater relevance to near-term commercial applications. Use of these predictive capabilities has the potential to increase the value of each test, improving the overall efficiency and cost effectiveness of transient testing for TRISO and other advanced fuels.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Probing Microstructure-induced Swelling & Thermal Property Changes in Ion-Irradiated Oxide Fuels using Laser-generated Surface Acoustic Waves

Radiation of fuel rods with neutrons during a fission reaction in a nuclear reactor is known to affect the material microstructure of the fuel as a result of fission fragment damage, and lead to the formation of atomic-level defects such as voids, dislocation loops, and lattice swelling from fission-gas release. A consequence of the radiation-induced damage in nuclear fuels is the drastic alteration of material properties, in particular, the reduction of the thermal conductivity – a key parameter that governs the transport of thermal energy released from fissile fuel atoms to the surrounding coolant. Swelling can induce high stresses and ultimate failure of the cladding. A fundamental understanding of the role of radiation-induced damage on the thermal transport and mechanical properties of nuclear fuels is therefore critical for efficient, reliable and safe operation of a nuclear power plant. As opposed to conventional post-irradiation examination techniques that are often time-consuming and require significant sample preparation, laser-based characterization methods have emerged as promising non-contact, non-destructive tools to measure the evolution of microstructure-induced material property changes. Moreover, laser methods offer the promise of in-situ characterization while the material is being irradiated. This project aims to develop an improved understanding of the impact of radiation-induced changes to material microstructure on the thermal and elastic properties of nuclear materials. A laser ultrasonic technique, known as the transient grating (TG) spectroscopy method, is used to simultaneously measure thermal diffusivity and elastic properties in unirradiated and ion-irradiated oxide nuclear fuel samples. The results will complement on-going investigations on electron- and phonon-mediated thermal transport in nuclear materials and will provide foundational work for incorporating the influence of defects in fuel performance codes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Radiation induced athermal diffusivity in uranium mononitride

Uranium mononitride (UN) is one of the ceramic nuclear fuel alternatives to oxide fuel considered for light water reactors and advanced reactor designs. Properties like self- and fission gas diffusivity need to be better understood, given that they influence key fuel performance phenomena such as fission gas swelling and release. In particular, the radiation induced athermal (D 3 ) diffusivity remains challenging to accurately predict and has only been sparsely characterized in UN, despite its importance as it likely governs diffusion at the low temperatures this high-thermal-conductivity fuel form may operate. Molecular Dynamics simulations are used to estimate the mean square displacement induced by a primary knock-on atom (PKA) with a given kinetic energy. These results are combined with the PKA energy distributions obtained from binary collision approximation calculations to obtain the displacement due to a particular fission fragment. Finally, this is combined with experimental fission fragment yields to determine the displacement due to an average fission event and, thus, express the athermal diffusivity as a function of the fission rate density. These results are in excellent agreement with available experimental data. In conclusion, a particular importance is given to the understanding and the quantification of the variability of these results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Understanding Formation of Irradiation-Induced Defects through 4D-STEM, Electron Tomography, and WBDF-STEM

A major challenge in advancing nuclear materials for next-generation fission and proposed fusion reactors is to comprehensively understand the formation of irradiation-induced defects. Here it is essential to correlate the evolution of irradiation-induced defects and the degradation of mechanical properties, as they collectively dictate the material's lifespan and ensure nuclear safety. Scanning transmission electron microscopy (STEM) based techniques have emerged as indispensable tools for irradiation-induced defect characterization, offering high spatial resolution imaging and chemical analysis, such as electron energy loss spectroscopy (EELS) and energy dispersive X-ray spectroscopy (EDXS). These techniques have been effectively used to obtain an atomic-scale view of the defect structure. Recent advances in electron microscopy, particularly in 4D-STEM, offer detailed insight into microstructural evolution by capturing full 2D diffraction patterns at every pixel position. Using high-speed direct electron detectors, this technology generates a four-dimensional dataset, overcoming the limitations of traditional STEM imaging.

36 MATERIALS SCIENCE↗

Investigating the Impacts of Direct Dissolution Conditions on the Radiolytic Longevity of Butyramide Extractants

Removing the nitric acid (HNO3) dissolution step in used nuclear fuel (UNF) reprocessing would reduce the volume of radioactive waste streams generated, thereby, improving process efficiency. A promising strategy for this is the direct dissolution of UNF that has been pretreated by voloxidation into an organic solvent composed of specialized extractants and diluent. However, removal of the aqueous HNO3 phase from the envisioned reprocessing system has the potential to drastically change the suite of radiation-induced processes occurring, and thus, alter the longevity of proposed reagents. Furthermore, the impacts of fission product and transuranic metal ion complexation on the aforementioned radiation-induced processes is poorly understood, and yet can cause significant changes in radiolytic longevity. To bridge these knowledge gaps and support the continued development of direct dissolution strategies, we present an investigation into the impacts of direct dissolution conditions on the gamma radiation-induced degradation of N,N-di-(2-ethylhexyl) butyramide (DEHBA) and N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) ligands—candidate replacements for tributyl phosphate—in pre-equilibrated n-dodecane solvent in the presence and absence of envisioned loading amounts of uranium.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Investigating the impacts of used nuclear fuel direct dissolution on the radiolytic longevity of solvent and butyramide extractants

Removing the nitric acid (HNO3) dissolution step in used nuclear fuel (UNF) reprocessing would reduce the volume of radioactive waste streams generated, thereby, improving process efficiency. A promising strategy for this is the direct dissolution of UNF that has been pretreated by voloxidation into an organic solvent composed of specialized extractants and diluent. However, removal of the aqueous HNO3 phase from the envisioned reprocessing system has the potential to drastically change the suite of radiation-induced processes occurring, and thus, alter the longevity of proposed reagents. Furthermore, the impacts of fission product and transuranic metal ion complexation on the aforementioned radiation-induced processes is poorly understood, and yet can cause significant changes in radiolytic longevity. To bridge these knowledge gaps and support the continued development of direct dissolution strategies, we present an investigation into the impacts of direct dissolution conditions on the gamma radiation-induced degradation of N,N-di-(2-ethylhexyl) butyramide (DEHBA) and N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) ligands—candidate replacements for tributyl phosphate—in pre-equilibrated n-dodecane solvent in the presence and absence of envisioned loading amounts of uranium.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Transverse Rupture Strength of Uranium Dioxide

Uranium dioxide (UO 2 ) fuel is used as fuel in light water reactors (LWRs). While the fuel pellet is technically the first engineering barrier for radionuclide release, pellet fracturing at intermediate- to high-burnup values releases fission gases into the fuel rod plenum [1, 2]. Therefore, the true engineering barrier is the fuel cladding, which performs very well in LWR environments [3]. The extreme temperature gradients generated by fission energy and the low thermal conductivity of UO 2 quickly induce radial cracking in UO 2 during operation [4]. Cracks in the fuel provide opportunities for fuel relocation, increased fission gas release, and pellet-cladding mechanical interaction (PCMI) [5]. The ability to predict and engineer the fracture of UO 2 fuel pellets using modern computational tools is therefore a key engineering goal that has been the focus of ongoing experimental and computational efforts [6, 7]. Accurate predictions of fuel pellet cracking during operation requires knowledge of more complex phenomena, but improved understanding of the fundamental fracture behavior of unirradiated UO 2 is first necessary.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗