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Microstructural heterogeneity of the buffer layer of TRISO nuclear fuel particles

Tristructural isotropic (TRISO) nuclear fuel particles contain a layered spherical shell designed to retain fission products; however, failure occurs in rare cases—commonly initiated in the porous pyrocarbon buffer layer. Achieving a comprehensive understanding of the buffer-initiated failure mechanisms requires detailed characterization of the buffer porosity and its heterogeneous distribution across multiple length scales. Here we performed FIB-SEM tomography across the buffer layer thickness (~100 µm) to produce 3D reconstructions of the buffer microstructure with 50 nm spatial resolution. We found an average overall porosity of ~14%, which does not solely account for the low density of the buffer (50% of the theoretical density). Additionally, the local porosity and its fluctuation increase from the kernel interface towards the inner pyrocarbon (IPyC) layer, which we attribute to the chemical vapor deposition process conditions during the TRISO particle fabrication. Detailed characterization of the porous microstructure—including analysis of the pore size, distribution, shape, and orientation—provides insight into the process-structure-property-performance relations of TRISO nuclear fuel particles and will inform multiscale models designed to predict the failure of TRISO particles under irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A discrete element based simulation framework to investigate particulate spray deposition processes

This work presents a computer simulation framework based on discrete element method to analyze manufacturing processes that comprise a loosely flowing stream of particles in a carrier fluid being deposited on a target surface. The individual particulate dynamics under the combined action of particle collisions, fluid–particle interactions, particle–surface contact and adhesive interactions is simulated, and aggregated to obtain global system behavior. A model for deposition which incorporates the effect of surface energy, impact velocity and particle size, is developed. The fluid–particle interaction is modeled using appropriate spray nozzle gas velocity distributions and a one-way coupling between the phases. It is found that the particle response times and the release velocity distribution of particles have a combined effect on inter-particle collisions during the flow along the spray. It is also found that resolution of the particulate collisions close to the target surface plays an important role in characterizing the trends in the deposit pattern. Analysis of the deposit pattern using metrics defined from the particle distribution on the target surface is provided to characterize the deposition efficiency, deposit size, and scatter due to collisions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Influence of Pt-Metal Alloy Catalysts with Various Ionomers on Oxygen Reduction Reaction in Fuel Cell Application

Pt-M/C (M = Co, Ni, Mn, etc.) alloy catalysts exhibit superior oxygen reduction reaction (ORR) activity compared to pure Pt/C, leading to a high energy efficiency in hydrogen fuel cells. However, many Pt-M/C alloy catalysts were synthesized and evaluated at the lab scale in model test-bed systems like rotating disc electrodes, which don't always correlate to performance within a fuel cell system; there is a clear need to evaluate catalysts in electrodes that can be prepared at industrially relevant scales to evaluate how factors like ink formulation can greatly affect device-level of fuel cell performance. Herein, three commercial Pt-M/C alloy catalysts (two Pt-Co/C and one Pt-Ni/C) were comprehensively characterized by various techniques. The results show that the average particle sizes of the three catalysts are close to 5 nm; the atomic ratio of Pt/M is around 4; and the M was successfully embedded into Pt lattice, resulting in the positive shift of Pt 4f in XPS spectra and XRD patterns. These catalytic materials were incorporated into 9 different cathode catalyst layers (CCLs) with three kinds of ionomers (Nafion D2020, high oxygen permeability ionomer (HOPI), and Aquivion D79-25BS), and their performance in proton exchange membrane fuel cells (PEMFCs) were investigated. The results demonstrate that the Pt-Co/C catalysts possess a higher mass activity (MA) than Pt-Ni/C; the cathodes with Nafion ionomer provide the highest MA while electrodes with Aquivion ionomer showed the lowest activity, attributed to poor H+ conductivity resulting from suboptimal ionomer incorporation. Finally, these alloys were shown to exceed DOE targets for MA and H2/Air performance reported in the recent publications at beginning of life and after 90k cycle catalyst AST protocol. This study provides valuable performance benchmarks for these materials guiding future Pt-M/C catalyst design and material integration for heavy duty PEMFC applications.

08 HYDROGEN↗

Dedicated beam position monitor pair for model-independent lattice characterization at NSLS-II

This paper reports recent lattice characterization results obtained at the National Synchrotron Light Source II (NSLS-II) storage ring, conducted without reliance on a lattice model. A pair of beam position monitors (BPMs) with bunch-by-bunch (B×B) resolution, were recently installed in a section of the storage ring free of magnetic fields. The new BPM pair measured the beam, or bunch’s transverse Poincar´e map precisely after the beam was excited. Linear one-turn-matrices (OTM) were then derived, and from these, the 4-dimensional coupled Twiss parameters were extracted at the locations of the BPM pair. By normalizing beam oscillation amplitudes with the Twiss parameters, the global action-variables were obtained. These action-variables facilitated the measurement of the local Twiss parameters observed by other BPMs independent on lattice model. This method is general, and particularly useful in certain scenarios such as a round beam mode in a diffraction-limited light source ring. We applied it to assess both weakly and strongly coupled lattices at the NSLS-II ring. Through analysis of the strongly coupled lattice, the quadrupole tilt errors were estimated to be less than 400 µrad. Utilizing the BPMs’ B×B resolution, for the first time we observed the variations of the linear lattice along a long bunch-train.

43 PARTICLE ACCELERATORS↗

Charging of Single Micron Sized Dust Grains by Secondary Electron Emission: A Laboratory Study

We present the details of a new laboratory study whose objective is to experimentally study the interaction of micron sized particles with plasmas and electromagnetic radiation. Specifically, to investigate under what conditions and to what extent do particles of various compositions and sizes become charged, or discharged, while exposed to an electron beam and ultraviolet radiation environment The emphasis is the study of the two charging mechanisms, secondary emission of electrons and photoelectric effect. The experiment uses a technique known as electrodynamic suspension of particles. With this technique, a single charged particle is electrodynamically levitated and then exposed to a controlled environment. Its charge to mass ratio is directly measured. Viscous drag measurements and the light scattering measurements characterize its size and optical characteristics. The environment to which the particle is expose may consist of room temperature and pressure or a rarefied atmosphere where only one major gaseous constituent is present, or, as in this case, a vacuum environment under electron bombardment or UV radiation . In addition, the environment can be cycled as part of the experiment. Therefore, using this technique, a single particle can be repeatedly exposed to a controlled environment and its response measured, or a single particle can be exposed to similar environments with minor differences and its response measured as a function of only the changed environmental conditions.

Spann, James F., Jr.↗

Mars 2001 Cruise Phase Radiation Measurments

Mars 2001 presents an exciting opportunity for advances in radiation risk management of a future human mission to Mars. The mission timing is particularly fortuitous, coming just after solar maxinuun, when there will be a high probability to observe significant solar particle events (SPEs). A major objective of this mission is to characterize the Martian radiation environment to support future human missions to Mars. In addition, the MARIE instruments on the Lander and Orbiter, designed to measure the energetic particle flux at Mars, can be used during the cruise phase to provide multipoint observations of SPEs in the critical region of the heliosphere (1 to 1.5 AU) needed to reduce the in-flight radiation risk to a future Mars-bound crew.

Turner, R. E.↗

Probing the oxidation kinetics of small permalloy particles

The oxidation of permalloys is important to apply in a wide range. The oxidation and diffusion mechanisms of small permalloy particles with different Fe content are studied by using thermal gravimetric analysis (TGA) and microstructure characterizations. Fe{sub 2}O{sub 3}/(Ni, Fe){sub 3}O{sub 4} plays a key role in the morphology evolution and diffusion mechanisms of small NiFe particles upon oxidation. The activation energies of grain boundary diffusion for the NiFe alloys increase from 141 kJ/mol to 208 kJ/mol as the Fe content increases from 0 to ~50 wt%. We have developed a diffusion process resolved temperature programed oxidation (PR-TPO) analysis method. Three diffusion mechanisms have been recognized by using this method: In addition to the grain boundary diffusion and lattice diffusion, our TGA analysis suggests that the phase conversion from Fe{sub 2}O{sub 3} to (Ni, Fe){sub 3}O{sub 4} induces diffusion change and affects the diffusion process at the intermediate temperature. Relevant oxidation kinetics and diffusion mechanisms are discussed. - Graphical abstract: The oxidation mechanisms of small Permalloy particles with different Fe content is studied by using thermal gravimetric analysis (TGA) and microstructure characterizations. The activation energies of grain boundary diffusion for the NiFe alloys increases from 140 kJ/mol to 208 kJ/mol as the Fe content increases from 0 to 50 wt% as determined by TGA. We have developed a diffusion process resolved temperature programed oxidation (DPR-TPO) analysis method, and three diffusion mechanisms have been recognized by using this method: In addition to the well-known grain boundary diffusion and lattice diffusion, we found that the phase conversion from Fe{sub 2}O{sub 3} to (Ni, Fe){sub 3}O{sub 4} will induce diffusion changes and affect the diffusion process at the intermediate temperature. The diffusion processes can be characterized by the corresponding characteristic peak temperatures in temperature programmed oxidation (TPO) analysis. This work not only give insight knowledge about the oxidation and diffusion processes of small permalloy particles, but also, provides a useful tool for analyzing solid-gas reactions of other materials. - Highlights: • The oxidation kinetics of small NiFe particles were studied by using thermoanalysis. • Grain boundary, lattice, and phase conversion induced diffusions were recognized. • The activation energy of oxidation increases with the Fe content in the alloy. • Each diffusion process corresponds to a characteristic temperature in TPO analysis. • NiFe alloys with ~5–10 wt% Fe content have the lowest oxidation rates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Science Case for a Wide Field-of-View Very-High-Energy Gamma-ray Observatory in the Southern Hemisphere

This white paper outlines the wide science program that would be enabled by the construction of a next-generation gamma-ray observatory using ground-level particle detectors in the Southern Hemisphere: the Southern Gamma-ray Survey Observatory (SGSO). This science case rests on four main pillars: unveiling galactic and extragalactic particle accelerators, monitoring the transient sky at very high energies, probing particle physics beyond the Standard Model, and the characterization of the cosmic ray flux. Several currently ongoing efforts to advance the technical performance of such an observatory will briefly be discussed in Section 8. However, the focus of this document will be on the broad spectrum of astrophysical questions SGSO will address, rather than the details of the technical implementation of a detector. To assess the potential to specific astrophysical applications, a “straw man” detector design is used. This design provides an increase in effective area, number of channels, and a lower energy threshold compared to existing observatories such as the HAWC gamma-ray observatory. Intrinsic figures of merit that quantify the potential performance of SGSO (like angular resolution and background rates) are based on the demonstrated performance of HAWC. Details on this design and its performance are given in Section 3. This approach is chosen as a balance to obtain both an ambitious and feasible performance, suitable to a wide range of applications, while keeping the assumptions about the technical implementation to a minimum. It is foreseen that some applications could benefit from enhanced performance over the straw man design in certain energy ranges; the feasibility and need of reaching enhanced performance will be discussed case by case. The outcome of the studies presented in this document will give an overview of the scientific potential of a next-generation gamma-ray observatory in the southern hemisphere and provide guidance to the finalization of the design of such an observatory.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Airborne Single Particle Mass Spectrometers (SPLAT II & miniSPLAT) and New Software for Data Visualization and Analysis in a Geo-Spatial Context

Understanding the effect of aerosols on climate requires knowledge of the size and chemical composition of individual aerosol particles - two fundamental properties that determine an aerosol’s optical properties and ability to serve as cloud condensation or ice nuclei. Here we present miniSPLAT, our new aircraft compatible single particle mass spectrometer, that measures in-situ and in real-time size and chemical composition of individual aerosol particles with extremely high sensitivity, temporal resolution, and sizing precision on the order of a monolayer. miniSPLAT operates in dual data acquisition mode to measure, in addition to single particle size and composition, particle number concentrations, size distributions, density, and asphericity with high temporal resolution. When compared to our previous instrument, SPLAT II, miniSPLAT has been significantly reduced in size, weight, and power consumption without loss in performance. We also present ND-Scope, our newly developed interactive visual analytics software package. ND-Scope is designed to explore and visualize the vast amount of complex, multidimensional data acquired by our single particle mass spectrometers, along with other aerosol and cloud characterization instruments on-board aircraft. We demonstrate that ND-Scope makes it possible to visualize the relationships between different observables and to view the data in a geo-spatial context, using the interactive and fully coupled Google Earth and Parallel Coordinates displays. Here we illustrate the utility of ND-Scope to visualize the spatial distribution of atmospheric particles of different compositions, and explore the relationship between individual particle composition and their activity as cloud condensation nuclei.

54 ENVIRONMENTAL SCIENCES↗

Three-Dimensional Mapping of Resistivity and Microstructure of Composite Electrodes for Lithium-Ion Batteries

Nanoparticle silicon–graphite composite electrodes are a viable way to advance the cycle life and energy density of lithium-ion batteries. However, characterization of composite electrode architectures is complicated by the heterogeneous mixture of electrode components and nanoscale diameter of particles, which falls beneath the lateral and depth resolution of most laboratory-based instruments. In this work, we report an original laboratory-based scanning probe microscopy approach to investigate composite electrode microstructures with nanometer-scale resolution via contrast in the electronic properties of electrode components. Applying this technique to silicon-based composite anodes demonstrates that graphite, SiOx nanoparticles, carbon black, and LiPAA binder are all readily distinguished by their intrinsic electronic properties, with measured electronic resistivity closely matching their known material properties. Resolution is demonstrated by identification of individual nanoparticles as small as ~20 nm. Our technique presents future utility in multiscale characterization to better understand particle dispersion, localized lithiation, and degradation processes in composite electrodes for lithium-ion batteries.

25 ENERGY STORAGE↗

MO-F-CAMPUS-T-05: Design of An Innovative Beam Monitor for Particle Therapy for the Simultaneous Measurement of Beam Fluence and Energy

Purpose: Monitoring the prescribed dose in particle therapy is typically carried out by using parallel plate ionization chambers working in transmission mode. The use of gas detectors has several drawbacks: they need to be calibrated daily against standard dosimeters and their dependence on beam quality factors need to be fully characterized and controlled with high accuracy. A detector capable of single particle counting is proposed which would overcome all these limitations. Combined with a gas ionization chamber, it will allow determining the average particle stopping power, thus providing an effective method for the online verification of the selected particle energy and range. Methods: Low-Gain Avalanche Detectors (LGADs) are innovative n-in-p silicon sensors with moderate internal charge multiplication occurring in the strong field generated by an additional p+ doping layer implanted at a depth of a few µm in the bulk of the sensor. The increased signal-to-noise ratio allows designing very thin, few tens of microns, segmented LGADs, called Ultra Fast Silicon Detectors (UFSD), optimized for very fast signal, which would be suitable for charged particle counting at high rates. A prototype UFSD is being designed for this purpose. Results: Different LGAD diodes have been characterized both in laboratory and beam tests, and the results compared both with those obtained with similar diodes without the gain layer and with a program simulating the signal in the sensors. The signal is found to be enhanced in LGADs, while the leakage current and the noise is not affected by the gain. Possible alternative designs and implementations are also presented and discussed. Conclusion: Thanks to their excellent counting capabilities, UFSD detectors are a promising technology for future beam monitor devices in hadron-therapy applications. Studies are ongoing to better understand their properties and optimize the design in view of this application.

61 RADIATION PROTECTION AND DOSIMETRY↗

Characterization of hypervelocity metal fragments for explosive initiation

The fragment impact response of two plastic-bonded explosive (PBX) formulations was studied using explosively driven aluminum fragments. A generic aluminum-capped detonator generated sub-mm aluminum particles moving at hypersonic velocities. The ability of these fragments to initiate reaction or otherwise damage two PBX materials was assessed using go/no-go experiments at standoff distances of up to 160 mm. Lower density PBX 9407 (RDX-based) was initiable at up to 115 mm, while higher density PBX 9501 (HMX-based) was only initiable at up to 6 mm. Several techniques were used to characterize the size, distribution, and velocity of the particles. Witness plate materials, including copper and polycarbonate, and backlit high speed video were used to characterize the distribution of particles, finding that the aluminum cap did not fragment homogeneously but rather with larger particles in a ring surrounding finer particles. Finally, precise digital holography experiments were conducted to measure the three-dimensional shape and size of the fastest-moving fragments, which ranged between 100 and 700 μm and traveled between 2.2 and 3.2 km/s. Crucially, these experiments showed variability in the fragmentation in terms of the number of fragments at the leading edge of the fragment field, indicating that both single and multiple shock impacts could be imparted to the target material. As a result, these types of data are critical for safety experiments and hydrocode simulations to quantify shock-to-detonation transition mechanisms and the associated risk-margins for these materials.

36 MATERIALS SCIENCE↗

Evaluation of energetic particle effects on BUV data and atmospheric ozone

To aid investigations of energetic particle effects on the backscattered ultraviolet (BUV) instrumentation aboard Nimbus 4, solar proton events characterized as polar cap absorption events occurring in the period April 1970 to April 1976 were summarized. Energetic particle effects on total ozone above the 4 mb pressure level measured by Nimbus 4 were analyzed. Proceedings of a workshop meeting of operation aurorozone are included as background material for possible effects of bremsstrahlung on atmospheric ozone.

Herman, J. R.↗

In-Situ Liquid Cell Transmission Electron Microscopy of Nanoparticles from Spent Nuclear Fuel

Noble Metal Particles (NMP) that are present in SNF play an important role in the Fuel Matrix Degradation (FMD) Model that is being considered for predicting the release rate of radionuclides from a waste package. Previous characterization of chemically separated NMP from SNF showed that these were well-crystallized nanoparticles containing Mo, Tc, Ru, Rh, and Pd with some evidence of actinides. These same chemically separated particles were re-characterized following 10 years of storage as the separated material in water. Scanning Transmission Electron Microscopy (STEM) analysis revealed that significant alteration had occurred in this material during storage, resulting in the almost complete degradation of the NMP. We hypothesized that radiolytic damaged had occurred in the material. To support these concepts, we synthesized a mixed Ru-Pd nanoparticle and subjected it to irradiation in the electron microscope in an in-situ liquid cell. We demonstrated that intense radiation can lead to the decomposition of these metallic particles.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Studying Corrosion Using Miniaturized Particle Attached Working Electrodes and the Nafion Membrane

We developed a new approach to attach particles onto a conductive layer as a working electrode (WE) in a microfluidic electrochemical cell with three electrodes. Nafion, an efficient proton transfer molecule, is used to form a thin protection layer to secure particle electrodes. Spin coating is used to develop a thin and even layer of Nafion membrane. The effects of Nafion (5 wt% 20 wt%) and spinning rates were evaluated using multiple sets of replicates. The electrochemical performance of various devices was demonstrated. Additionally, the electrochemical performance of the devices is used to select and optimize fabrication conditions. The results show that a higher spinning rate and a lower Nafion concentration (5 wt%) induce a better performance, using cerium oxide (CeO2) particles as a testing model. The WE surfaces were characterized using atomic force microscopy (AFM), scanning electron microscopy-focused ion beam (SEM-FIB), time-of-flight secondary ion mass spectrometry (ToF-SIMS), and X-ray photoelectron spectroscopy (XPS). The comparison between the pristine and corroded WE surfaces shows that Nafion is redistributed after potential is applied. Our results verify that Nafion membrane offers a reliable means to secure particles onto electrodes. Furthermore, the electrochemical performance is reliable and reproducible. Thus, this approach provides a new way to study more complex and challenging particles, such as uranium oxide, in the future.

42 ENGINEERING↗

Chemical and structural characterization of particulate fallout isolated from air-filters

We report particulate nuclear fallout is the radioactive byproduct of a nuclear event formed by the mixture of proximate environmental materials with vaporized bomb debris. The fallout debris can be transported into the atmosphere during cloud rise, raining out locally and dispersing globally constituting a radiation hazard and contributing to the distribution of anthropogenic radionuclides in the environment. Questions remain on how entrainment of environmental material in the fireball affects fallout formation processes and radionuclide incorporation and distribution during cooling. To inform the characterization of fallout including the development of fallout size distributions and how radionuclides are incorporated into fallout debris where entrainment plays a role, we analyzed an archived historic US air-filter collected by aircraft in the aftermath of ground interacting nuclear tests. Particulate fallout collected on the filter was isolated and analyzed using scanning electron microscopy (SEM), transmission electron microscopy (TEM) and NanoSIMS (Secondary Ion Mass Spectrometry) to determine chemistry, structure, morphology, and size of the particles. Results demonstrate that the particles isolated from the filter have spherical shape, display complex internal structures, and are mainly composed of Fe and Si oxides. In these spherical particles, Pu is preferentially associated with Fe-rich composition. The characterization of fallout particulate samples can provide information on nucleation and particle growth from the vapor phase to improve modeling and simulation of fallout hazards.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Single-Particle Studies Reveal a Nanoscale Mechanism for Elastic, Bright, and Repeatable ZnS:Mn Mechanoluminescence in a Low-Pressure Regime

Mechanoluminescent materials, which emit light in response to elastic deformation, are demanded for use as in situ stress sensors. ZnS doped with Mn is known to exhibit one of the lowest reported thresholds for appearance of mechanoluminescence, with repeatable light emission under contact pressure <10 MPa. Here, the physical basis for such behavior remains as yet unclear. Here, reliable microscopic detection of mechanoluminescence of single ZnS:Mn microparticles, in combination with nanoscale structural characterization, provides evidence that the mechanoluminescent properties of these particles result from interplay between a non-centrosymmetric crystal lattice and its defects, viz., dislocations and stacking faults. Statistical analysis of the distributions of mechanoluminescence energy release trajectories reveals two distinct mechanisms of excitation: one attributable to a piezo-phototronic effect and the other due to dislocation motion. At pressures below 8.1 MPa, both mechanisms contribute to mechanoluminescent output, with a dominant contribution from the piezo-phototronic mechanism. In contrast, above 8.1 MPa, dislocation motion is the primary excitation source. For the piezo-phototronic mechanism, we propose a specific model that accounts for elastic ZnS:Mn mechanoluminescence under very low pressure. The charged interfaces in stacking faults lead to the presence of filled traps, which otherwise would be empty in the absence of the built-in electric field. Upon application of external stress, local enhancement of the piezoelectric field at the stacking faults’ interfaces facilitates release of the trapped carriers and subsequent luminescence. This field enhancement explains how <10 MPa pressure produces thousands of photons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characterization of wear debris generated in accelerated rolling-element fatigue tests

A ferrographic analysis was used to determine the types and quantities of wear debris generated during accelerated rolling contact fatigue tests. The five-ball rolling contact fatigue tester was used. Ball specimens were made of a corrosion resistant, high-temperature bearing steel. The lubricant was a superrefined naphthenic mineral oil. Conditions included a maximum Hertz stress of 5.52 10 to the 9th power Pa and a shaft speed of 10,000 rpm. Four types of wear debris were observed: (1) normal rubbing wear particles, (2) fatigue microspall particles, (3) spheres, and (4) friction polymer deposits. The characterization of wear debris as a function of time was of limited use in predicting fatigue failures in these accelerated tests.

Jones, W. R., Jr.↗