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At least 109 records · Page 6

Mapping of carbon concentrations in the Allende meteorite with the C-12(d,p)C-13 method

Carbon concentrations in a 4.2 x 4.2 mm area of the Allende meteorite were mapped with the C-12(d,p)C-13 nuclear method. The x,y resolution perpendicular to the deuteron beam was 65 microns; the depth resolution was 0.6 micron. The matrix of the meteorite contains about 1 wt pct carbon, which is uniformly distributed at the 65-micron level of resolution. The matrix contains most, perhaps close to all, C of this meteorite. The coarse-grained constituents, such as chondrules, show a very strong enhancement of C in the depth range 2 to about 0 micron; the matrix does not show this enhancement. The enhancement may be due to contamination of the coarse-grained areas or else to migration of C in solid solution from the interiors of comparatively large crystals to their freshly polished surfaces.

Van Der Stap, C. A. H.↗

Helium irradiated cavity formation and defect energetics in Ni-based binary single-phase concentrated solid solution alloys

In this study, binary single-phase concentrated solid solution alloys (SPCSAs), including Ni 80 Co 20 , Ni 80 Fe 20 , Ni 80 Cr 20 , Ni 80 Pd 20 , and Ni 80 Mn 20 (in atomic percentage), were irradiated with 200 keV He + ions at 500 °C. He cavity size and density distribution were systematically investigated using transmission electron microscope. Here we show that alloying elements have a clear impact on He cavity formation. Cavity size is the smallest in Ni 80 Mn 20 but the largest in Ni 80 Co 20 . Alloying elements could also substantially affect cavity density profile. In-depth examination of cavities at peak damage region (~500 nm) and at low damage region (~300 nm) demonstrates that cavity size is depth (damage) dependent. Competition between consumption and production of vacancies and He atoms could lead to varied cavity size. Density functional theory (DFT) calculations were performed to obtain the formation and migration energies of interstitials and vacancies. Combined experimental and simulation results show that smaller energy gap between interstitial and vacancy migration energies may lead to smaller cavity size and narrower size distribution observed in Ni 80 Mn 20 , comparing with Ni 80 Co 20 . Finally, the results of this study call attention to alloying effects of specific element on cavity formation and defect energetics in SPCSAs, and could provide fundamental understanding to predict radiation effects in more complexed SPCSAs, such as high entropy alloys.

36 MATERIALS SCIENCE↗

Evolution of a magnetic flux tube in two-dimensional penetrative convection

Highly supercritical compressible convection is simulated in a two-dimensional domain in which the upper half is unstable to convection while the lower half is stably stratified. This configuration is an idealization of the layers near the base of the solar convection zone. Once the turbulent flow is well developed, a toroidal magnetic field B sub tor is introduced to the stable layer. The field's evolution is governed by an advection-diffusion-type equation, and the Lorentz force does not significantly affect the flow. After many turnover times the field is stratified such that the absolute value of B sub tor/rho is approximately constant in the convective layer, where rho is density, while in the stable layer this ratio decreases linearly with depth. Consequently most of the magnetic flux is stored in the overshoot layer. The inclusion of rotation leads to travelling waves which transport magnetic flux latitudinally in a manner reminiscent of the migrations seen during the solar cycle.

Jennings, R. L.↗

Alkali metal for ultraviolet band-pass filter

An alkali metal filter having a layer of metallic bismuth deposited onto the alkali metal is provided. The metallic bismuth acts to stabilize the surface of the alkali metal to prevent substantial surface migration from occurring on the alkali metal, which may degrade optical characteristics of the filter. To this end, a layer of metallic bismuth is deposited by vapor deposition over the alkali metal to a depth of approximately 5 to 10 A. A complete alkali metal filter is described along with a method for fabricating the alkali metal filter.

Mardesich, Nick↗

Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities

Affordable sodium ion batteries hold great promise for revolutionizing stationary energy storage technologies. Sodium layered cathode materials are usually multicomponent transition metal (TM) oxides and each TM plays a unique role in the operating cathode chemistry, e.g., redox activity, structural stabilization. Engineering the three-dimensional (3D) distribution of TM cations in individual cathode particles can take advantage of a depth-dependent charging mechanism and enable a path towards tuning local TM–O chemical environments and building resilience against cathode–electrolyte interfacial reactions that are responsible for capacity fading, voltage decay and safety hazards. In this study, we create 3D compositional heterogeneity in a ternary and biphasic (O3–P3) sodium layered cathode material (Na 0.9 Cu 0.2 Fe 0.28 Mn 0.52 O 2 ). The cells containing this material deliver stable voltage profiles, and discharge capacities of 125 mA h g –1 at C/10 with almost no capacity fading after 100 cycles and 75 mA h g –1 at 1C with negligible capacity fading after 200 cycles. The direct performance comparison shows that this material outperforms other materials with similar global compositions but different mesoscale chemical distributions. Synchrotron X-ray spectroscopy/imaging and density functional theory studies reveal depth-dependent chemical environments due to changes to factors such as charge compensation and strength of orbital hybridization. Finally, 3D spectroscopic tomography illuminates the path towards optimizing multicomponent sodium layered cathode materials, to prevent the migration of TMs upon prolonged cycling. Furthermore, the study reports an inaugural effort of multifaceted and counterintuitive investigation of sodium layered cathode materials and strongly implies that there is plenty of room at the bottom by tuning nano/meso scale chemical distributions for stable cathode chemistry.

25 ENERGY STORAGE↗

Diffusion-mediated chemical concentration variation and void evolution in ion-irradiated NiCoFeCr high-entropy alloy

High-entropy alloys (HEAs) are proposed as potential structural materials for advanced nuclear systems, but little is known about the response of matrix chemistry in HEAs upon irradiation. Here, we reveal a substantial change of matrix chemical concentration as a function of irradiation damage (depth) in equiatomic NiCoFeCr HEA irradiated by 3 MeV Ni ions. After ion irradiation, the matrix contains more Fe/Cr in depth shallower than ~900–1000 nm but more Ni/Co from ~900–1000 nm to the end of the ion-damaged region due to the preferential diffusion of vacancies through Fe/Cr. Preferential diffusion also facilitates migration of vacancies from high radiation damage region to low radiation damage region, leading to no void formation below ~900–1000 nm and void formation around the end of the ion-damaged region at a fluence of 5 × 10 16 cm -2 (~123 dpa, displacements per atom, peak dose under full cascade mode). As voids grow significantly at an increased fluence (8 × 10 16 cm -2 , 196 dpa), the matrix concentration does not change dramatically due to new voids formed below ~900–1000 nm.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Diffusion-mediated chemical concentration variation and void evolution in ion-irradiated NiCoFeCr high-entropy alloy

High-entropy alloys (HEAs) are proposed as potential structural materials for advanced nuclear systems, but little is known about the response of matrix chemistry in HEAs upon irradiation. Here, we reveal a substantial change of matrix chemical concentration as a function of irradiation damage (depth) in equiatomic NiCoFeCr HEA irradiated by 3 MeV Ni ions. After ion irradiation, the matrix contains more Fe/Cr in depth shallower than ~900–1000 nm but more Ni/Co from ~900–1000 nm to the end of the ion-damaged region due to the preferential diffusion of vacancies through Fe/Cr. Preferential diffusion also facilitates migration of vacancies from high radiation damage region to low radiation damage region, leading to no void formation below ~900–1000 nm and void formation around the end of the ion-damaged region at a fluence of 5 × 10 16 cm –2 (~123 dpa, displacements per atom, peak dose under full cascade mode). As voids grow significantly at an increased fluence (8 × 10 16 cm –2 , 196 dpa), the matrix concentration does not change dramatically due to new voids formed below ~900–1000 nm.

36 MATERIALS SCIENCE↗

Transmission electron microscopy characterization of the fuel-cladding chemical interactions in HT9 cladded U-10Zr fuel

Fuel cladding chemical interaction (FCCI) is a key phenomenon needs to be better understood to establish the design basis for U-10Zr metallic fuel performance. Characterizing the microstructure and chemical composition of FCCI at micron and sub-micron scale is critically important toward a more mechanistic understanding of FCCI phenomenon and its potential effects on cladding integrity and metallic fuel performance. This paper, by using transmission electron microscopy, investigated the FCCI region in HT9 cladded U-10Zr fuel irradiated to 5.7% FIMA burnup at a peak inner cladding temperature of 615 °C in Fast Flux Test Facility (FFTF). Four distinct layers are identified in the FCCI region. The migration of Fe into the fuel side leads to the formation of several U-Zr-Fe ternary phases, including ?-Fe0.5Zr0.32U0.18, e-Fe0.3Zr0.4U0.3, and ?-Fe0.06Zr0.23U0.71, mingled with UFe2, U6Fe, and U phase at various Fe penetration depth up to ~ 150 µm. On the cladding side, grain coarsening and significant lanthanides infiltration along grain boundaries are observed. Laves phase, (Fe,Cr)2(Mo,W), which typically does not exist in fresh HT9, is identified in a wide radial range in the cladding. The typical HT9 martensitic lath structure and pre-existing M23C6 precipitates disappear, partially or completely, depending on the radial distance from the fuel-cladding interface. Those microstructural and compositional changes could cause mechanical degradation in the HT9 cladding. The present characterization results will improve the understanding of FCCI phenomenon and facilitate the development of microstructure-informed FCCI modeling for metallic fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Melt segregation from partially molten source regions - The importance of melt density and source region size

An investigation is conducted regarding the changes expected in the density contrast between basic melts and peridotites with increasing pressure using the limited data available on the compressibilities of silicate melts and data on the densities of mantle minerals. It is concluded that since compressibilities of silicate melts are about an order of magnitude greater than those of mantle minerals, the density contrast between basic melts and mantle minerals must diminish significantly with increasing pressure. An earlier analysis regarding the migration of liquid in partially molten source regions conducted by Walker et al. (1978) is extended, giving particular attention to the influence of the diminished density contrast between melt and residual crystals with increasing source region depth and to the influence of source region size. This analysis leads to several generalizations concerning the factors influencing the depths at which magmas will segregate from their source regions and the degrees of partial melting that can be achieved in these source regions before melt segregation occurs.

Stolper, E.↗

A Test of Maxwell's Z Model Using Inverse Modeling

In modeling impact craters a small region of energy and momentum deposition, commonly called a "point source", is often assumed. This assumption implies that an impact is the same as an explosion at some depth below the surface. Maxwell's Z Model, an empirical point-source model derived from explosion cratering, has previously been compared with numerical impact craters with vertical incidence angles, leading to two main inferences. First, the flowfield center of the Z Model must be placed below the target surface in order to replicate numerical impact craters. Second, for vertical impacts, the flow-field center cannot be stationary if the value of Z is held constant; rather, the flow-field center migrates downward as the crater grows. The work presented here evaluates the utility of the Z Model for reproducing both vertical and oblique experimental impact data obtained at the NASA Ames Vertical Gun Range (AVGR). Specifically, ejection angle data obtained through Three-Dimensional Particle Image Velocimetry (3D PIV) are used to constrain the parameters of Maxwell's Z Model, including the value of Z and the depth and position of the flow-field center via inverse modeling.

Anderson, J. L. B.↗

3D characterisation and quantification of an offshore freshened groundwater system in the Canterbury Bight

Although offshore freshened groundwater (OFG) systems have been documented in numerous continental margins worldwide, their geometry, controls and emplacement dynamics remain poorly constrained. Here we integrate controlled-source electromagnetic, seismic reflection and borehole data with hydrological modelling to quantitatively characterise a previously unknown OFG system near Canterbury, New Zealand. The OFG system consists of one main, and two smaller, low salinity groundwater bodies. The main body extends up to 60 km from the coast and a seawater depth of 110 m. We attribute along-shelf variability in salinity to permeability heterogeneity due to permeable conduits and normal faults, and to recharge from rivers during sea level lowstands. A meteoric origin of the OFG and active groundwater migration from onshore are inferred. However, modelling results suggest that the majority of the OFG was emplaced via topographically-driven flow during sea level lowstands in the last 300 ka. Global volumetric estimates of OFG will be significantly revised if active margins, with steep coastal topographies like the Canterbury margin, are considered.

54 ENVIRONMENTAL SCIENCES↗

Assessment of Multiple Monitoring Methods for Detection of Brine and CO2 Leakage

We assess the effectiveness of four surface-based geophysical methods and in situ monitoring of pressure and chemical changes for detecting brine and CO2 leakage from legacy wells into underground sources of drinking water (USDW) overlying a CO2 storage reservoir. This is the first such effort to evaluate and compare six monitoring methods for detection of CO2 leakage. This assessment, conducted in support of the USDOE National Risk Assessment Partnership (NRAP), utilizes 3000 synthetic data sets, generated in an uncertainty quantification (UQ) model framework. This framework combines the results of (1) a CO2 storage reservoir model of a hypothetical storage operation of 5 MT/yr for 50 years into the 1700-m deep Vedder Fm. at a site near Kimberlina, California with (2) wellbore leakage models of a legacy well and (3) multi-phase flow and reactive transport models of brine and CO2 plume migration in aquifer layers overlying the storage reservoir. Leakage drives subsurface changes, quantified by pressure plumes, CO2-saturation plumes, and total dissolved solids (TDS) plumes, the latter being related to changes in pH and species concentrations. Depending on the depth of leakage, aquifer permeability, and regional groundwater gradient, pressure plume volumes can become larger than the CO2 and TDS plumes; however, reaching detectable thresholds may take too long to be useful. For a single monitoring well located 500 m downgradient of a leaky legacy well, a depth of 570 m is found to be optimal for sampling pressure and chemical changes. We assess four surface-based geophysical monitoring methods: electrical resistivity tomography (ERT), magnetotellurics (MT), gravity, and seismic methods. Sensors cover a 4-km × 2-km area. Both ERT and MT methods are sensitive to changes in CO2 saturation and TDS concentration, whereas gravity and seismic methods detect changes in CO2 saturation. The six monitoring methods complement each other in space and time, and we find that a minimum of 20 kT of CO2 leakage is required for the leakage plume to be detected. Of the four surface-based geophysical methods, gravity monitoring appears to be the most sensitive to CO2 leaks, while the usefulness of in situ pressure and chemical monitoring will depend on the level of unfilterable background noise. Geophysical monitoring methods may detect a leak anywhere in a large area and in a large depth range, but the effectiveness of pressure and chemical monitoring depends on the number of monitoring wells, where those wells are located, and the depth of sampling. Surface-based geophysical monitoring methods are cost-effective alternatives to in situ pressure and chemical monitoring methods.

NRAP, CCS, monitoring, geophysical methods, gravit↗

Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries

The shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) are the major issues impeding the practical applications of lithium-sulfur batteries (LSBs). Herein, a highly-efficient Ni 2 P electrocatalyst supported on N, P co-doped graphene (Ni 2 P@NPG) is developed via a simple “recrystallization-self-assembly” method to address the above issues. Here, the ultrafine Ni 2 P nanoparticles ensure abundant adsorption-diffusion-conversion interfaces for accelerating LiPSs transformation and Li 2 S deposition, which extremely decreases the accumulation of LiPSs in the electrolyte and therefore prevents the migration of LiPSs. Their superior catalytic performance is demonstrated by reduced Gibbs free energy changes of rate-limiting step based on the systematic theoretical calculations and the reduced shuttle effect is tested by the three-dimensional reconstructions of Raman depth profiles. Benefiting from these synergistic effects, the LSBs with Ni 2 P@NPG modified separators present a superior cycling performance with an average capacity decay rate of 0.048 % per cycle at 1C around the 400 cycles and a high-rate capacity of 731 mAh/g at 2C. Even with a high-sulfur loading of 3.53 mg cm –2 , the cell can still contain a reversible capacity of 809 mAh/g at 0.2C with a remarkable columbic efficiency of 98.4 %.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Distribution of Tritium in the Near Surface of Type 316 Stainless Steel

The distribution of tritium in the near surface of stainless steel, type 316, has been measured using a combination of a ZnCl 2 wash and acid etching with diluted aqua regia. This method improves upon etching measurements reported in the literature: results show depth resolutions of ~10 nm using the diluted aqua regia. The ZnCl 2 wash results show very high surface concentrations (~1.5 x10 13 Bq/cm 3 ), which decreases by a factor of 10 6 after etching to a depth of ~10 um. Further, the tritium concentrations in the near surface (<10 um) of unmodified stainless-steel samples do not change significantly over the course of 233 days, which indicates a quasi-equilibrium state has been reached. Tritium migration to the surface from the subsurface region was measured by etching a sample, then storing it in air for 2 to 4 days. After storing in air, the surface concentrations increased a thousandfold and rapidly decreased to base levels after etching an additional ~2 um. Finally, these measurements indicate that perturbing the quasi-equilibrium concentration profile results in tritium migration to the surface in order to reestablish the prior equilibrium state.

36 MATERIALS SCIENCE↗

Apollo drill core depth relationships

Preliminary depth relationships are presented for the Apollo 15, 16, and 17 drill core samples. For a given depth in any of these drill stems, the in situ lunar surface depth can be estimated. Ranges of uncertainty are also established, based on percent core recovery and degree of sample disturbance. The most likely explanation for the sample disturbance observed in the top three sections of the Apollo 16 drill stem is sample migration after the stem was capped on the lunar surface; essentially no sample was lost. Similar disturbance occurred in the Apollo 17 drill core, although to a lesser degree. The average original bulk densities (i.e., before any disturbance occurred) of the Apollo 15, 16, and 17 drill cores are 1.76, 1.59, and 1.87 g/cu cm, respectively. The Apollo 15 and 17 values are probably close to the in situ values; but the Apollo 16 average in situ density could be as much as 13% less than the already low density in the drill core.

Carrier, W. D., III↗

Characterization of Oil Well Cement Performance during Early Hydration under Simulated Borehole Conditions

Summary Experiments on oil well cement (OWC) slurries were performed using the newly developed laboratory-scale wellbore simulation chamber (WSC). The WSC can simulate hydrostatic pressure reduction in the cemented annulus and possible gas migration under representative conditions. Forensic analysis shows that pressurized fluids can result in porous cement and gas channeling during cement slurry gelation. The effects of different factors on slurry pore pressure were also studied, including formation permeability, initial overburden pressure (OBP) representing the depth of interest, wellbore temperature, water/cement (w/c) ratio, cement composition, and the use of a calcium chloride (CaCl2)-based accelerator. By analyzing the temperature history of hydrating cement using degree of hydration, the evolution of cement hydration was characterized for slurry designs cured at different hydration rates. This provides the opportunity to parameterize the slurry designs and other important factors associated with wellbore conditions.

Engineering↗

X-Ray Fluorescence Solvent Detection at the Substrate-Adhesive Interface

With environmental regulations limiting the use of volatile organic compounds, low-vapor pressure solvents have replaced traditional degreasing solvents for bond substrate preparation. When used to clean and prepare porous bond substrates such as phenolic composites, low vapor pressure solvents can penetrate deep into substrate pore networks and remain there for extended periods. Trapped solvents can interact with applied adhesives either prior to or during cure, potentially compromising bond properties. Currently, methods for characterizing solvent time-depth profiles in bond substrates are limited to bulk gravimetric or sectioning techniques. While sectioning techniques such as microtome allow construction of solvent depth profiles, their depth resolution and reliability are limited by substrate type. Sectioning techniques are particularly limited near the adhesive-substrate interface where depth resolution is further limited by adhesive-substrate hardness and, in the case of a partially cured adhesive, mechanical properties differences. Additionally, sectioning techniques cannot provide information about lateral solvent diffusion. Cross-section component mapping is an alternative method for measuring solvent migration in porous substrates that eliminates the issues associated with sectioning techniques. With cross-section mapping, the solvent-wiped substrate is sectioned perpendicular rather than parallel to the wiped surface, and the sectioned surface is analyzed for the solvent or solvent components of interest using a two-dimensional mapping or imaging technique. Solvent mapping can be performed using either direct or indirect methods. With a direct method, one or more solvent components are mapped using red or Raman spectroscopy together with a moveable sample stage and/or focal plane array detector. With an indirect method, an elemental "tag" not present in the substrate is added to the solvent before the substrate is wiped. Following cross sectioning, the tag element can then be mapped by its characteristic x-ray emission using either x-ray fluorescence, or electron-beam energy-and wavelength-dispersive x-ray spectrometry. The direct mapping techniques avoid issues of different diffusion or migration rates of solvents and elemental tags, while the indirect techniques avoid spectral resolution issues in cases where solvents and substrates have adjacent or overlapping peaks. In this study, cross-section component indirect mapping is being evaluated as a method for measuring migration of d-limonene based solvents in glass-cloth phenolic composite (GCP) prior to and during subsequent bonding and epoxy adhesive cure.

Wurth, Laura↗

Wash Penalty Factors: Insight into the Effects of Water Wash Down of Building Materials for Radionuclide/Nuclear (Rn) Decontamination - 20153

The release of radiological material to the urban environment can have a devastating socio-economic impact. In an urban release scenario, areas around the dispersal epicenter and any areas contaminated via atmospheric deposition may require extensive decontamination. Most recently, our group reported the decontamination efficacy of pressurized water washing of common porous building materials, and compared the penetration depth of the contaminations before and after exposure to pressurized tap water. Here, we continue evaluation of the decontamination efficacy of wash solutions based on potassium (K{sup +}) salt for cesium (Cs), strontium (Sr), and europium (Eu) contaminations on common building surfaces. The surfaces included: the cement used in concrete, the aggregate used in concrete, intact concrete, roadway asphalt, asphalt shingles, and latex paint. We deposited solutions of {sup 137}Cs, {sup 85}Sr, and {sup 152}Eu onto numerous common building materials and exposed these materials to a static bath or low-pressure flow of tap water, 0.1 M potassium chloride (KCl), and 0.5 M KCl. The decontamination efficacy and the depth profile for residual contamination were measured to determine the conditions under which applying a wash solution has benefit compared to physically removing the surface material. To aid in these analyses, we introduced a 'wash penalty factor' to quantify the degree to which contamination migrated into the bulk material by the action of the wash method. On asphalt, 70-80% of the radionuclides were found to be within 0.02 mm of the surface. Cs{sup +} bonded to negative charge sites on the surface of the mineral aggregate (used in concrete) so decontamination was improved by ion exchange with K{sup +}. Sr{sup 2+} is soluble and removed by water, while not bonding to aggregate or demonstrating solubility in the liquid asphalt. Eu{sup 3+} is precipitated and not removed in gentle wash but displays mobility within the pore space that suggests its presence as a colloid. Concrete is more porous than asphalt, and 80% of the radionuclides were within 0.2 mm of the surface for {sup 137}Cs and {sup 152}Eu and 50- 80% for {sup 85}Sr. On concrete, Cs{sup +} bonds similarly to asphalt. Sr{sup 2+} bonds to the cement or precipitates from the alkaline pore water. Eu{sup 3+} sorbs to the cement and then precipitates. In brick, the results for Cs{sup +} and Sr{sup 2+} suggested that diffusion of ions from deeper in the coupon was important. Eu{sup 3+} is removed poorly due to precipitation. We will explain and report example wash penalty factors that vary from 0 to > 1 for the various methods and the implications for deciding when to implement wash down methods. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗