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At least 325 records · Page 18

Assessment of tritium effluent from Prototype Generation IV Sodium-cooled Fast Reactor

We report a tritium transport model for a pool-type sodium cooled fast reactor was developed for estimation of tritium effluents from the Prototype Generation IV Sodium-cooled Fast Reactor (PGSFR). For this purpose, the transport model developed for Experimental Breeder Reactor II and Fast Flux Test Facility was updated and validated. The tritium production rate from ternary fission and activations in PGSFR were calculated by the Argonne Reactor Computation (ARC) code suite for fast reactor analysis, and due to the potential uncertainties in source terms and variations of cold trap performance and material permeability during reactor operation, the tritium distributions and tritium effluents were estimated for several bounding cases. The upper bounding gaseous and liquid tritium release rates from PGSFR are similar to ~440.7 Ci/year and 14.7 Ci/year, respectively. The gaseous tritium effluent is about few orders of magnitude smaller than the regulatory constraint of the tritium concentration in the air. The peak tritium concentration in the steam-generator feedwater is similar to ~1.1x10 -3 mu Ci/g, which is required to be diluted prior to releasing as tritiated water. The accumulated tritium in the cold trap after five cycle operations is ~ 52,000 Ci. Because of significant conservatism in these upper bounding estimations, it is expected that the tritium effluent at the nominal case with plausible source terms would be about 2 orders of magnitude smaller than that of the upper bounding case.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Harvesting krypton isotopes from the off-gas of an irradiated water target to generate 76Br and 77Br

Abstract A flowing-water target was irradiated with a 150 MeV/nucleon beam of 78 Kr at the National Superconducting Cyclotron Laboratory to produce 77 Kr and 76 Kr. Real-time gamma-imaging measurements revealed the mass transport of the krypton radioisotopes through the target-water processing, or “isotope harvesting”, system. The production rates were determined to be 2.7(1) × 10 –4 nuclei of 76 Kr and 1.18(6) × 10 –2 nuclei of 77 Kr formed per incident 78 Kr ion. Utilizing an off-gas processing line as part of the isotope harvesting system, a total of 7.2(1) MBq of 76 Kr and 19.1(6) MBq of 77 Kr were collected in cold traps. Through the decay, the daughter radionuclides 76 Br and 77 Br were generated and removed from the traps with an average efficiency of 77 ± 12%. Due to the differences in half-lives of 76 Kr and 77 Kr, it was possible to isolate a pure sample of 76 Br with 99.9% radionuclidic purity. The successful collection of krypton radioisotopes to generate 76 Br and 77 Br demonstrates the feasibility of gas-phase isotope harvesting from irradiated accelerator cooling-water. Larger-scale collections are planned for collecting by-product radionuclides from the Facility for Rare Isotope Beams.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

76535 - An old lunar rock

Measurements of Rb-Sr systematics, K-Ar gas retention ages, and the isotopic compositions of He, Ne, and Ar have been performed for lunar troctolite 76535. Other investigators have presented evidence that this important rock formed as a cumulate at depth, which would make it an important link in the early chronology of the moon. Rb-Sr data do not define an isochron. Total Ar-40/K ages of whole rock and plagioclase range from 4.40-4.54 b.y. The trapped Ne and Ar in 76535 cannot be uniquely characterized as either 'planetary derived' or solar wind derived, but appear to have characteristics of both. The data suggest that 76535 formed 4.3-4.6 b.y. ago, and the accumulation process and/or subsequent annealing may have incorporated excess noble gases. Separation of radiogenic parents and daughters with incomplete isotopic equilibration may also have occurred during cooling or during a subsequent 'event'.

Bogard, D. D.↗

A Glass Spherule of Questionable Impact Origin from the Apollo 15 Landing Site: Unique Target Mare Basalt

A 6 mm-diameter dark spherule, 15434,28, from the regolith on the Apennine Front at the Apollo 15 landing site has a homogeneous glass interior with a 200 microns-thick rind of devitrified or crystallized melt. The rind contains abundant small fragments of Apollo 15 olivine-normative mare basalt and rare volcanic Apollo 15 green glass. The glass interior of the spherule has the chemical composition, including a high FeO content and high CaO/Al2O3, of a mare basalt. Whereas the major element and Sc, Ni, and Co abundances are similar to those of low-Ti mare basalts, the incompatible elements and Sr abundances are similar to those of high-Ti mare basaits. The relative abundance patterns of the incompatible trace elements are distinct from any other lunar mare basalts or KREEP; among these distinctions are a much steeper slope of the heavy rare earth elements. The 15434,28 glass has abundances of the volatile element Zn consistent with both impact glasses and crystalline mare basalts, but much lower than in glasses of mare volcanic origin. The glass contains siderophile elements such as Ir in abundances only slightly higher than accepted lunar indigenous levels, and some, such as Au, are just below such upper limits. The age of the glass, determined by the Ar-40/Ar-39 laser incremental heating technique, is 1647 +/- 11 Ma (2 sigma); it is expressed as an age spectrum of seventeen steps over 96% of the Ar-38 released, unusual for an impact glass. Trapped argon is negligible. The undamaged nature of the sphere demonstrates that it must have spent most of its life buried in regolith; Ar-38 cosmic ray exposure data suggest that it was buried at less than 2m but more than a few centimeters if a single depth is appropriate. That the spherule solidified to a glass is surprising; for such a mare composition, cooling at about 50 C/s is required to avoid crystallization, and barely attainable in such a large spherule. The low volatile abundances, slightly high siderophile abundances, and the young age are perhaps all most consistent with an impact origin, but nonetheless not absolutely definitive.

Ryder, Graham↗

Water Injected Turbomachinery

From antiquity, water has been a source of cooling, lubrication, and power for energy transfer devices. More recent applications in gas turbines demonstrate an added facet, emissions control. Fogging gas turbine inlets or direct injection of water into gas turbine combustors, decreases NOx and increases power. Herein we demonstrate that injection of water into the air upstream of the combustor reduces NOx by factors up to three in a natural gas fueled Trapped Vortex Combustor (TVC) and up to two in a liquid JP-8 fueled (TVC) for a range in water/fuel and fuel/air ratios.

Hendricks, R. C.↗

Franck-Condon Tuning of Optical Cycling Centers by Organic Functionalization

Laser induced electronic excitations that spontaneously emit photons and decay directly to the initial ground state (“optical cycling transitions”) are used in quantum information and precision measurement for state initialization and readout. To extend this primarily atomic technique to large, organic compounds, we theoretically investigate optical cycling of alkaline earth phenoxides and their functionalized derivatives. We find that optical cycle leakage due to wave function mismatch is low in these species, and can be further suppressed by using chemical substitution to boost the electron-withdrawing strength of the aromatic molecular ligand through resonance and induction effects. This provides a straightforward way to use chemical functional groups to construct optical cycling moieties for laser cooling, state preparation, and quantum measurement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A passively pumped vacuum package sustaining cold atoms for more than 200 days

Compact cold-atom sensors depend on vacuum technology. One of the major limitations to miniaturizing these sensors is the active pumps—typically ion pumps—that are required to sustain the low pressure needed for laser cooling. Although passively pumped chambers have been proposed as a solution to this problem, technical challenges have prevented successful operation at the levels needed for cold-atom experiments. The authors present the first demonstration of a vacuum package successfully independent of ion pumps for more than a week; their vacuum package is capable of sustaining a cloud of cold atoms in a magneto-optical trap (MOT) for greater than 200 days using only non-evaporable getters and a rubidium dispenser. Measurements of the MOT lifetime indicate that the package maintains a pressure of better than 2×10−7 Torr. This result will significantly enable the development of compact atomic sensors, including those sensitive to magnetic fields, where the absence of an ion pump will be advantageous.

Little, Bethany J. (ORCID:0000000332892798)↗

Role of surface diffusion in formation of unique reactivity for graphite oxidation: Time-resolved measurements in a pulsed diffusion reactor

Quantification of oxidation kinetics is essential to develop graphitic materials for diverse applications: from refractories found in gas-cooled nuclear reactors to catalysts needed for chemical manufacturing. In this work, using well-defined highly oriented pyrolytic graphite, low-pressure isotopic transient experiments combined with controlled annealing periods, we resolve the role of surface diffusion and quantify oxidation kinetics with nanomole-precision. We observe an unexpected increase in reactivity following annealing which is explained by the role of surface diffusion increasing the probability for trapping mobile oxygen at more reactive edge sites. Here, the locus of adsorption and spillover to the basal plane is distinct from the trapping location creating a more active oxygen species. Isotopic products reflect the population dynamics of oxygen added at the edge and surface diffusion that relocates basal plane oxygen to more reactive edge sites. Since this process proceeds in parallel with direct oxidation reactions, it is not likely to be observed using steady-state or conventional ‘bulk’ characterization techniques. Our unique time-resolved non-equilibrium measurement in a well-defined transport regime, enables observation of three distinct behaviors: short-term deactivation due to the balance of rates in oxygen supply/product formation, reactivity increases due to surface diffusion and longer-term reactivity increase with oxygen accumulation.

36 MATERIALS SCIENCE↗

Axions and SN1987A

The effect of free-streaming axion emission on numerical models for the cooling of the newly born neutron star associated with SN1987A is considered. It is found that for an axion mass of greater than approximately 10 to the -3 eV, axion emission shortens the duration of the expected neutrino burst so significantly that it would be inconsistent with the neutrino observations made by the Kamiokande II and Irvine-Michigan-Brookhaven detectors. However, the possibility has not been investigated that axion trapping (which should occur for masses greater than or equal to 0.02 eV) sufficiently reduces axion emission so that axion masses greater than approximately 2 eV would be consistent with the neutrino observations.

Burrows, Adam↗

Acoustic composition sensor for cryogenic gas mixtures

An acoustic sensor useful for the determination of the composition of a gaseous binary mixture in cryogenic liquid spills has been characterized. One version of the instrument traps a known mixture of helium and nitrogen at ambient temperature in a tube which is interrogated by sonic pulses to determine the speed of sound and hence the composition. Experimental data shows that this sensor is quite accurate. The second version uses two unconfined microphones which sense sound pulses. Experimental data acquired during mixing when liquid nitrogen is poured into a vessel of gaseous helium is presented. Data during transient cooling of the tubular sensor containing nitrogen when the sensor is dipped into liquid nitrogen and during transient warm-up when the sensor is withdrawn are also presented. This sensor is being developed for use in the mixing of liquid cryogens with gas evolution in the simulation of liquid hydrogen/liquid oxygen explosion hazards.

Shakkottai, P.↗

AGR-5/6/7 Irradiation As Run Predictions Using PARFUME

The PARticle FUel ModEl (PARFUME), a fuel performance modeling code used for high-temperature gas-cooled reactors, was used to model the Advanced Gas Reactor (AGR)-5/6/7 irradiation test using as-run physics and thermal data. The AGR-5/6/7 irradiation test consists of the combined fifth, sixth, and seventh planned irradiations of the AGR Fuel Development and Qualification Program. The AGR-5/6/7 test train is a multi-capsule, instrumented experiment that is designed for irradiation in the 133.4-mm diameter northeast flux trap position of the Advanced Test Reactor (ATR) at Idaho National Laboratory. Each capsule contains compacts filled with uranium oxycarbide unaltered fuel particles. This report documents the calculations performed to predict the failure probability of tristructural isotropic (TRISO)-coated fuel particles during the AGR-5/6/7 experiment. In addition, this report documents the calculated fission product release fraction from the fuel. The calculations include modeling of the AGR 5/6/7 irradiation that occurred from February 2018 to July 2020 over nine ATR cycles, including six normal cycles and three power axial locator mechanism cycles, for a total of approximately 376 effective full power days (EFPD). The irradiation conditions and material properties of the AGR-5/6/7 test predicted zero fuel particle failures in Capsules 1, 3, and 4. Fuel particle failures were predicted in two of the compacts in Capsule 2 and one particle failure is predicted in each one of the compacts in Capsule 5. All compacts that exhibited fuel particle failures predicted by PARFUME were caused by localized stress concentrations in the silicon carbide (SiC) layer caused by cracking in the inner pyrolytic (IPyC) layer. In addition, shrinkage of the buffer and IPyC layer during irradiation resulted in formation of a buffer-IPyC gap. Compacts with a lower irradiation temperature and fluence experienced the smallest buffer-IPyC gap formation. Conversely, higher irradiated temperature compacts with a high fluence experienced the largest buffer-IPyC gap formation. Compact 3-6-3 experienced the largest buffer IPyC gap formation of just under 21.7 µm. The release fraction of fission products silver (Ag), cesium (Cs), and strontium (Sr) vary depending on capsule location and irradiation temperature. The maximum release fraction of Ag occurs in Capsule 3, reaching up to 59.5% for the TRISO fuel particles (compact 3-6-3). The release fraction of the other two fission products, Cs and Sr, are much smaller. A maximum Cs release fraction of 1.1% occurred in compact 3-4-3 and 4.4% for Sr in compact 3-6-3.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Initial Observations from AGR 5/6/7 Capsule 1

The fourth and final irradiation experiment in the Advanced Reactor Technologies (ART) Advanced Gas Reactor (AGR) fuel development and qualification program is designated as AGR-5/6/7. Data collected from the fabrication, irradiation, and post-irradiation examination (PIE) of this tristructural isotropic (TRISO) fuel are intended to serve as the primary data set for the qualification of this fuel for use in high-temperature gas-cooled reactors (INL 2021, Collin 2018b). However, data collected from the three preceding irradiations (i.e., AGR-1, AGR-2, and AGR-3/4) may also be used to supplement data collected from AGR-5/6/7. All components of the AGR-5/6/7 fuel (i.e., UCO kernels, TRISO coatings, and fuel compacts) were produced on an engineering scale at BWXT (Lynchburg, Virginia USA) according to the fuel specification (Marshall 2017). This fuel was irradiated in the northeast flux trap (NEFT) at the Advanced Test Reactor (ATR) at Idaho national Laboratory (INL) from February 16, 2018 to July 22, 2020 (Pham et al. 2021). Measurements in the fission product monitoring system (FPMS) indicated unexpected and significant numbers of failures of TRISO particles in Capsule 1 near the end of the sixth irradiation cycle (ATR Cycle 166A). In the fourth cycle (ATR Cycle 164B) and beyond, the sweep gas flow became very low (presumably from degradation of the capsule gas outlet line via an unidentified mechanism), and the program deliberately isolated Capsule 1 from gas flow periodically. In later cycles, attempts to reestablish any kind of flow in Capsule 1 were unsuccessful. With little or no flow through Capsule 1, FPMS measurements and enumerations of failed particles in Capsule 1 were difficult or impossible as was the ability to control the helium/neon gas mixture used for temperature control. Gas flows and fission gas activity in the effluent gas from the other AGR-5/6/7 capsules were also impacted by the Capsule 1 gas flow issues and the large increase in fission gas released from the Capsule 1.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Accretion disks around black holes

The physics of accretion flow very close to a black hole is dominated by several general relativistic effects. It cannot be described by the standard Shakura Sunyaev model or by its relativistic version developed by Novikov and Thome. The most important of these effects is a dynamical mass loss from the inner edge of the disk (Roche lobe overflow). The relativistic Roche lobe overflow induces a strong advective cooling, which is sufficient to stabilize local, axially symmetric thermal and viscous modes. It also stabilizes the non-axially-symmetric global modes discovered by Papaloizou and Pringle. The Roche lobe overflow, however, destabilizes sufficiently self-gravitating accretion disks with respect to a catastrophic runaway of mass due to minute changes of the gravitational field induced by the changes in the mass and angular momentum of the central black hole. One of the two acoustic modes may become trapped near the inner edge of the disk. All these effects, absent in the standard model, have dramatic implications for time-dependent behavior of the accretion disks around black holes.

Abramowicz, M. A.↗

Small-Scale Gravity Waves in ER-2 MMS/MTP Wind and Temperature Measurements during CRYSTAL-FACE

Lower stratospheric wind and temperature measurements made from NASA's high-altitude ER-2 research aircraft during the CRYSTAL-FACE campaign in July 2002 were analyzed to retrieve information on small scale gravity waves (GWs) at the aircraft's flight level (typically approximately 20 km altitude). For a given flight segment, the S-transform (a Gaussian wavelet transform) was used to search for and identify small horizontal scale GW events, and to estimate their apparent horizontal wavelengths. The horizontal propagation directions of the events were determined using the Stokes parameter method combined with the cross S-transform analysis. The vertical temperature gradient was used to determine the vertical wavelengths of the events. GW momentum fluxes were calculated from the cross S-transform. Other wave parameters such as intrinsic frequencies were calculated using the GW dispersion relation. More than 100GW events were identified. They were generally high frequency waves with vertical wavelength of approximately 5 km and horizontal wavelength generally shorter than 20 km. Their intrinsic propagation directions were predominantly toward the east, whereas their ground-based propagation directions were primarily toward the west. Among the events, approximately 20% of them had very short horizontal wavelength, very high intrinsic frequency, and relatively small momentum fluxes, and thus they were likely trapped in the lower stratosphere. Using the estimated GW parameters and the background winds and stabilities from the NCAR/NCEP reanalysis data, we were able to trace the sources of the events using a simple reverse ray-tracing. More than 70% of the events were traced back to convective sources in the troposphere, and the sources were generally located upstream of the locations of the events observed at the aircraft level. Finally, a probability density function of the reversible cooling rate due to GWs was obtained in this study, which may be useful for cirrus cloud models.

Wang, L.↗

Single Ru(II) Ions on Ceria as a Highly Active Catalyst for Abatement of NO

Atom trapping leads to catalysts with atomically dispersed Ru 1 O 5 sites on (100) facets of ceria, as identified by spectroscopy and DFT calculations. This is a new class of ceria-based materials with Ru properties drastically different from the known M/ceria materials. They show excellent activity in catalytic NO oxidation, a critical step that requires use of large loadings of expensive noble metals in diesel aftertreatment systems. Ru 1 /CeO 2 is stable during continuous cycling, ramping, and cooling as well as the presence of moisture. Furthermore, Ru 1 /CeO 2 shows very high NO x storage properties due to formation of stable Ru–NO complexes as well as a high spill-over rate of NO x onto CeO 2 . Only ~0.05 wt % of Ru is required for excellent NO x storage. Ru 1 O 5 sites exhibit much higher stability during calcination in air/steam up to 750 °C in contrast to RuO 2 nanoparticles. Here we clarify the location of Ru(II) ions on the ceria surface and experimentally identify the mechanism of NO storage and oxidation using DFT calculations and in situ DRIFTS/mass spectroscopy. Moreover, we show excellent reactivity of Ru 1 /CeO 2 for NO reduction by CO at low temperatures: only 0.1–0.5 wt % of Ru is sufficient to achieve high activity. Modulation-excitation in situ infrared and XPS measurements reveal the individual elementary steps of NO reduction by CO on an atomically dispersed Ru ceria catalyst, highlighting unique properties of Ru 1 /CeO 2 and its propensity to form oxygen vacancies/Ce +3 sites that are critical for NO reduction, even at low Ru loadings. Our study highlights the applicability of novel ceria-based single-atom catalysts to NO and CO abatement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fractionation Trends Among IVA Iron Meteorites: Contrasts with IIIAB Trends

A neutron-activation study of 49 group-IVA irons shows much lower negative slopes on Ir-Au and Ir-As diagrams than observed in the larger magmatic group IIIAB. This difference seems to reflect the tendency of D(sub Ir), D(sub Au), and D(sub As) to increase with increasing S content. Contents of S and other volatiles are much lower in IVA irons than IIIAB irons. We show that both groups can be fit with Dx values that depend quadratically on S, with initial IVA S contents about 6X lower than those in IIIAB. The IVA scatter fields show a spread in Au or As at constant Ir that appears to reflect variations in the fraction of trapped melt between 0% and 30%. Copper shows an S-shaped trend that may reflect moderate positive and negative changes in D(sub Cu) as the magma evolved or, less likely, sampling variations in a broad band reflecting fractionation and trapping of melt. Gibeon, the largest IVA iron with a mass greater than 30 tons, shows an appreciable range in compositions consistent either with differences in the degree of magma crystallization or with differences in the content of trapped melt. A striking difference between IVA and IIIAB is observed in the Ir/Au ratios in the most Ir-rich irons in the groups; that in IVA is 40% lower than the IIIAB ratio, and lower than those in other iron-meteorite groups, The IVA Ir/Au ratio is about half the ratios in the chondrite groups. We examined three possible explanations of this anomaly: (1) the high-Ir irons contain large amounts of trapped melt: or (2) half of the IVA core (i.e., the first 50% to crystallize) is missing from the terrestrial set of IVA irons; or (3) the IVA magma formed by incomplete melting of the metal in the chondritic precursor material, with the metal that remained in the mantle having high Ir and low Au contents. Plausibility arguments favor the third possibility. The third scenario is the most plausible, but the second cannot be ruled out. We review recent evidence regarding the cooling rates in group IVA. In contrast to recent interpretations, we note several lines of evidence that indicate constant cooling rates independent of composition, as expected if all IVA meteorites were in the same core when cooling between 900 and 650 K occurred.

Wasson, J. T.↗

Cosmochemical Studies: Meteorites, Asteroidal Processes, Chondrules

Our research mainly concerned the asteroidal processes involved in the formation of meteorites and meteoritic chondrules. We continued to generate large amounts of instrumental-neutron-activation analysis (INAA) data, both for irons, chondrites and primitive achondrites. Major themes of our chondrule research were: (1) the temperature and crystallization history of individual chondrules, and (2) the evolution of the solar nebula during the period within which chondrule formation occurred. Much of our chondrule research was focused on the highly primitive CO3 chondrites. We initiated a study of the cooling history of high-FeO chondrules by characterizing the overgrowth layers on relict grains.. We also continued our studies of the composition and the formation of iron meteorites and the evolution of their parent planets. The large data sets that we have generated at UCLA allows systematic comparisons of the large magmatic groups both in terms of fractional crystallization (including rough estimates of non-metal contents of the parental melts) and in terms of the effects of variable contents of trapped melt. We have completed a preliminary study of group IIIAB in which we developed a trapped-melt model and more detailed studies of group IVA and the main-group pallasites. By comparing these large groups and modeling them by a combination of crystallization and melt trapping, we are able to better define both the formation processes and the nature of the solid/liquid elemental partitioning. We helped maintain the excellent neutron-activation facilities at UCLA, a major resource for the cosmochemical community.

Wasson, John T.↗

Structural Characterization of Crystalline Ice Nanoclusters

Water ice nanoclusters are useful analogs for studying a variety of processes that occur within icy grains in the extraterrestrial environment. The surface of ice nanoclusters prepared in the laboratory is similar to the surface of interstellar ice grains. In cold molecular clouds, the silicate cores of interstellar grains are typically approx. 100 nm in diameter and have a coating of impure amorphous water ice. Depositional, thermal and radiolytic processes leave the surface and subsurface molecules in a disordered state. In this state, structural defects become mobile and reactions of trapped gases and small molecules can occur. The large surface area of nanocluster deposits relative to their bulk allows for routine observation of such surface-mediated processes. Furthermore, the disordered surface and subsurface layers in nanocluster deposits mimic the structure of amorphous ice rinds found on interstellar dust grains. Transmission Electron Microscopy (TEM has been used tn characterize the crystallinity, growth mechanism, and size distribution of nanoclusters formed from a mixture of water vapor with an inert carrier gas that has been rapidly cooled to 77K. E M imaging reveals a Gaussian size distribution around a modal diameter that increases from approx. 15 to 30 nm as the percentage of water vapor within the mixture increases from 0.5 to 2.007, respectively . TEM bright and dark field imaging also reveals the crystalline nature of the clusters. h4any of the clusters show a mosaic structure in which crystalline domains originate at the center Other images show mirror planes that are separated by approx. 10 nm. Electron diffraction patterns of these clusters show that the clusters are composed of cubic ice with only a small hexagonal component. Further, the crystalline domain size is approximately the same as the modal diameter suggesting that the clusters are single crystals.

Blake, David↗