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At least 91 records · Page 5

Simultaneous Isotopic Analysis of U, Pu, and Am in Spent Nuclear Fuel by Resonance Ionization Mass Spectrometry

Solid samples of spent nuclear fuel were analyzed for actinide isotopic composition by resonance ionization mass spectrometry. Isotopes of U, Pu, and Am were simultaneously quantified using a new method that removes and/or resolves the isobaric interferences at 238 U/ 238 Pu and 241 Pu/ 241 Am without sample preparation other than cutting and mounting small (~10 μm) samples. Trends in burnup and neutron capture product distributions were correlated with the sampling positions inside the reactor. Overall, the results show the skin effect, in which the core and near-edge regions of a fuel pellet exhibit strong differences in actinide concentrations and isotope distributions due to differences in the neutron energy spectra between the pellet rim and the core. While no elemental concentration measurements were made, the ability to measure the 238 Pu/ 239 Pu ratio in the presence of a 7400× excess of 238 U enabled an estimate of the enhancement in Pu concentration due to the skin effect at the rim of the pellet.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Product Consistency Test Results for the LAW Phase 5 Glasses

This report provides the results of the Vapor Hydration Test solutions and the Product Consistency Test leachates from the Low-Activity Waste Phase 5 glasses, a series of simulated nuclear waste glasses fabricated at the Pacific Northwest National Laboratory. The series included quenched and canister-centerline cooled versions of the glasses. These data will be used in the development of enhanced property/composition models for waste glass vitrification at Hanford. Several of the blanks had detectable amounts of sodium and/or silicon. The measured concentrations (mg/L) of boron, sodium, and silicon for the low-activity test reference material glass included with the Product Consistency Tests were much lower than the expected low-activity test reference material test results. A review of the Product Consistency Test data indicated that there was generally little difference between the normalized values based on targeted or measured glass composition. Heat treatment had various impacts on the normalized concentration values. Most of the glasses had NC B , NC Na , and NC Si values that were greater than the Hanford Tank Waste Treatment and Immobilization Plant low-activity waste constraint of 4 g/L. The release rates for boron, sodium, and silicon were highly correlated for the study glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Comprehensive Baseline Environmental Monitoring of an Interim Legacy Waste Store in Arid Zone Australia - 20062

Radionuclide containing soil and rubble from the clean-up of a former uranium, thorium and rare earth minerals processing research facility carried out in the early 50's and 60's is currently stored at the Woomera Test Range in South Australia awaiting final disposal. Prior to developing a final disposal pathway commensurate with waste acceptance criteria, a comprehensive baseline environmental monitoring has been carried out to establish the background radiation levels. The survey included in situ gamma scanning of the surface soil ({sup 238}U, {sup 232}Th, {sup 40}K), a laboratory analysis of 86 soil samples (from 0-20 cm depth), which involved XRF measurements (U, Th, and rare earth metals) and spectroscopic analysis ({sup 238}U, {sup 232}Th, {sup 226}Ra and daughter nuclides). A time series of radon concentration measurements in air was established, while soil radon ({sup 222}Rn) and thoron ({sup 220}Rn) flux measurements were undertaken at 18 different locations. The 2018 comprehensive baseline survey demonstrated radiation levels in the immediate vicinity of the Woomera interim waste store are typical background values of soil and rock. No contamination was detected. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Enabling Microscale Processing: Combined Raman and Absorbance Spectroscopy for Microfluidic On-Line Monitoring

Microfluidics have many potential applications including characterization of chemical processes on a reduced scale, spanning the study of reaction kinetics using on-chip liquid–liquid extractions, sample pretreatment to simplify off-chip analysis, and for portable spectroscopic analyses. The use of in situ characterization of process streams from laboratory-scale and microscale experiments on the same chemical system can provide comprehensive understanding and in-depth analysis of any similarities or differences between process conditions at different scales. A well-characterized extraction of Nd(NO 3 ) 3 from an aqueous phase of varying NO 3– (aq) concentration with tributyl phosphate (TBP) in dodecane was the focus of this microscale study and was compared to an earlier laboratory-scale study utilizing counter current extraction equipment. Here, we verify that this same extraction process can be followed on the microscale using spectroscopic methods adapted for microfluidic measurement. Concentration of Nd (based on UV–vis) and nitrate (based on Raman) was chemometrically measured during the flow experiment, and resulting data were used to determine the distribution ratio for Nd. Extraction distributions measured on the microscale were compared favorably with those determined on the laboratory scale in the earlier study. Both micro-Raman and micro-UV–vis spectroscopy can be used to determine fundamental parameters with significantly reduced sample size as compared to traditional laboratory-scale approaches. This leads naturally to time, cost, and waste reductions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Method for calculating radon activity and radon rejection using a beta-gamma detector

Radon interferes with concentration measurements used by atmospheric radioxenon systems. We demonstrate a method to quantify the amount of radon that is present in the detectors, the impact of radon activity on the minimum-detectable-concentrations, and how to determine the needed radon rejection levels. An example calculation shows a radon rejection level of 10 5 is sufficient to limit impact on the detector sensitivity. We anticipate this method will give analysist a better understanding of radon present in their measurements and allow system designers to tailor their systems’ radon rejection better for its location.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

In situ aerobic methane oxidation rates in a stratified lake

Abstract Microbial aerobic methane oxidation is an important sink for aquatic methane worldwide. Despite its importance to global methane fluxes, few aerobic methane oxidation rates have been obtained in freshwater or marine environments without imposing changes to the microbial community through use of ex situ methods. A novel in situ incubation method for continuous time‐series measurements was used in Jordan Lake, North Carolina, during 2020–2021, to determine reaction kinetics for aerobic methane oxidation rates across a wide range of naturally varying methane (55–1833 nM) and dissolved oxygen (DO; 28–366 μM) concentrations and temperatures (17–30°C). Methane oxidation began immediately at the start of each of 21 incubations and methane oxidation rates were 1 st order with respect to methane. The data density allowed for accurate calculation of 1 st ‐order rate constants,k, that ranged from 0.018 to 0.462 h −1 (R 2 > 0.967). Addition of ammonium (20–45 μM) to natural concentrations ranging from 0.057 to 2.4 μM did not change aerobic methane oxidation rate kinetics, suggesting that the natural population of aerobic methane oxidizers in this eutrophic lake was not nitrogen limited. Values ofkinversely correlated most strongly with initial DO concentrations (R 2 = 0.82) rather than temperature. Values forkincreased with Julian day throughout our sampling period, suggesting seasonal influences on methane oxidation via responses to geochemical changes or shifts in microbial community abundance and composition. These experiments demonstrate a high variability in the enzymatic capacity for 1 st ‐order methane oxidation rates in this eutrophic lake that is tightly and inversely coupled to oxygen concentrations. Measurements of in situ aerobic methane oxidation rate constants allow for the direct quantification and modeling of the microbial community's capacity for methane oxidation over a wide range of natural methane concentrations.

Marine & Freshwater Biology↗

Void formation during cyclic oxidation of oxide dispersion strengthened FeCrAl alloys

Here, oxide dispersion strengthened FeCrAl alloys are considered for various high-temperature applications due to their excellent mechanical properties and oxidation resistance, but void formation is a concern for component durability. Cyclic oxidation testing was conducted on alloy MA956 and PM2000 at 1100–1200ºC for durations of up to 10,000 h and the void content was determined from optical cross-sections by image analysis. At 1100ºC, 100 h cycle, the low void concentrations measured were consistent with two competing mechanisms proposed in the literature: coalescence of process-induced nano-voids and alloy sintering. At 1200ºC using 1 h cycles, the void concentration was much higher, reaching ~3% to 6% for specimens tested to breakaway oxidation. The void growth was attributed to the high oxidation rates and the annihilation of oxidation-induced vacancies at the surface of the process-induced voids.

36 MATERIALS SCIENCE↗

Influence of background sources and topographic resolution in the Weather Research and Forecasting Model on xenon plume characteristics at monitoring stations

For many atmospheric monitoring applications, networks of measurement sites—such as the radionuclide stations of the International Monitoring System—can be sparse. With measurement locations potentially hundreds to thousands of kilometers from a release it is important to quantify the effects of physical processes on transport and dispersion of plumes between source and measurement locations. This study addresses the effects of background sources and topography resolution near the release location of radionuclides. We use the Weather Research and Forecasting (WRF) model with inline chemistry to investigate (1) how an additional, time-varying source of 133 Xe, such as an operational medical isotope production facility, contributes to activity concentration measurements at monitoring sites, and (2) how complex topography influences on atmospheric conditions near emission sources impact plume concentrations at varying distances from the source. Two 133 Xe emission sources, including (1) a high flux rate of short duration representing an explosive event, and (2) a variable and continuous background source, are simulated. The continuous background source contributes significantly to total 133 Xe concentrations at several monitoring stations. Further, a WRF simulation at 9 km horizontal resolution is compared with a nested grid simulation, where the innermost domain has a resolution of 1 km. Increased topographic resolution leads to an improved representation of plume responses to local winds, with topographic influences greatest at locations closest to the sources. Differences between the two domain resolutions decrease at greater distances from the sources, as plumes have time to spread and mix and are influenced by synoptic scale circulation patterns that are represented similarly in both simulations.

54 ENVIRONMENTAL SCIENCES↗

Composition Measurements of the LAW Phase 5 Glasses

This report provides the results from the chemical analyses of glass compositions for the Low-Activity Waste Phase 5 study glasses, a series of simulated nuclear waste glasses fabricated at Pacific Northwest National Laboratory. These data will be used in the development of enhanced property/composition models for waste glass vitrification at Hanford. Chemical analyses were performed on a representative sample of each of the quenched glasses to allow for comparisons with targeted compositions. The relative differences between the targeted and measured concentrations of CaO, Cl - , K 2 O, Li 2 O, and SO 3 for some of the glasses were greater than 10%. Several of these glass samples were rerun to verify original measurements; however, there were no significant changes in the measurements to indicate errors in preparation or analysis of the samples. These results can be used in further characterization of this series of glasses, including the normalization of Product Consistency Test results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Chemical clocks: using otolith geochemistry to enhance estimation of age and growth of white hake (Urophycis tenuis)

The white hake (Urophycis tenuis) is a groundfish distributed throughout the Gulf of Maine. Catch advice is based on stock assessments done with age-based population dynamics models; however, otolith aging is challenging because of unclear growth increments. To address this concern, we compared the consistency of aging with counts of visual annuli to that of aging with cycles of elemental concentrations measured by using laser ablation inductively coupled plasma mass spectrometry. We tested the hypothesis that oscillations in both environmental conditions and internal physiology through time influence uptake of elements during otolith mineralization. Concentrations of manganese, in comparison with those of the other investigated trace elements (magnesium, strontium, and barium), had the most promising correlation with visual growth increments (~100% age agreement, ±1 year), offering an additional tool to enhance increment identification. In our examination of 550 otoliths collected during 2007–2021, we found that white hake lived a maximum of 10.3 years and exhibited sexual dimorphism in maximum length and age. By using generated von Bertalanffy growth functions, L(t)=110(1–e–0.113(t+0.45)) for males and L(t)=140(1–e–0.113(t–0.30)) for females (where L(t) is length at time t), size and age at maturity were calculated for males (37.4 cm in total length (TL), 3.3 years) and females (47.4 cm TL, 4.2 years). These results demonstrate that otolith geochemistry can be used to improve the accuracy and precision of the estimation of fish age and maturity, even for challenging species.

59 BASIC BIOLOGICAL SCIENCES↗

BTRIC Technical Support for Appalachia: FY 2024 Summary Report on Net Negative Carbon Building Demonstration with AgPod

This report investigates the effects of various concentrations of CO 2 on the photosynthesis and biomass accumulation of crops growing in an AgPod, using kale as the test crop. In the first year of the study, increasing the CO 2 concentration in the AgPod was found to promote higher photosynthetic rates in kale plants up to 1,300 ppm (the highest CO 2 concentration measured). An interesting finding was that net photosynthetic rates of kale leaves remain unsaturated until reaching unusually high levels of photosynthetically active radiation (PAR, > 1,200 µmol m -1 s -1 ) and CO 2 concentration (> 1,100 ppm). Such high levels of saturating PAR and CO 2 concentration values rarely occur under natural conditions, suggesting a promising potential for carbon capture via enriched controlled environment agriculture (ECEA). During the second year of the study, a second crop was planted to confirm the actual effects on growth with increased CO 2 concentrations. Our results suggest that growing kale plants in the AgPod system at higher CO 2 levels resulted in a successful and highly productive crop, up to three times the amount grown at 415 CO 2 . Further, the kale plants grown under higher CO 2 conditions (1000 ppm) are not CO 2 saturated and can potentially further improve yield at even higher CO 2 environments.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Spatiotemporal Changes in Trace Metal Bioavailability in the Sediment Pore water of a Constructed Wetland Using Passive Pore water Samplers

Sediments in aquatic systems often act as a major sink for contaminants. Diffusive gradient in thin films (DGTs) and in situ equilibrium dialysis samplers (peepers) are two major in situ pore water sampling devices that overcome the problems associated with conventional pore water sampling methods. In the present study, DGTs and peepers were used to study the spatial and seasonal effects (cool months, October–February; warm months, May–September) on metal bioavailability in the H‐02 constructed wetland and the sink versus source role of the sediments by calculating the metal resupply capacity. Data showed similar seasonal trends in metal concentrations using passive samplers, peepers, and DGTs. Pooled Cu and Zn concentrations measured using DGTs were lower in warm months (1.67 ± 1.50 and 2.62 ± 0.68 μg L –1 , respectively, p < 0.001) versus in cool months (2.12 ± 0.65 and 5.58 ± 1.33 μg L –1 , respectively, p < 0.001; mean ± 95% confidence interval). Sulfate (SO 4 2− ) concentrations were significantly (p = 0.0139) lower in warm months (averaged at 0.22 ± 0.05 mg L –1 ) compared to in cool months (0.16 ± 0.05 mg L –1 ). The increase in SO 4 2− concentration is an indicator of the lower activity of sulfate‐reducing bacteria, which need SO 4 2− during anaerobic respiration, in which SO 4 2− is reduced to sulfide (S 2– ) that forms insoluble salts with Cu and Zn, which could partially explain the higher bioavailability of these metals in the cool season. Metal resupply capacity of the sediments was mostly <0.2 for Cu and Zn. Taken together, the H0‐2 wetland sediments mostly acted as a sink to both Cu and Zn over the course of the present study. Environ Toxicol Chem 2023;42:2726–2736. © 2023 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.

54 ENVIRONMENTAL SCIENCES↗

Classroom aerosol dispersion modeling: experimental assessment of a low-cost flow simulation tool

The purpose of this study was to assess the utility of a low-cost flow simulation tool for an indoor air modeling application by comparing its outputs with the results of a physical experiment, as well as those from a more advanced computational fluid dynamics (CFD) software package. In this study, five aerosol dispersion tests were performed in two different classrooms by releasing a CO 2 tracer gas from six student locations. Resultant steady-state concentrations were monitored at 13 locations around the periphery of the room. Subsequently, the experiments were modeled using both a low-cost tool (SolidWorks Flow Simulation) and a more sophisticated tool (STAR-CCM+). Models were evaluated based on their ability to predict the experimentally measured concentrations at the 13 monitoring locations by calculating four performance parameters commonly used in the evaluation of dispersion models: fractional mean bias (FB), normalized mean-square error (NMSE), fraction of predicted value within a factor of two (FAC2), and normalized absolute difference (NAD). The more sophisticated model performed better in 15 of the 20 possible cases (five tests at four parameters each), with parameters meeting acceptance criteria in 19 of 20 cases. However, the lower-cost tool was only slightly worse, with parameters meeting acceptance criteria in 18 of 20 cases, and it performed better than the other tool in 3 of 20 cases. Because it provides useful results at a fraction of the monetary and training cost and is already widely accessible to many institutions, such a tool may be worthwhile for many indoor aerosol dispersion applications, especially for students or researchers just beginning CFD modeling.

54 ENVIRONMENTAL SCIENCES↗

Effective Mass from Seebeck Coefficient

Abstract Engineering semiconductor devices requires an understanding of the effective mass of electrons and holes. Effective masses have historically been determined in metals at cryogenic temperatures estimated using measurements of the electronic specific heat. Instead, by combining measurements of the Seebeck and Hall effects, a density of states effective mass can be determined in doped semiconductors at room temperature and above. Here, a simple method to calculate the electron effective mass using the Seebeck coefficient and an estimate of the free electron or hole concentration, such as that determined from the Hall effect, is introduced here is the Seebeck effective mass, n H is the charge carrier concentration measured by the Hall effect ( n H = 1/ eR H , R H is Hall resistance) in 10 20 cm −3 , T is the absolute temperature in K, S is the Seebeck coefficient, and k B / e = 86.3 μV K −1 . This estimate of the effective mass can aid the understanding and engineering of the electronic structure as it is largely independent of scattering and the effects of microstructure (grain boundary resistance). It is particularly helpful in characterizing thermoelectric materials.

Snyder, Gerald Jeffrey↗

Integrating Metal-Hydride and Gas-Detector for Tritium Gas Detection

Detection of trace amounts of environmental tritium is a challenging problem, driving the need for field-deployable systems that offer high sensitivity, selectivity, and minimal false positives. We present a technique for high-sensitivity, high-selectivity tritium measurement, which integrates metal-hydride and gas-detector concepts into a compact field-deployable tritium sensor. A hydrogen-storage metal embedded in a gas proportional counter selectively absorbs protium (1H)/tritium (3H), which are subsequently released into the counter volume with a reduced radiation background. Ionizations induced by 3H beta particles are then measured in proportional counting mode, achieving high detection efficiency. Preliminary studies conducted with palladium (Pd) thin films coated on stainless-steel substrates demonstrated 3H absorption and metal-tritide formation, followed by 3H desorption upon heating the metal-tritide. These processes were confirmed using activity concentrations measured by a commercial tritium monitor and pulse height spectra acquired from a custom-built detector.

Gas-proportional counter↗

Measurements of Six-Junction Concentrator Solar Cells

Accurate measurements of six-junction inverted metamorphic concentrator solar cells under AM1.5 direct spectrum are obtained by adjusting the spectrum of a tunable high-intensity solar simulator with custom mirrors. Isotype reference cells and broadband InGaAs QE calibration cells were developed for accurate measurements. Modeling and varying the illumination show that an unavoidable 15% - 17% overillumination on the sixth junction does not result in significant error of these 6J IMM devices. Spectrally adjusted flash measurements are independently confirmed by NREL's Cell and Module Performance team. Concentration measurements of a 6J IMM solar cell resulted in 47.1 ± 3.2% (absolute) efficiency at 143 suns.

41 EE - Solar Energy Technologies Office (EE-4S)↗

Open cells exhibit weaker entrainment of free-tropospheric biomass burning aerosol into the south-east Atlantic boundary layer

This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm -3 ) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ~1000 cm -3 . Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

54 ENVIRONMENTAL SCIENCES↗