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At least 577 records · Page 32

Development of a bench-scale dissolution concept for the direct extraction of nuclear fuel

Current used nuclear fuel reprocessing efforts utilize a hydrometallurgical approach in which the UNF is dissolved in hot nitric acid followed by solvent extraction into an organic solvent to harvest target nuclides. Previous studies have shown that the dissolution and loading process could be combined into a single organic dissolution/extraction step, producing loaded organic in a single step process. This single step process also includes the advantage of selectively targeting key nuclides in the dissolution while leaving undesirable constituents as part of the undissolved solids. This process is referred to hereafter as direct extraction. Ongoing research from multiple national labs has proven the effectiveness of this technique at research scale. Therefore, potential methods to implement direct extraction at both bench and industrial scale have been developed. The key features of potential dissolver system designs were identified via the team at Pacific Northwest National Laboratory and several designs based on industrial counterparts were assessed for feasibility. This report summarizes the advantages and disadvantages of multiple methods, concluding with a path forward to create multiple unique dissolver designs. The first design will be a single stage recirculating eductor mixer. The second design recommendation is a stator rotor static mixing flow loop design. Each dissolver could be utilized separately, simultaneously, or in series to answer questions surrounding reaction kinetics including residence time, provide a proof of concept for targeted extractions of specific nuclides, and inform needs for industrial scale implementation

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Harvesting Isotopically Pure Ac-225 from Ra-225 Produced in Thorium Target Spallation Reaction

A method for isolating Ra-225 from linear accelerator irradiated Th metal chemical processing waste streams has been established. Separating Ra-225 from the complex matrix following proton irradiation of Th metal provides a source of isotopically pure Ac-225 free of the Ac-227 impurity that is present in accelerator-produced Ac-225. Ra isotopes are first separated from the irradiated Th target via cation exchange methods. Importantly, the Ra-containing fraction is cleaned from residual citrate via dilute nitric acid washes (0.5 M) on AG50W-X8 resin. The mixed Ra isotopes are then further purified from Ba-140 impurity using a Sr resin column. Ra elutes through the resin with successive washes of 2.5 M HNO 3 while Ba-140 is retained. Ac-225 is then harvested by loading the Ra content onto an AG50W-X8 cation exchange column where the Ra-225 parent is eluted with 2.5 M HNO 3 before the Ac-225 daughter is eluted with 8 M HNO 3 .

07 ISOTOPE AND RADIATION SOURCES↗

Inverse prediction of PuO2 processing conditions using Bayesian seemingly unrelated regression with functional data

Over the past decade, a variety of innovative methodologies have been developed to better characterize the relationships between processing conditions and the physical, morphological, and chemical features of special nuclear material (SNM). Different processing conditions generate SNM products with different features, which are known as “signatures” because they are indicative of the processing conditions used to produce the material. These signatures can potentially allow a forensic analyst to determine which processes were used to produce the SNM and make inferences about where the material originated. This article investigates a statistical technique for relating processing conditions to the morphological features of PuO 2 particles. We develop a Bayesian implementation of seemingly unrelated regression (SUR) to inverse-predict unknown PuO 2 processing conditions from known PuO 2 features. Model results from simulated data demonstrate the usefulness of the technique. Applied to empirical data from a bench-scale experiment specifically designed with inverse prediction in mind, our model successfully predicts nitric acid concentration, while results for Pu concentration and precipitation temperature were equivalent to a simple mean model. Our technique compliments other recent methodologies developed for forensic analysis of nuclear material and can be generalized across the field of chemometrics for application to other materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Chemically Stable Styrenic Electrospun Membranes with Tailorable Surface Chemistry

Membranes with tailorable surface chemistry have applications in a wide range of industries. Synthesizing membranes from poly(chloromethyl styrene) directly incorporates an alkyl halide surface-bound initiator which can be used to install functional groups via SN2 chemistry or graft polymerization techniques. In this work, poly(chloromethyl styrene) membranes were synthesized through electrospinning. After fabrication, membranes were crosslinked with a diamine, and the chemical resistance of the membranes was evaluated by exposure to 10 M nitric acid, ethanol, or tetrahydrofuran for 24 h. The resulting membranes had diameters on the order of 2–5 microns, porosities of >80%, and permeance on the order of 10,000 L/m2/h/bar. Crosslinking the membranes generally increased the chemical stability. The degree of crosslinking was approximated using elemental analysis for nitrogen and ranged from 0.5 to 0.9 N%. The poly(chloromethyl styrene) membrane with the highest degree of crosslinking did not dissolve in THF after 24 h and retained its high permeance after solvent exposure. The presented chemically resistant membranes can serve as a platform technology due to their versatile surface chemistry and can be used in membrane manufacturing techniques that require the membrane to be contacted with organic solvents or monomers. They can also serve as a platform for separations that are performed in strong acids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Separation of Lanthanide Isotopes from Mixed Fission Product Samples

The measurement of radioactive fission products from nuclear events has important implications for nuclear data production, environmental monitoring, and nuclear forensics. In a previous paper, the authors reported the optimization of an intra-group lanthanide separation using LN extraction resin from Eichrom Technologies®, Inc. and a nitric acid gradient. In this work, the method was demonstrated for the separation and quantification of multiple short-lived fission product lanthanide isotopes from a fission product sample produced from the thermal irradiation of highly enriched uranium. The separations were performed in parallel in quadruplicate with reproducible results and high decontamination factors for 153 Sm, 156 Eu, and 161 Tb. Based on the results obtained here, the fission yields for 144 Ce, 153 Sm, 156 Eu, and 161 Tb are consistent with published fission yields. This work demonstrates the effectiveness of the separations for the intended application of short-lived lanthanide fission product analysis requiring high decontamination factors.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Observationally constrained analysis on the distribution of fine- and coarse-mode nitrate in global models

Nitrate plays an important role in the Earth system and air quality. A key challenge in simulating the life cycle of nitrate aerosol in global models is to accurately represent mass size distribution of nitrate aerosol. In this study, we evaluate the performance of the Energy Exascale Earth System Model version 2 (E3SMv2) and the Community Earth System Model version 2 (CESM2), along with Aerosol Comparisons between Observations and Models (AeroCom) phase III models, in simulating spatial distribution of fine-mode nitrate, the mass size distribution of fine- and coarse-mode nitrate, and the gas–aerosol partitioning between nitric acid gas and nitrate, using long-term ground-based observations and measurements from multiple aircraft campaigns. We find that most models underestimate the annual mean PM 2.5 (particulate matter with diameter less than 2.5 µm) nitrate surface concentration averaged over all sites. The observed nitrate PM 2.5 / PM 10 and PM 1 / PM 4 ratios are influenced by the relative contribution of fine sulfate or organic particles and coarse dust or sea salt particles. Overall, the ground-based observations give an annual mean surface nitrate PM 2.5 / PM 10 ratio of 0.7. Most models underestimate the annual mean PM 2.5 / PM 10 ratio in all regions. There are large spreads in the modeled nitrate PM 1 / PM 4 ratios, which span the full range from 0 to 1. Most models underestimate the surface molar ratio of nitrate to total inorganic nitrate averaged across all sites. Our study indicates the importance of gas–aerosol partition parameterization and the simulation of dust and sea salt in correctly simulating the mass size distribution of nitrate.

Nitrate↗

Comparison of ozone formation attribution techniques in the northeastern United States

The Integrated Source Apportionment Method (ISAM) has been revised in the Community Multiscale Air Quality (CMAQ) model. This work updates ISAM to maximize its flexibility, particularly for ozone (O 3 ) modeling, by providing multiple attribution options, including products inheriting attribution fully from nitrogen oxide reactants, fully from volatile organic compound (VOC) reactants, equally from all reactants, or dynamically from NO x or VOC reactants based on the indicator gross production ratio of hydrogen peroxide (H 2 O 2 ) to nitric acid (HNO 3 ). The updated ISAM has been incorporated into the most recent publicly accessible versions of CMAQ (v5.3.2 and beyond). This study's primary objective is to document these ISAM updates and demonstrate their impacts on source apportionment results for O 3 and its precursors. Additionally, the ISAM results are compared with the Ozone Source Apportionment Technology (OSAT) in the Comprehensive Air-quality Model with Extensions (CAMx) and the brute-force method (BF). All comparisons are performed for a 4 km horizontal grid resolution application over the northeastern US for a selected 2 d summer case study (9 and 10 August 2018). General similarities among ISAM, OSAT, and BF results add credibility to the new ISAM algorithms. However, some discrepancies in magnitude or relative proportions among tracked sources illustrate the distinct features of each approach, while others may be related to differences in model formulation of chemical and physical processes. Despite these differences, OSAT and ISAM still provide useful apportionment data by identifying the geographical and temporal contributions of O 3 and its precursors. Both OSAT and ISAM attribute the majority of O 3 and NO x contributions to boundary, mobile, and biogenic sources, whereas the top three contributors to VOCs are found to be biogenic, boundary, and area sources.

54 ENVIRONMENTAL SCIENCES↗

Didymium compound improves nickel-cadmium cell

Nickel electrodes impregnated with an additive solution of didymium hydrate and nitric acid mixed with nickel nitrate increases ampere-hour capacity of cells and does not affect the voltage characteristics.

Source record↗

A Method for Prevention of Screaming in Rocket Engines

Lateral and longitudinal combustion-pressure oscillations that occurred in screaming combustion of a 1000-pound-thrust rocket engine using white fuming nitric acid and JP-4 fuel as propellants were successfully prevented by means of longitudinal fins in the combustion chamber. Fin position was critical, and complete attenuation was achieved only when the fins were located in a zone approximately 8 to 16 inches from the injector. Fins located in other zones, that is, near the injector or far downstream from the injector, did not stop the oscillations. When oscillations occurred in finned chambers, the longitudinal mode seemed more dominant than the lateral mode; in chambers without fins, the lateral mode tended to be dominant. The lateral oscillation was distorted and its intensity diminished by the fins. Fins, however, did not affect the frequencies; the longitudinal frequency varied inversely with chamber length, and lateral frequencies varied only slightly from an average of 6000 cycles per second.

ROCKET ENGINE NOISE↗

Continuous analysis of nitrogen dioxide in gas streams of plants

Analyzer and sampling system continuously monitors nitrogen dioxide concentrations in the feed and tail gas streams of a facility recovering nitric acid. The system, using a direct calorimetric approach, makes use of readily available equipment and is flexible and reliable in operation.

Durkin, W. T.↗

A method for precision anodize stripping

Felt templates saturated with etch solution remove anodized finish from aluminum without damage to the surface. The solution is a combination of nitric acid, chromic acid, and hydrofluoric acid.

Peters, R. L.↗

H2SO4-HNO3-H2O ternary system in the stratosphere

Estimation of the equilibrium vapor pressure over the ternary system H2SO4-HNO3-H2O to study the possibility of stratospheric aerosol formation involving HNO3. It is shown that the vapor pressures for the ternary system H2SO4-HNO3-H2O with weight composition around 70-80% H2SO4, 10-20% HNO3, 10-20% H2O at -50 C are below the order of 10 to the minus 8th mm Hg. It is concluded that there exists more than sufficient nitric acid and water vapor in the stratosphere to participate in ternary system aerosol formation at -50 C. Therefore, HNO3 should be present in stratospheric aerosols, provided that H2SO4 is also present.

Kiang, C. S.↗

Absorption cross sections of stratospheric molecules

Two classes of molecular species must be considered in a calculation of photochemical rates in the stratosphere. The first class consists of molecular oxygen and ozone, while the second class contains the remainder of the minor constituents. If accurate values of the transmitted fluxes are required at large optical depths, the cross sections for molecular oxygen and ozone must be known to within a few per cent at least. On the other hand, the photochemical rates for the minor species are given simply by the relevant cross sections. A review of published cross sections is presented, giving attention to molecular oxygen, ozone, nitric oxide, nitrogen dioxide, nitrous oxide, nitric acid, ammonia, water vapor, hydrogen peroxide, carbon monoxide, carbon dioxide, and sulfur dioxide.

Hudson, R. D.↗

Lead isotope systematics of some Apollo 17 soils and some separated components from 76501

Isotopic lead data from bulk samples of Apollo 17 soils were analyzed, and they define a chord in a concordia diagram, showing the presence of a component or components containing excess radiogenic lead with Pb-207/Pb-206 equal to about 1.32. The chord is distinctly different from the cataclysm chord, for which Pb-207/Pb-206 is approximately 1.45. Nitric acid analysis of plagioclase indicates lead ages of around 4.35 AE, in agreement with previous findings. Agglutinates from soil 76501,34 show loss of approximately 15% of lead.

Church, S. E.↗

Two techniques for eliminating luminol interference material and flow system configurations for luminol and firefly luciferase systems

Two methods for eliminating luminol interference materials are described. One method eliminates interference from organic material by pre-reacting a sample with dilute hydrogen peroxide. The reaction rate resolution method for eliminating inorganic forms of interference is also described. The combination of the two methods makes the luminol system more specific for bacteria. Flow system designs for both the firefly luciferase and luminol bacteria detection systems are described. The firefly luciferase flow system incorporating nitric acid extraction and optimal dilutions has a functional sensitivity of 3 x 100,000 E. coli/ml. The luminol flow system incorporates the hydrogen peroxide pretreatment and the reaction rate resolution techniques for eliminating interference. The functional sensitivity of the luminol flow system is 1 x 10,000 E. coli/ml.

Thomas, R. R.↗

Gold recovery process from polyimide film

Process economically separates gold from goldized polyimide film and other nonmetallic scrap without hazards of conventional processes. Technique uses nitric acid to destroy nonmetallic material, leaving gold intact.

Houston, D. W.↗

Interhemispheric survey of minor upper atmospheric constituents during October - November 1976

The CV-990 aircraft coordinated several flights with a NASA U-2 aircraft, NOAA ground station measurements in Alaska, Hawaii, and American Samoa, and with Australian and New Zealand ground stations, aircraft, and a balloon experiment in the Southern hemisphere. Data were obtained for species including ozone, total ozone, the oxides of nitrogen, the chlorofluoromethanes, water vapor, nitric acid, carbon monoxide, carbon dioxide, hydrogen chloride, Aitken nuclei, ammonia, aerosols, temperatures, and winds. Individual experiment results and selected analyses are presented. The experimental data include total column densities, latitude variations, interhemisphere differences, and vertical profiles.

Gauntner, D. J.↗

The NASA Ames Research Center one- and two-dimensional stratospheric models. Part 2: The two-dimensional model

The two-dimensional model of stratospheric constituents is presented in detail. The derivation of pertinent transport parameters and the numerical solution of the species continuity equations, including a technique for treating the stiff differential equations that represent the chemical kinetic terms, and appropriate methods for simulating the diurnal variations of the solar zenith angle and species concentrations are discussed. Predicted distributions of tracer constituents (ozone, carbon 14, nitric acid) are compared with observed distributions.

Whitten, R. C.↗