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At least 181 records · Page 10

BEYONDPLANCK XIII. Intensity foreground sampling, degeneracies, and priors

We present the intensity foreground algorithms and model employed within the BEYONDPLANCK analysis framework. The BEYONDPLANCK analysis is aimed at integrating component separation and instrumental parameter sampling within a global framework, leading to complete end-to-end error propagation in the Planck Low Frequency Instrument (LFI) data analysis. Given the scope of the BEYONDPLANCK analysis, a limited set of data is included in the component separation process, leading to foreground parameter degeneracies. In order to properly constrain the Galactic foreground parameters, we improve upon the previous Commander component separation implementation by adding a suite of algorithmic techniques. These algorithms are designed to improve the stability and computational efficiency for weakly constrained posterior distributions. These are: (1) joint foreground spectral parameter and amplitude sampling, building on ideas from MIRAMARE; (2) component-based monopole determination; (3) joint spectral parameter and monopole sampling; and (4) application of informative spatial priors for component amplitude maps. We find that the only spectral parameter with a significant signal-to-noise ratio using the current BEYONDPLANCK data set is the peak frequency of the anomalous microwave emission component, for which we find $ν$ p = 25.3 ± 0.5 GHz; all others must be constrained through external priors. Future works will be aimed at integrating many more data sets into this analysis, both map and time-ordered based, thereby gradually eliminating the currently observed degeneracies in a controlled manner with respect to both instrumental systematic effects and astrophysical degeneracies. When this happens, the simple LFI-oriented data model employed in the current work will need to be generalized to account for both a richer astrophysical model and additional instrumental effects. This work will be organized within the Open Science-based COSMOGLOBE community effort.

79 ASTRONOMY AND ASTROPHYSICS↗

Initial Assessment of TeF 6 Adsorption

Research and development that supports the management of off-gases from nuclear fuel reprocessing has historically been focused on the off-gas streams that arise from aqueous reprocessing technology. However, as Gen-IV reactor development pathways move toward deployment, alternative spent nuclear fuel (SNF) processing and disposition pathways have been considered more actively. This work is focused upon aspects of fluoride volatility (FV) processing. The versatility of this method for deployment against multiple types of spent fuel encourages the continued advancement of both the primary separations processes and the secondary processes, including waste treatment, material control and accountability, and engineering designs. Recent work noted that TeF 6 , the most highly volatile fluorinated compound produced during FV processing, did not have a clear abatement technology recommended in the literature. Thus, this work performed scoping tests on activated alumina and copper shot to assess whether they could be used to remove TeF 6 from gas streams that bear F 2 . Previous work on this topic was not well described in the literature and was not performed with excess F 2 in the stream as would be typical of spent fuel processing via FV. To support an understanding of the concentration of TeF 6 contacting the adsorbent beds, a series of preliminary testing identified the TeF 6 production rate and the equilibrium concentration of TeF 6 in the gas stream contacting the adsorbent. Excess F 2 was determined to not affect the ability of activated alumina to remove TeF 6 from the gas stream quickly and completely. A determination of whether excess F 2 affected the distribution depth of Te in the sorbent bed is still pending analysis of the used sorbent. Literature suggests that when activated alumina is near saturation, TeF 6 could migrate from the sorbent bed. Future testing should investigate this possibility. Copper metal did not adsorb TeF 6 in the presence of F 2 across the sorbent temperature range of 50 to 335°C. F 2 was fully removed by the copper bed. Although preliminary thermodynamics would indicate adsorption to be energetically favorable, other factors that impact adsorption (e.g., slow kinetics, excess fluorine on the copper surface, an unfavorable transition state) are likely preventing the adsorption of TeF 6 at an easily measurable rate. The work also investigated TeF 6 production from multiple forms of Te in the temperature range of 100 to 250°C. No previous study had assessed the initial reaction rates for this process. A carefully designed study allowed determination of the activation energy for the production of TeF 6 from Te metal. The substantial amount of data collected during this study merits analysis beyond what is described here. A more in-depth kinetic analysis will be pursued. Additional analytical results will provide the ability to benchmark adsorption coefficients for TeF 6 , understand the distribution of TeF 6 within the alumina bed, and better understand the effect of F 2 partial pressure on Te fluorination. The data from this report, as supplemented by these additional analyses, will be submitted to a peer-reviewed journal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High Yield, Economical and Environmentally Benign Production of Rare Earth Elements from Coal Ash [Abstract]

Fly ash stored in landfills and ponds across the United States is an attractive, abundant domestic resource for the cost-effective recovery of rare earth elements (REE) and other critical minerals (CM). Physical Sciences Inc. (PSI) and its team members, Winner Water Services (WWS) and University of Kentucky/Center for Applied Energy Research (UK/CAER) successfully executed a multiphase program that developed and demonstrated pilot plant operations for cost-effective and environmentally-friendly production of rare earth element oxide (REO) concentrates, and the critical minerals scandium and aluminum (in the forms of salts or oxide products). We constructed and operated a sub-scale (0.5 kg/day) micropilot facility to demonstrate the key physical and chemical processing operations, predict yields, and troubleshoot process bottlenecks. The project team then designed, constructed and operated two decoupled pilot plant operations: (1) an operational pilot plant for physical separation processes with a capacity of 0.4 metric tons per day (tpd) where we optimized processes to produce selected ash fractions as the feedstock for chemical processing as well as valuable byproducts such as cement substitute, cenospheres, magnetic ash and secondary fuel carbon, and (2) an operational pilot plant for chemical processing with a capacity of 0.5 tpd that developed optimized processes for the production of: (a) REO concentrates, (b) critical minerals recovery (Sc, Al), and (c) beneficiated ash as valuable byproduct suitable for cement applications.

01 COAL, LIGNITE, AND PEAT↗

On the Onset Delays of Solar Energetic Electrons and Protons: Evidence for a Common Accelerator

The processes responsible for the acceleration of solar energetic particles (SEPs) are still not well understood, including whether SEP electrons and protons are accelerated by common or separate processes. Using a numerical particle transport model that includes both pitch-angle and perpendicular spatial diffusion, we simulate, among other quantities, the onset delay for MeV electrons and protons and compare the results to observations of SEPs from widely separated spacecraft. Such observations have previously been interpreted, in a simple scenario assuming no perpendicular diffusion, as evidence for different electron and proton sources. We show that, by assuming a common particle source together with perpendicular diffusion, we are able to simultaneously reproduce the onset delays for both electrons and protons. We argue that this points toward a common accelerator for these particles. Moreover, a relatively broad particle source is required in the model to correctly describe the observations. This is suggestive of diffusive shock acceleration occurring at large shock structures playing a significant role in the acceleration of these SEPs.

R D Strauss↗

Modeling and simulation of gas separations with spiral–wound membranes

Models for gas separations with spiral–wound membranes are developed and found to exhibit good agreement with experiments performed on N 2 /O 2 mixtures. The two–dimensional (2D) model can be accurately approximated by a one–dimensional (1D) surrogate model when the spacer widths are chosen to make the channel pressure drops small. Subsequently, the separation of propane/propylene mixtures from the recycle purge stream of a polypropylene reactor is investigated. Assuming ideal gas is found to lead to significant overestimations in membrane stage cuts (sometimes more than 10%), an extent comparable to that associated with extrapolating constant olefin permeance from a low–pressure condition. While olefin permeance can change significantly with pressure, using a constant–permeance formulation can result in a small (< 2.5%) underprediction in stage cut if the value for the permeance is taken from the feed condition. Finally, membrane properties and costs necessary for a viable separation process are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomistic origins of biomass recalcitrance in organosolv pretreatment

Separation of lignocellulosic biomass components for use in sustainable energy and biomaterials applications remains challenging, since biopolymers such as cellulose and hemicellulose carbohydrates and polyaromatic lignin are found in close proximity within the plant secondary cell wall. Organic solvents have been used to pretreat recalcitrant biomass and separate the interacting polymers, solubilizing the lignin fraction for lignin-first valorization approaches. However, no single organosolv pretreatment approach has proven superior for heterogeneous biomass samples. Here we present a complementary atomic view of interactions between biomass components using molecular simulations, specific to lignin and cellulose, resolving mechanistic hypotheses for how lignin-cellulose composition influences separation processes. Further, using lignin-cellulose binding free energy calculated using molecular simulations, we find polar protic solvents such as methanol and ethanol separate lignin from cellulose, irrespective of the charge on the lignin monomer. Aprotic organic solvents (DMSO, THF, 1,4-dioxane) separate uncharged lignin (phenols and monolignols) from cellulose, while charged lignin (cinnamates) prefer binding to cellulose.

09 BIOMASS FUELS↗

FAST - A multiprocessed environment for visualization of computational fluid dynamics

The paper presents the Flow Analysis Software Toolset (FAST) to be used for fluid-mechanics analysis. The design criteria for FAST including the minimization of the data path in the computational fluid-dynamics (CFD) process, consistent user interface, extensible software architecture, modularization, and the isolation of three-dimensional tasks from the application programmer are outlined. Each separate process communicates through the FAST Hub, while other modules such as FAST Central, NAS file input, CFD calculator, surface extractor and renderer, titler, tracer, and isolev might work together to generate the scene. An interprocess communication package making it possible for FAST to operate as a modular environment where resources could be shared among different machines as well as a single host is discussed.

Bancroft, Gordon V.↗

Methane Pyrolysis and Disposing Off Resulting Carbon

Sabatier/Electrolysis (S/E) is a leading process for producing methane and oxygen for application to Mars ISPP. One significant problem with this process is that it produces an excess of methane for combustion with the amount of oxygen that is produced. Therefore, one must discard roughly half of the methane to obtain the proper stoichiometric methane/oxygen mixture for ascent from Mars. This is wasteful of hydrogen, which must be brought from Earth and is difficult to transport to Mars and store on Mars. To reduced the problem of transporting hydrogen to Mars, the S/E process can be augmented by another process which reduces overall hydrogen requirement. Three conceptual approaches for doing this are (1) recover hydrogen from the excess methane produced by the S/E process, (2) convert the methane to a higher hydrocarbon or other organic with a lower H/C ratio than methane, and (3) use a separate process (such as zirconia or reverse water gas shift reaction) to produce additional oxygen, thus utilizing all the methane produced by the Sabatier process. We report our results here on recovering hydrogen from the excess methane using pyrolysis of methane. Pyrolysis has the advantage that it produces almost pure hydrogen, and any unreacted methane can pass through the S/E process reactor. It has the disadvantage that disposing of the carbon produced by pyrolysis presents difficulties. Hydrogen may be obtained from methane by pyrolysis in the temperature range 10000-12000C. The main reaction products are hydrogen and carbon, though very small amounts of higher hydrocarbons, including aromatic hydrocarbons are formed. The conversion efficiency is about 95% at 12000C. One needs to distinguish between thermodynamic equilibrium conversion and conversion limited by kinetics in a finite reactor.

Sharma, P. K.↗

Experimental Investigation of Transition to Turbulence as Affected by Passing Wakes: Effects of High FSTI and Increased Rod Spacing

Experimental results from a study of the effects of passing wakes upon laminar-to-turbulent transition in a low-pressure turbine passage are presented. The test section geometry is designed to simulate the effects of unsteady wakes resulting from rotor-stator interaction upon laminar-to-turbulent transition in turbine blade boundary layers and separated flow regions over suction surfaces. Single-wire, thermal anemometry techniques are used to measure time-resolved and phase-averaged, wall-normal profiles of velocity, turbulence intensity and intermittency at multiple streamwise locations over the turbine airfoil suction surface. The Reynolds number based on suction surface length and stage exit velocity is 50,000. This study compares a previously documented base case flow having an approach flow turbulence intensity of 2.5 percent and a wake passing Strouhal number of 0.792 to two additional cases: one having an increased rod spacing case having a wake passing Strouhal number of 0.396, and another having an elevated approach flow turbulence intensity of 10 percent. From these data, the effects of increased rod spacing and elevated FSTI upon transition and separation processes in the near-wall flow are documented. The results show that a decreased wake passing Strouhal number results in an earlier separation with a larger separation bubble, while the elevated FSTI results in earlier separation, but with a shorter, thinner, separation bubble. The data and animations are included in an accompanying CD ROM.

Kaszeta, Richard W.↗

Establishing Pb-203 production from electrodeposited Tl targets at Brookhaven National Laboratory

Background: Promising developments in Pb-212 radiopharmaceutical therapies have increased demand for Pb-203 diagnostic agents. Building on previous work from various isotope production facilities, this study optimized Pb-203 production from electrodeposited Tl targets at Brookhaven National Laboratory (BNL). The additional supply of Pb-203 may help meet growing preclinical and clinical demands. Results: Two Tl targets were irradiated at the Brookhaven Linac Isotope Producer facility with 30 ± 1 MeV protons, measured using previously published cross section data. Distribution coefficients for Pb Resin in acetate media were investigated for both Na + and K + cations, where potassium acetate was ~ 4 times more effective at stripping Pb from the Pb Resin. The Tl electrodeposition was optimized to deposit 350 mg of Tl (~ 60 mg/cm 2 ) on Au backing in under 6 h. The proposed separation process was completed in < 1.5 h and achieved > 98% and 92 ± 3% recovery of Tl and Pb, respectively, with an overall Tl-Pb separation factor of 6 × 10 5 . The experimentally measured half-life of Pb-203 was 52.4 ± 0.7 h, agreeing with 51.93 ± 0.02 h reported by the National Nuclear Data Center. The radioisotopic purity of the Pb fraction at 24 h post end of bombardment (EOB) from a 24 h irradiation was 66% Pb-203, 28% Pb-201, and 6% Pb-200. Following chemical separation, the Pb-203 produced in this work (21 MBq Pb-203 EOB) achieved apparent molar activities of 10 ± 5 and 0.9 ± 0.5 GBq/µmol for [ 203 Pb]Pb-DOTAM and [ 203 Pb]Pb-DO3A, respectively, decay corrected to EOB. Data derived from this work suggests BNL can produce > 10’s GBq Pb-203 with > 99% radiochemical and radioisotopic purity from Tl-205 for worldwide distribution. Conclusions: The production and separation of Pb-203 from natural Tl target material was successfully demonstrated at BNL. Existing methods were adapted and optimized for the facilities at BNL. Results from this work will guide future large-scale Pb-203 production opportunities at BNL for clinical applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Energy-efficient carbon capture from industrial point sources via commercially available green solvent and hollow fiber membrane contactors

Solvent-based absorption systems have emerged in the carbon capture space due to their high absorption capacities, reusability, and favorable energy requirements. Using diethyl sebacate as a solvent for pre- and post-combustion carbon capture has advantages over other solvents, including high hydrophobicity, low viscosity, low vapor pressure, high CO 2 solubility, high CO 2 selectivity, and being commercially available in large quantities. Despite these advantageous properties, the use of diethyl sebacate as a solvent for post-combustion carbon capture has not been studied in detail. To examine the capability of diethyl sebacate, a scalable, energy-efficient, hollow fiber membrane (microporous polypropylene and polyvinylidene fluoride) contactor (HFMC)-based process with low-cost and high surface area is investigated. A purity of 95.3 % CO 2 with 46 % recovery in one absorption stage was achieved, with a permeate flux over one magnitude greater than using a deep eutectic solvent in the same system. Technoeconomic analysis determined a ∼ 0.8 GJ per ton of CO 2 at a processing cost of ∼$93 per ton of CO 2 . Results from this work underscore the potential for utilizing green solvents in HFMC-based separation processes for effective carbon capture and provide a pathway towards practical deployment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Methods of reducing energy consumption of the oxidant supply system for MHD/steam power plants

An in-depth study was conducted to identify possible improvements to the oxidant supply system for combined cycle MHD power plants which would lead to higher thermal efficiency and reduction in the cost of electricity, COE. Results showed that the oxidant system energy consumption could be minimized when the process was designed to deliver a product O2 concentration of 70 mole percent. The study also led to the development of a new air separation process, referred to as liquid pumping and internal compression. MHD system performance calculations show that the new process would permit an increase in plant thermal efficiency of 0.6 percent while allowing more favorable tradeoffs between magnetic energy and oxidant system capacity requirements.

A. J Juhasz↗

Methods of reducing energy consumption of the oxidant supply system for MHD/steam power plants

An in-depth study was conducted to identify possible improvements to the oxidant supply system for combined cycle MHD power plants which would lead to higher thermal efficiency and reduction in the cost of electricity, COE. Results showed that the oxidant system energy consumption could be minimized when the process was designed to deliver a product O2 concentration of 70 mole percent. The study also led to the development of a new air separation process, referred to as 'liquid pumping and internal compression'. MHD system performance calculations show that the new process would permit an increase in plant thermal efficiency of 0.6 percent while allowing more favorable tradeoffs between magnetic energy and oxidant system capacity requirements.

Juhasz, A. J.↗

Computation of unsteady separation using Lagrangian procedures

The interaction between increased knowledge of unsteady separation processes and computational techniques is examined, emphasizing the use of Lagrangian coordinates. Examples include boundary layer solutions of two-dimensional unsteady flows, and separation from rotating and translating spheres. Advances in Lagrangian techniques for the Navier-Stokes equations are illusrated by means of high resolution random-walk computations of the impulsively started circular cylinder.

Van Dommelen, L. L.↗

Hierarchical 3D Printed Porous Silicones with Porosity Derived from Printed Architecture and Silicone-Shell Microballoons

A method is reported to prepare siloxane microballoons that can be loaded into a direct ink write siloxane ink for 3D printing. The resulting structure is subjected to a solvent removal and supercritical drying process to provide a final printed siloxane having both macroscopic and microscopic porosity. Core-shell particles are generated by an emulsion template and phase separation process. Intra-strand closed-cell porosities can be achieved between 10 and 40 vol% thus facilitating additional compressive strain before lockup. Here short term compression set testing highlights the excellent shape retention properties of these elastomers, which have less than 8% relative compression set under load.

36 MATERIALS SCIENCE↗

Toward ultrafast soft x-ray spectroscopy of organic photovoltaic devices

Novel ultrafast x-ray sources based on high harmonic generation and at x-ray free electron lasers are opening up new opportunities to resolve complex ultrafast processes in condensed phase systems with exceptional temporal resolution and atomic site specificity. In this perspective, we present techniques for resolving charge localization, transfer, and separation processes in organic semiconductors and organic photovoltaic devices with time-resolved soft x-ray spectroscopy. We review recent results in ultrafast soft x-ray spectroscopy of these systems and discuss routes to overcome the technical challenges in performing time-resolved x-ray experiments on photosensitive materials with poor thermal conductivity and low pump intensity thresholds for nonlinear effects.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

14 MeV Irradiation and Analysis of a 93% 239 Pu Target in Preparation for a F2019 FY22 Pu Campaign

In this work, we present the irradiation of a 93% 239 Pu with 14 MeV neutrons and subsequent analysis of the fission and activation products. The fully assembled target, a Pu metal bead encapsulated in Al, further encapsulated in welded stainless steel, was analyzed 22 times over more than 100 days using gamma emission analysis (GEA). Using the results from these analyses, R-values and fission yields for fission products were determined. To prepare for the FY22 Pu irradiation using the GODIVA critical assembly at NCERC, the irradiated Pu target was disassembled, dissolved, and separated using chemistry provided by LANL collaborators. This chemical separation was intended to remove the Pu from solution with little to no effect on the remaining elements. The chemistry was assessed to try to determine possible routes of fractionation of the sample and the fission products. The separation process used was successful for the bulk of the analyzed fission and activation products, as well as the added radiotracers. The final dissolved solution and separated fractions were analyzed by GEA looking at the remaining fission, activation and radiotracers and thermal ionization mass spectrometry analysis looking at the Pu isotopics.

14MeV↗

The optimization air separation plants for combined cycle MHD-power plant applications

Some of the design approaches being employed during a current supported study directed at developing an improved air separation process for the production of oxygen enriched air for magnetohydrodynamics (MHD) combustion are outlined. The ultimate objective is to arrive at conceptual designs of air separation plants, optimized for minimum specific power consumption and capital investment costs, for integration with MHD combined cycle power plants.

Juhasz, A. J.↗