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At least 55 records · Page 3

Radiolytic evaluation of acetohydroxamic acid (AHA) under biphasic (n-dodecane and TBP/DEHBA/DEHiBA) used nuclear fuel reprocessing conditions

Acetohydroxamic acid (AHA) has been proposed as a substitute for uranium(IV) and hydrazine as a plutonium complexant and neptunium reductant for simplified, single-cycle used nuclear fuel reprocessing flowsheets. However, the chemical behavior of AHA in an intense multi-component radiation field is poorly understood, especially under representative biphasic reprocessing solvent system conditions. In response to this critical knowledge gap, this study has investigated the gamma radiolytic integrity of AHA in aqueous nitric solutions in contact with an organic phase, comprising current and future reprocessing ligands (TBP, DEHBA, and DEHiBA) dissolved in n-dodecane diluent. Our data show negligible effect of the organic phase on the radiolytic behavior of AHA compared to complementary single-phase experiments.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Actinide Radiation Chemistry and Used Nuclear Fuel Reprocessing

Although the actinides boast many unique physical and chemical properties, their inherent susceptibility to radioactive decay—and subsequent consequences of radiation-induced chemistry—are what make them truly interesting and challenging elements to understand. From a closed nuclear fuel cycle perspective, the ability to predict and control the effects of actinide-driven radiolysis is critical for the design, development, and deployment of advanced used nuclear fuel reprocessing strategies and technologies. The absorption of ionizing radiation from actinide decay leads to the formation of a variety of transient and steady-state radicals, ions, and molecular radiolysis products that can lead to significant changes in a reprocessing solvent system’s physical and chemical properties, which ultimately limits that process’ efficiency and longevity. Presented here is an overview of recent advances in actinide radiation chemistry as it applied to used nuclear fuel reprocessing.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Elucidating the Radiation-Induced Redox Chemistry of Plutonium Under Used Nuclear Fuel Reprocessing Conditions

Plutonium plays a critical role in the development of sustainable nuclear fuel cycles, and yet, our fundamental understanding of this element’s inherent radiation-induced redox chemistry and associated impacts on nuclear fuel cycle technologies is limited. Unanticipated changes in oxidation state distribution can influence the speciation and transport of plutonium in a given process. Control of these parameters is especially important for used nuclear fuel reprocessing technologies, wherein the separation and recovery of plutonium is typically achieved by the selective formation, maintenance, and complexation of specific oxidation states. Furthermore, plutonium’s inherent radiation-induced redox chemistry has the capacity to influence the radiolytic behavior of its complexes, the longevity of which are critical in the design of efficient and cost-effective advanced reprocessing technologies. These radiation-induced processes are unavoidable under fuel cycle conditions owing to the inherency of ionizing radiation fields to the decay of plutonium’s isotopes and to the various other radioisotopes generated by nuclear fission and neutron-capture process and the subsequent radioactive decay of their products. As such, mechanistically understanding the response of plutonium’s multiple oxidation states to multi-component ionizing radiation fields is essential for predicting the behavior of this critical element under used nuclear fuel reprocessing conditions. Here, through a combination of time-resolved (electron pulse) and steady-state (alpha and gamma) irradiation experiments complemented by quantitative, multiscale modeling calculations, we present advances in our understanding of radiation-induced plutonium redox chemistry!

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radiation Effects in Next Generation Used Nuclear Fuel Reprocessing Strategies

With the global community committed to significantly expanding nuclear energy capacity, the development of efficient used nuclear fuel (UNF) management strategies has become more critical than ever. These strategies are vital to fostering the widespread adoption of closed fuel cycles, which are essential for sustainable nuclear energy production and security. Achieving this ambitious goal necessitates a comprehensive understanding of radiation effects on next-generation technologies, as radiolysis can often limit the longevity and performance of these systems. This seminar will provide an overview of next-generation UNF reprocessing strategies, highlighting the latest advancements and innovative approaches in the field. Particular attention will be given to two key areas of recent research: 1. Radiation robustness and performance of advanced sulfur chloride-based chlorination technologies. We will explore the efficacy of sulfur chloride-based chlorination processes in the presence of surrogate cladding materials, specifically aluminum. These processes have shown promise in the dissolution, decontamination, and recovery of cladding materials for reuse. Detailed findings on how the composition and performance of these sulfur chloride solvents respond to radiation exposure will be discussed. 2. Impacts of metal ion complexation and direct dissolution conditions on monoamide-based reprocessing strategies. We will delve into the time-resolved and dose accumulation effects of irradiation on the direct dissolution of voloxidized uranium and rhenium using N,N-di-(2-ethylhexyl) butyramide (DEHBA) or N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) in pre-equilibrated n-dodecane solvent. The implications of these interactions on dissolution efficiency, radiolytic stability, and overall process performance will be examined. These studies aim to underscore the importance of understanding radiation effects in the development of next-generation UNF reprocessing technologies and the global transition towards more sustainable and efficient nuclear energy systems.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗

Covalent Adaptable Networks: Reprocessable Cross-Linked Polymers

Thermoset polymers have desirable properties, such as excellent thermal and mechanical stability, but their covalent cross-links typically prevent repair or recycling. By enabling and controlling dynamic exchange reactions within polymer networks, their covalent bonds rearrange and allow the polymer to be reshaped. These viscoelastic polymer networks, now known as covalent adaptable networks (CANs), are an important frontier for improving plastic circularity, as well as for designing valuable stimuli-responsive materials. This Review describes the history of CANs, dating back to the early days of polymer science, and the evolution of their classification and nomenclature. A comprehensive survey of dynamic reactions and linkage chemistries is provided, as well as methods to characterize and reprocess CANs. Beyond straightforward reprocessing, many advanced applications of CANs and their composites are now emerging. Lastly, we provide perspective on how the development of new chemistries, strategies to control stimuli-responsive bond exchange and mechanical properties, and a deep understanding of exchange reactions will advance this field toward scalable, sustainable, and high-value materials.

Sun, Molly [Northwestern University, Evanston, IL ↗

The Future of Nuclear Energy: Electrochemical Reprocessing of Fuel Takes Center Stage

Nuclear power plants use energy-dense fuel and provide dependable baseload energy without generating greenhouse gas emissions. Despite these advantages, the long-term management of used nuclear fuel (UNF) remains a key challenge due to its lifetime (hundreds of thousands of years) and radiotoxicity. The components of UNF that contribute the most to this challenge are the actinide elements. A potential solution to this issue is to separate these radioisotopes from the bulk of the UNF and recycle them as fuel in advanced nuclear reactors. These separations can be achieved using electrochemical reprocessing, which employs electrochemical conversion and electrodeposition in a high-temperature molten salt electrolyte medium to separate the actinides from UNF. In this work, we review the current status, fundamental challenges, and future prospects of electrochemical reprocessing as they relate to UNF recycling.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

BE Ursae Majoris - A detached binary with a unique reprocessing spectrum

New infrared photometry, optical and UV spectrophotometry, and a photographic ephemeris are presented for the detached binary BE UMa. Results show the primary to be a DO white dwarf with an effective temperature of 80,000 + or - 15,000 K and a mass of 0.6 + or - 0.1 solar masses. No evidence is found for variability of the primary. The main-sequence secondary star is shown to be of early-M spectral type, with a formal range of M1-M5 being possible. A reflection effect in reprocessed line and continum radiation is produced by EUV radiation from the primary incident on the secondary atmosphere. It is suggested that the temperature of the reprocessed component of the secondary's atmosphere is in the 5000-8500 K range, and that emission lines of decreasing ionization form deeper in the irradiated envelope. Relatively narrow He II and high-excitation metal lines are formed from recombination and continuum fluorescence processes.

Ferguson, Donald H.↗

BE Ursae Majoris: A detached binary with a unique reprocessing spectrum

New infrared photometry, optical and UV spectrophotometry, and a photographic ephemeris are presented for the detached binary BE UMa. Results show the primary to be a DO white dwarf with an effective temperature of 80,000 + or - 15,000 K and a mass of 0.6 + or - 0.1 solar masses. No evidence is found for variability of the primary. The main sequence secondary star is shown to be of early M spectral type, with a formal range of M1 to M5 being possible. A reflection effect in reprocessed line and continuum radiation is produced by EUV radiation from the primary incident on the secondary atmosphere. It is suggested that the temperature of the reprocessed component of the secondary's atmosphere is in the 5000 to 8500 K range, and that emission lines of decreasing ionization form deeper in the irradiated envelope. Relatively narrow He II and high excitation metal lines are formed from recombination and continuum fluorescence processes.

Ferguson, Donald H.↗

External comparisons of reprocessed SBUV/TOMS ozone data

Ozone Retrievals from the Solar Backscatter Ultraviolet (SBUV) Instrument on-board the Nimbus-7 Satellite have been reprocessed using an improved internal calibration. The resulting data set covering November, 1978 through January, 1987 has been archived at the National Space Science Data Center in Greenbelt, Maryland. The reprocessed SBUV total ozone data as well as recalibrated Total Ozone Mapping Spectrometer (TOMS) data are compared with total ozone measurements from a network of ground based Dobson spectrophotometers. The SBUV also measures the vertical distribution of ozone, and these measurements are compared with external measurements made by SAGE II, Umkehr, and Ozonesondes. Special attention is paid to long-term changes in ozone bias.

Wellemeyer, C. G.↗

Echo Tomography of Reprocessing Sites in X-Ray Binaries

We discovered correlated rapid variability between the optical/UV and X-ray emission for the first time in a soft X-ray transient, GRO J1655-40. Hubble Space Telescope light curves show features similar to those seen by the Rossi X-ray Timing Explorer, but with a mean delay of up to 10 - 20 s. We interpret the correlation as the result of reprocessing of X-rays into optical and UV emission, with a delay owing to finite light travel time; this assumption enables us to perform echo mapping of the system. The time-delay distribution has a mean of 14.6 +/-1.4 s and a dispersion of 10.5+/-1.9 s at binary phase 0.4. This establishes that the reprocessing region is the accretion disk around the compact star, rather than the mass-donating secondary. These results have been published.

Patterson, Joseph↗

Reprocessing Microflare Data

The report concerns work on detecting and cataloging solar microflares using an automated. An accompanying figure represents the solar microflare distribution during the period of April 1991 to November 1992, the height of solar activity after the launch of CGRO. It also shows the distribution extending below the distribution obtained at GSFC by manual means. We have implemented significant refinements in the search algorithm. The algorithm in its simplest form searches for transient events and based upon the distribution of the signal among the different BATSE detectors, we can assign it to be of solar origin if the signal distribution conforms to what one expects from a burst or transient from that direction. One of the major problems in an earlier effort was to search for microflares and large flares simultaneously. The requirement for a dynamic range of almost 10(exp 4) resulted in ambiguous identifications at the low side of the distribution. We have since restricted the search to events with peak count rates under 2000/s. Larger events are easily identified in the manual search, so we have chosen not to duplicate that work. The second problem was that missing counts existed below channel 0 in the BATSE Large Area Detector (LAD) data. These have been recovered and are now included in the search process. This provides data below 20 keV, and as we get closer to the thermal part of the spectrum, it provides greater sensitivity. The third problem was that too many BATSE detectors were used in the search. Detectors with pointing directions far from the Sun, although detecting the event, had poorly known responses. Detectors greater than approximately 60 degrees off the Sun are no longer included in the search process. By reducing the systematic errors with the large off-axis detectors we can conduct more rigorous statistical tests of a candidate event to ascertain whether it originated from the solar direction. We have reprocessed the period in the early mission that covers solar maximum and constructed the microflare distribution shown in the figure. The results of the automated search start to deviate from the manual search results below about 1000/s. Not only do we now have this distribution but we have a database of solar microflares that was used to construct the distribution. This database contains the signal at higher energy channels as well as that in channel zero (and below). From this one can, using software at GSFC, construct a photon spectrum for some of the larger microflares. It can also be used in other solar studies, especially those that correlate the X-ray flux with emission at other wavelengths. With some additional effort we hope to integrate this database into the corresponding one residing at the Solar Data Analysis Center at GSFC. The entire CGRO mission's data can now be reprocessed to obtain the microflare distribution at all phases of the solar cycle. This work is in progress. The results of this work will be presented in forthcoming scientific workshops and conferences.

Ryan, James M.↗

Spatial and Temporal Distribution of Cloud Properties Observed by MODIS: Preliminary Level-3 Results from the Collection 5 Reprocessing

The Moderate Resolution Imaging Spectroradiometer (MODIS) was developed by NASA and launched onboard the Terra spacecraft on December 18, 1999 and Aqua spacecraft on May 4, 2002. It achieved its final orbit and began Earth observations on February 24, 2000 for Terra and June 24, 2002 for Aqua. A comprehensive set of operational algorithms for the retrieval of cloud physical and optical properties (optical thickness, effective particle radius, water path, thermodynamic phase) have recently been updated and are being used in the new "Collection 5" processing stream being produced by the MODIS Adaptive Processing System (MODAPS) at NASA GSFC. All Terra and Aqua data are undergoing Collection 5 reprocessing with an expected completion date by the end of 2006. The archived products from these algorithms include 1 km pixel-level (Level-2) and global gridded Level-3 products. The cloud products have applications in climate change studies, climate modeling, numerical weather prediction, as well as fundamental atmospheric research. In this talk, we will summarize the available Level-3 cloud properties and their associated statistical data sets, and show preliminary Terra and Aqua results from the available Collection 5 reprocessing effort. Anticipated results include the latitudinal distribution of cloud optical and radiative properties for both liquid water and ice clouds, as well as joint histograms of cloud optical thickness and effective radius for selected geographical locations around the world.

King, Michael D.↗

On the Reprocessing and Reanalysis of Observations for Climate

The long observational record is critical to our understanding of the Earth s climate, but most observing systems were not developed with a climate objective in mind. As a result, tremendous efforts have gone into assessing and reprocessing the data records to improve their usefulness in climate studies. Many challenges remain, such as tracking the improvement of processing algorithms and limited spatial coverage. Reanalyses have fostered significant research, yet reliable global trends in many physical fields are not yet attainable, despite significant advances in data assimilation and numerical modeling. Communication of the strengths, limitations and uncertainties of reprocessed observations and reanalysis data, not only among the community of developers, but also with the extended research community, including the new generations of researchers and the decision makers is crucial for further advancement of the observational data records. WCRP provides the means to bridge the different motivating objectives on which national efforts focus.

Bosilovich, Michael G.↗

65 Years of Reprocessed GLDAS Version 2.0 Data and Their Exploration Using the NASA GES DISC Giovanni

GLDAS-2.0 data have been reprocessed with updated Princeton meteorological forcing data within the Land Information System (LIS) Version 7, and temporal coverage have been extended to 1948-2012.Global Land Data Assimilation System Version 2 (GLDAS-2) has two components: GLDAS-2.0: entirely forced with the Princeton meteorological forcing data GLDAS-2.1: forced with atmospheric analysis and observation-based data after 2001In order to create more climatologically consistent data sets, NASA GSFC's Hydrological Sciences Laboratory (HSL) has recently reprocessed the GLDAS-2.0, by using updated Princeton meteorological forcing data within the LIS Version 7.GLDAS-2.0 data and data services are provided at NASA GES DISC Hydrology Data and Information Services Center (HDISC), in collaboration with HSL.

data assimilation↗

Dome Degradation Characterization of Wide-Field-of-View Nonscanner Aboard ERBE and Its Reprocessing

Earth Radiation Budget Experiment (ERBE) wide-field-of-view (WFOV) nonscanners aboard ERBS and NOAA- 9/NOAA-10 provided broadband shortwave and longwave irradiances from 1985 to 1999. The previous analysis showed dome degradation in the shortwave nonscanner instruments. The correction was performed with a constant spectral (gray assumption) degradation. We suspect that the gray assumption affected daytime longwave irradiance and led to a day-minus-night longwave flux differences (little change in night time longwave) increase over time. Based on knowledge from the CERES process, we will reprocess entire ERBE nonscanner radiation dataset by characterizing shortwave dome transmissivity with spectral dependent degradation using the solar data observed by these instruments. Once spectral dependent degradation is derived, imager derived cloud fraction and the cloud phase as well as surface type over the FOV of nonscanner instruments will be used to model unfiltering coefficients. This poster primarily explains the reprocessing techniques and includes initial comparison of several months of data processed with existing and our recent methods.

Shrestha, Alok K.↗

Multiscale Evaluation of Acetohydroxamic Acid (AHA) Radiolysis Under Used Nuclear Fuel Reprocessing Solvent System Conditions

Acetohydroxamic acid (AHA) has been proposed as an alternative agent for the selective separation of plutonium and neptunium from co-extracted uranium during the reprocessing of used nuclear fuel. However, the fundamental radiolytic behavior of this molecule under envisioned process conditions – i.e., acidic biphasic solvent systems – is not sufficiently understood to support process applications. Here we present a systematic irradiation study (steady-state gamma and time-resolved pulsed electron) into the radiolytic integrity of AHA and formation of degradation products in aqueous nitric acid (HNO3) solutions (0.2 M) in presence and absence of an organic phase, comprising current (tri-butyl phosphate - TBP) and future (N,N-di-(2-ethylhexyl)butyramide - DEHBA and di-2-ethylhexylisobutyramide - DEHiBA) reprocessing ligands dissolved in n-dodecane diluent. Experimental data are complimented by predictive multiscale model calculations for the elucidation of underpinning mechanisms.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Adsorption of molecular iodine and alkyl iodides from spent-nuclear-fuel-reprocessing off-gas using reduced silver mordenite

Radioactive iodine is a hazardous byproduct of spent-nuclear-fuel reprocessing that must be removed from the off-gas stream before it can be discharged. Reduced silver mordenite (Ag 0 Z) is currently the baseline material for iodine capture in the U.S. Although the performance characteristics and capture mechanisms of I 2 and CH 3 I have been established, similar investigations into long-chain organic iodides have yet to be performed. In this study, thin beds of Ag 0 Z were loaded with I 2 , CH 3 I, C 4 H 9 I, and C 12 H 25 I (5 ppm to 50 ppm) carried in a dry air stream at 150°C. The maximum iodine capacity was 105 ± 5 mg I/g Ag 0 Z for all species. Saturated Ag 0 Z samples were characterized using scanning electron microscopy, X-ray fluorescence, X-ray photoelectron spectroscopy, diffuse reflectance UV–visible spectroscopy, pair distribution function analysis, and thermogravimetric analysis. Further, near-complete Ag utilization and similar physical/chemical properties were observed for all samples. Through a comparison with previous studies and an investigation of aged Ag 0 Z, we propose that iodine species react with Ag + at exchange sites, forming α-AgI within the mordenite channels, and with surface Ag 0 nanoparticles, yielding β-/γ-AgI. The available Ag sites in the interior (Ag + ) and exterior (Ag 0 ) of mordenite determine the adsorption capacity since α-AgI formation is limited by the total pore volume. Potential iodine uptake routes were summarized for aging and non-aging environments. A scalable predictive model was implemented for deep-bed iodine removal, and predictions were in good agreement with experimental data. Sensitivity analysis suggests that iodine uptake kinetics is governed by pore diffusion.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗