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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Performance Criteria for Capture and/or Immobilization Technologies (Revision 1)

The capture and subsequent immobilization of regulated volatile radionuclides from the off-gas streams of a used nuclear fuel (UNF) reprocessing facility has been a topic of substantial research interest for the US Department of Energy and its international counterparts. Removal of specific radionuclides from the plant effluent streams before discharge to the environment is required to meet regulations set forth by the US Environmental Protection Agency. Upon removal, the radionuclides, as well as associated sorbents that cannot be regenerated in a cost-effective manner, are destined for conversion to a waste form. Research in separation and capture methodologies has included a wide range of technology types, and studies of waste forms are correspondingly diverse. In considering the future development and implementation of both sorbents and waste forms, it is necessary to identify benchmark measures of performance to objectively evaluate each sorbent system or waste form. Sets of performance criteria and associated metrics have been developed for sorbent and waste form evaluation. These criteria address physical, radiological, and chemical characteristics, technical practicality, technical maturity, cost, and, for sorbents, system performance. The criteria and metrics appear to be robust and should be applicable despite the eventual waste classification (as either high- or low-level waste). They are flexible enough to address both aqueous reprocessing and electrochemical reprocessing of UNF. These criteria sets can serve as tools to evaluate performance at multiple stages within the development process, and in this revision (Revision 1) they have been used to assess technologies relating to krypton/xenon separations and iodine capture from off-gas streams arising from UNF reprocessing. Assessment of krypton/xenon separations using engineered forms of two zeolite minerals (silver mordenite and hydrogen mordenite in a polyacrylonitrile-based binder [AgZ-PAN/HZ-PAN]) found that the zeolite-based separation is relatively advanced in its development, but several key issues require resolution. First, desorption processes for both krypton and xenon require refinement to provide an understanding of the product purity that can be achieved. Second, adsorption rate data is needed in order to calculate the bed depth required for effective separation. Finally, it is strongly recommended that a technical review of krypton/xenon separation by AgZ-PAN/HZ-PAN be performed to synergize available data and assess the cost savings and operational benefits that may be realized from implementation of this technology. Assessment of metal organic frameworks (MOFs) for their use in the separation of krypton/xenon found that the ideal separation would be performed using a single-column system with a MOF selective for krypton over xenon. A robust research effort should work to identify a krypton-selective MOF designed to operate at temperatures of approximately 0°C or higher, which could be preferred over cryogenic krypton/xenon capture for used fuel reprocessing off-gas streams. In the case of the CaSDB-MOF (the most well-understood xenon sorbent to date), two issues are judged of high importance. First, xenon breakthrough capacity for the CaSDB-MOF in prototypical conditions should be determined. Preliminary research indicates that breakthrough may be near immediate, presenting a substantial obstacle in separative system design. Second, development of desorption methodology should be performed to determine regeneration time, energy requirements, and the product stream composition. Silver-based sorbents (AgZ and AgAero) for use in iodine capture from the dissolver off-gas were evaluated against the established criteria. These sorbents are significantly better understood for this application as a result of research efforts over the past decade. The potential implementation of AgAero at a large scale is hindered by its physical degradation by components of the dissolver off-gas stream. Less is known about the adsorption of iodine by these sorbents from other off-gas streams in the plant. Initial experimental efforts have been closely coordinated in an effort to understand organic iodine (such as would be found in the vessel off-gas) adsorption by AgZ and AgAero. Future work should expand this experimental program, and analysis of other reprocessing facility off-gas streams such as the vitrification off-gas stream should be conducted to better understand other potential applications for iodine sorbents. A review of iodine waste form development shows that this area is diverse and that multiple promising waste forms have been identified for the immobilization of radioactive iodine. Efforts related to the direct conversion of iodine sorbents (including AgZ and AgAero) should be continued because of the advantages of direct conversion in a waste management strategy and other sorbents should continue to be advanced as merited.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS2003

RXTE and BeppoSAX Observations of MCG-5-23-16: Reflection From Distant Cold Material

We examine the spectral variability of the Seyfert 1.9 galaxy MCG-5-23-16 using RXTE and BeppoSAX observations spanning 2 years from April 1996 to April 1998. During the first year the X-ray source brightens by a factor of approximately 25% on timescales of days to months. During this time, the reprocessed continuum emission seen with RXTE does not respond measurably to the continuum increase. However, by the end of the second year during the BeppoSAX epoch the X-ray source has faded again. This time, the reprocessed emission has also faded, indicating that the reprocessed flux has responded to the continuum. If these effects are caused by time delays due to the distance between the X-ray source and the reprocessing region, we derive a light crossing time of between approximately 1 light day and approximately 1.5 light years. This corresponds to a distance of 0.001 pc to 0.55 pc, which implies that the reprocessed emission originates between 3 x 10(exp 15) cm and 1.6 x 10(exp l8) cm from the X-ray source. In other words, the reprocessing in MCG-5-23-16 is not dominated by the inner regions of a standard accretion disk.

Mattson, B. J.↗
DOE OSTI2023

Endowing Polythioester Vitrimer with Intrinsic Crystallinity and Chemical Recyclability

Abstract Technologically important thermosets face a long‐standing end‐of‐life (EoL) problem of non‐reprocessability, a more sustainable solution of which has resolved to nascent vitrimers that can merge the robust material properties of thermosets and the reprocessability of thermoplastics. However, the lifecycle of vitrimers is still finite, as they often suffer from significant deterioration of mechanical performance following multiple reprocessing cycles, analogous to mechanical recycling, and they often show undesired creep under working conditions. To address these two key limitations, we have developed a cross‐linked semi‐crystalline polythioester with both dynamic covalent bonds and intrinsic crystallinity and chemical recyclability, affording a vitrimeric system that exhibits not only reprocessability and crystallinity‐restricted creep but also complete chemical recyclability to initial monomer by catalyzed depolymerization in solution or bulk. Therefore, reported herein is an “infinite” vitrimer system that is empowered with a facile closed‐loop EoL option once serial reprocessing deteriorates performance and the material can no longer meet the application requirements. Specifically, the polythioester vitrimer was constructed by copolymerization of a bicyclic thioester with a bis‐dithiolane, producing dynamically cross‐linked polythioesters with excellent property tunability, from amorphous to semi‐crystalline states and melting transition temperatures from 91 to 178 °C.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Correlating processing variables to material properties in recycled polypropylene: A data‐driven approach

Abstract Polypropylene (PP) is one of the most widely used plastics, yet its recycling remains limited, with less than 1% of solid waste PP being reprocessed. Mechanical recycling through extrusion is the most practical method, but inconsistent reprocessing conditions introduce variability in material properties. While temperature, screw speed, and residence time influence the thermomechanical stress applied during reprocessing, there are no standardized guidelines for optimizing these parameters. This study examines how these factors shape the properties of recycled PP, using conditions designed to mimic post‐industrial recycled (PIR) scrap. Residence time was measured using colorimetric tracking and correlated with molecular weight, viscosity, and mechanical properties over multiple extrusion cycles. Data‐driven modeling, including response surface methodology, support vector machines, and artificial neural networks, identified processing temperature as the dominant factor in material degradation, followed by residence time. Mechanical properties remained stable, while viscosity decreased predictably with increasing residence time. By linking reprocessing conditions to property evolution, this study provides a method to optimize processing parameters and reduce variability in recycled PP. These findings help manufacturers improve process control, making recycled PP more predictable for reuse in manufacturing. Highlights Study of PIR‐quality PP without additives or compatibilizers. Residence time analysis shows processing temperature drives PP property changes. Mark‐Houwink enables quick molecular weight checks for quality control. Models predict mechanical and rheological shifts in reprocessing. Optimized processing parameters minimize property degradation in recycling.

Estela‐García, John E. [Polymer Engineering Center↗
DOE OSTI2024

Covalent adaptable polymer networks with CO 2 -facilitated recyclability

Cross-linked polymers with covalent adaptable networks (CANs) can be reprocessed under external stimuli owing to the exchangeability of dynamic covalent bonds. Optimization of reprocessing conditions is critical since increasing the reprocessing temperature costs more energy and even deteriorates the materials, while reducing the reprocessing temperature via molecular design usually narrows the service temperature range. Exploiting CO 2 gas as an external trigger for lowering the reprocessing barrier shows great promise in low sample contamination and environmental friendliness. Herein, we develop a type of CANs incorporated with ionic clusters that achieve CO 2 -facilitated recyclability without sacrificing performance. The presence of CO 2 can facilitate the rearrangement of ionic clusters, thus promoting the exchange of dynamic bonds. The effective stress relaxation and network rearrangement enable the system with rapid recycling under CO 2 while retaining excellent mechanical performance in working conditions. This work opens avenues to design recyclable polymer materials with tunable dynamics and responsive recyclability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Electrochemical Manipulation and Radiolytic Evaluation of Organic Phase Neptunium

Presentation for Seed LDRD proposal presentation: This Seed LDRD research proposes to test an innovative approach to precisely control the oxidation state distribution of neptunium (Np) under used nuclear fuel (UNF) reprocessing conditions using novel electrochemical methods. Current UNF reprocessing technologies are not financially viable in the US, requiring significant scientific and technological innovation to improve cost efficiency. Reducing the number of process cycles is one avenue for increasing cost efficiency, of which resolving the challenge associated with isolating Np is critical. Under envisioned process conditions, Np is present in a mixture of extractable (Np(IV) and Np(VI)) and inextractable (Np(V)) oxidation states, the distribution of which is dependent on several factors, including ionizing radiation dose, that change throughout a reprocessing scheme. Consequently, Np unintentionally partitions into various UNF reprocessing phases and product streams, ultimately increasing the number of process cycles to isolate UNF components. Here, we propose to employ novel, high surface area, optically transparent, Ligand Modified tin-doped indium oxide Electrodes (LMES). These LMEs bind Np, and therefore enable concurrent generation and spectroscopic characterization of Np oxidation states in organic solutions. These proof-of-concept experiments will: (i) facilitate optimization of the proposed electrochemical system conditions for Np oxidation state manipulation; (ii) identify the accessible electrochemical window for Np complexes in the organic phase; (iii) report characteristic optical spectra for each accessible complexed Np oxidation state; and (iv) determine the lifetime and partitioning of a given atypical Np oxidation state in the organic phase in the presence and absence of ionizing radiation fields. The data gathered by this Seed LDRD will provide support for the design of an electrochemical process concept for the precise manipulation of Np oxidation states in UNF reprocessing solvent systems, with the intention of providing advanced control over Np mass transfer, and thus greater process efficiency and economy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

MARIE: A Python-Based Framework for Comprehensive Fuel Recycling Modeling

One of the most pressing challenges to the continued deployment of nuclear energy systems is in the ultimate management and disposition of discharged fuel assemblies. While reprocessing and recovery of valuable materials from UNF assemblies has been considered as part of an overall strategy for minimization of the volume of reactor-based wastes to be managed, the deployment of commercial-scale reprocessing facilities presents an enormous economic challenge. The MARIE software package has been developed as a means of confronting this challenge. Representing components of a generic fuel reprocessing operation as individual physical processes, MARIE is designed as a modular framework intended to allow for analysis and cost-optimization for a hypothetical reprocessing facility while realistically accounting for the physical characteristics of the used fuel source term, such as decay heat, activity, and radiation dose (informing corresponding shielding requirements). Capabilities supported by MARIE include head-end operations such as fuel shearing, voloxidation, and dissolution; generic solvent extraction operations informed by available open-literature data; a suite of unit operations intended to represent electrochemical processing of used fuel assemblies (i.e., oxide reduction, electrorefining, and electrowinning); and finally, accounting for both costs and physical features of discharged waste streams, which can be used to inform follow-on analyses such as the feasibility of deep-borehole disposal of HLW. This paper presents an overview of the MARIE software capabilities, including how individual unit operations are implemented to enable a larger-scale optimization of a hypothetical reprocessing operation on aspects such as cost and recovery of valuable materials.

Skutnik, Steve [ORNL] (ORCID:000000016441135X)↗
DOE OSTI2020

Development of a Regulatory Strategy for Post Operational Clean Out Activities at Sellafield Limited Nuclear Licensed Site - 20273

The Thermal Oxide Reprocessing Plant (THORP) at the Sellafield nuclear licensed site carried out its final commercial shear of spent nuclear fuel in November 2018, since when the facility has undergone rundown prior to cessation of operations. The Magnox Reprocessing Facility (MRF) is also due to cease operating, around the end of 2020. Following the cessation of spent fuel reprocessing, the facilities and supporting infrastructure will transition into Post Operational Clean Out (POCO), which will become an increasingly significant portion of Sellafield Limited's (SL) activities. POCO is defined as the set of activities undertaken directly after a nuclear facility comes to the end of its operational life, in order to place the plant in a suitable state for the subsequent decommissioning steps. The decommissioning strategy at SL is for deferred dismantling of these facilities, which will be subject to a period of Surveillance and Maintenance (S and M) following completion of POCO. This paper outlines the development and implementation of a regulatory strategy for POCO activities at the Sellafield site by the Office for Nuclear Regulation (ONR), the independent nuclear safety, transport and security regulator in the United Kingdom. The paper also describes how this regulatory strategy is applied to nuclear installations undergoing transition into POCO and subsequent decommissioning. ONR works jointly with the Environment Agency, as the environmental regulators in England, to ensure that matters relevant to them have been duly considered. In developing a regulatory strategy, ONR has taken a site-wide approach, moving away from regulation on a facility-by-facility basis, to promote consistency, as well as maximising efficiency and effectiveness. The aim of this integrated approach was to prevent complications during future decommissioning and dismantling that have been experienced previously at similar facilities in France. The strategy recognised that once reprocessing operations are concluded, the hazard present will be reduced significantly, which provides the opportunity for ONR to consider how best to deliver a proportionate approach to regulatory interventions. Once POCO has been completed and the facility has transitioned into a period of S and M, the scale and frequency of ONR's interventions will reduce, commensurate with the safety case covering the remaining hazard and activities associated with maintaining the facility prior to final decommissioning. This approach allows ONR to consider risks holistically, considering the full life cycle of the facility and by taking due account of the interdependencies between facilities across the site. The strategy also aligns with existing regulation of high hazard and risk reduction activities, which remain ONR's top priority. As SL progresses with POCO activities in THORP and across the rest of the site, ONR will review its regulatory strategy to ensure that the intended safety benefits are realised. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Updates to a Preliminary Probabilistic Performance Assessment Model for Radiological and Chemical Contamination at the West Valley Site, New York - 20420

The New York State Energy Research and Development Authority (NYSERDA) is the owner of the Western New York Nuclear Service Center (WNYNSC), a 1,351-ha site located approximately 48 km south of Buffalo, New York. In 1962, Nuclear Fuel Services, Inc. (NFS) entered into agreements with the Atomic Energy Commission and New York State to construct the first commercial reprocessing plant of nuclear fuel in the United States at the WNYNSC. NFS built and operated the spent fuel reprocessing plant and waste disposal facilities, processing 640 Mg (640 metric tons) of spent nuclear fuel from 1966 to 1972 under an Atomic Energy Commission license. Nuclear fuel reprocessing operations halted in 1972 and never restarted, leaving behind radioactive and chemical wastes. The U.S. Department of Energy (DOE) was required to complete certain waste management activities under the West Valley Demonstration Project (WVDP) Act of 1980 including decommissioning of WVDP facilities. As collaborating agencies, NYSERDA and the DOE are tasked with making decisions about decommissioning and risk reduction for the West Valley Site. Neptune and Company, Inc. (Neptune) was contracted to develop a probabilistic performance assessment (PPA) model to assist the agencies in their decision making process for decommissioning the WVDP and WNYNSC. One important tool that is needed in order to inform the decision-making process is a science-based model of the West Valley Site that evaluates potential future consequences for human health and the environment. This forms the core of the spatial domain of the West Valley PPA Model. The PPA Model, developed using the GoldSim system modeling software, is a tool intended to provide support for decision making that evaluates uncertainty, in a manner that is transparent, defensible, and robust. The PPA Model includes contaminant transport and health effects components, and is organized around geographically-grouped contaminated facilities. These include the waste disposal areas licensed by the U.S. Nuclear Regulatory Commission and the State of New York, a waste tank farm for storage of high level radioactive waste resulting from reprocessing operations, and several areas contaminated with radioactive and chemical constituents. The PPA Model evaluates contaminant transport from these sources to points of exposure across the site and into receiving surface waters and sediments. Hypothetical people and wildlife could be exposed to contamination at these locations, and the effects of these exposures are evaluated. Contaminant transport processes to be evaluated in the PPA Model include groundwater and surface water transport, contaminant translocation by plants and animals, diffusion, and erosion. The evaluation of exposures to people in this preliminary model is limited to a resident farmer scenario, and ecological assessment is performed at the level of a screening analysis. The results of these preliminary evaluations inform future model developments. PPA Model results are subjected to sensitivity analysis in order to determine those pathways and parameters that are most significant in influencing the results. This information allows analysts and decision makers to focus on those aspects of Site behavior and processes. With this information, the decision makers can drive informed, defensible decisions regarding decommissioning of the Site. This paper includes an update of the information presented at WM2019 [1]. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Self-Adjusting Metal–Organic Framework for Efficient Capture of Trace Xenon and Krypton

The capture of the xenon and krypton from nuclear reprocessing off-gas is essential to the treatment of radioactive waste. Although various porous materials have been employed to capture Xe and Kr, the development of high-performance adsorbents capable of trapping Xe/Kr at very low partial pressure as in the nuclear reprocessing off-gas conditions remains challenging. Herein, we report a self-adjusting metal-organic framework based on multiple weak binding interactions to capture trace Xe and Kr from the nuclear reprocessing off-gas. The self-adjusting behavior of ATC-Cu and its mechanism have been visualized by the in-situ single-crystal X-ray diffraction studies and theoretical calculations. The self-adjusting behavior endows ATC-Cu unprecedented uptake capacities of 2.65 and 0.52 mmol g -1 for Xe and Kr respectively at 0.1 bar and 298 K, as well as the record Xe capture capability from the nuclear reprocessing off-gas. Further, our work not only provides a benchmark Xe adsorbent but proposes a new route to construct smart materials for efficient separations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

A literature review of pyroprocessing safeguards

Pyroprocessing is a promising technology for reprocessing used nuclear fuel (UNF) from light water reactors (LWR) and sodium fast reactors (SFR). With the advancement of fast reactors with projects from companies such as TerraPower, the prospects of pyroprocessing are more promising than ever before, as fast reactors can consume all actinides, not just uranium and plutonium. Before pyroprocessing can be implemented commercially, pre-existing safeguards used for aqueous reprocessing must be adapted for pyroprocessing. Safeguards, as determined by both the Nuclear Regulatory Commission (NRC) and the International Atomic Energy Agency (IAEA), are discussed in this review as guidelines for approaches used in both domestic and international reprocessing plants. The implementation of safeguards in aqueous reprocessing was then reviewed based on the experience from existing aqueous facilities. The experimental pyroprocessing facilities were identified as pyroprocessing plants in the design stage with one operating exception of the Fuel Conditioning Facility (FCF). The safeguard methods implemented or designed for each and the accompanying challenges of utilizing existing safeguards in pyroprocessing are considered and a summary of applicable approaches is included.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Integrated Off-gas System: A Preconceptual Design of an Integrated Off-Gas Treatment System

The U.S. has a vested interest in the advancement of nuclear energy to achieve aggressive net-zero goals, with reprocessing and recycling of used nuclear fuels (UNF) playing a vital role. It will not be possible to meet U.S. regulatory requirements without robust off-gas treatment, so it is crucial to advance treatment technologies to facilitate the design of future reprocessing facilities. For many years, teams of researchers across the U.S. Department of Energy (DOE) National Laboratory complex have been investigating off-gas treatment technologies for the capture and removal of volatile radionuclides (i.e., 85 Kr, Xe, 14 C, and 129 I) and oxides of nitrogen (NO X ) that are produced from reprocessing. These investigations have been focused on developing individual technologies for the capture of Kr, Xe, iodine, and CO 2 . Capture technologies for each constituent were tested independently from one another by utilizing nonradioactive surrogates to simulate simplified off-gas streams. The tests have been relatively small, laboratory-scale experiments of up to approximately 1 L/minute total gas flow rate. To increase the readiness of these technologies for deployment, an integrated test system with a larger-scale capacity is needed to bridge the gap between promising bench scale and fully scalable UNF reprocessing off-gas treatment. This document contains the goals, design basis, functional requirements, preconceptual design, and cost estimates for an integrated off-gas demonstration system for the capture and removal of NO x , Kr, Xe, CO 2 , and iodine at 10× higher throughput than earlier laboratory studies. The order-of-magnitude cost estimate for this system is approximately $\$$886,000. Next phases include conceptual design, detailed design, fabrication, and commissioning.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1994

On the modulated light in the intermediate polar FO Aquarii/H 2215-086

The modulated light in the Intermediate Polar FO Aqr at the three periods P(sub spin) = 20.9 min, P(sub orb) = 4.85 hr and P(sub beat) = 22.5 min is studied in different spectral ranges to derive information on their nature. In this system the accretion geometry, with or without an accretion disk, is still a matter of debate (Hellier 1991; Norton et al. 1992). The different orbital behavior of phase coherence between the spin and beat pulses in the X-rays (Norton et al. 1992) and in the optical/IR regions cannot be easily accounted for by only a diskless dominated geometry where the accretion flow is switching from one pole to the other each half of the beat period. We therefore propose an accretion scenario where a non-axisymmetric disk is present. In such a non-standard accretion disk an azimuthal structure provides not only the source of variable mass transfer to the white dwarf, but also a reprocessing site which is mainly viewing the X-ray emission from the lower pole. Our spectral analysis shows that reprocessing is also occurring at the surface of the secondary star. The spin pulsation in the optical and IR continua can be explained by the so-called 'accretion curtain' model (Rosen et al. 1988) though an additional reprocessing component at the spin period cannot be excluded. In contrast to the X-rays, the beat optical/IR modulation is not intrinsic. Reprocessing at the surface of the secondary star and at the thickened part of the disk can also account for the orbital modulation in the UV, optical and IR regions.

Martino, D. DE↗
NASA NTRS1998

Variability Analysis and the Structure of Active Galactic Nuclei

This five-year Long-Term Space Astrophysics grant provided the support for several major steps in advancing our knowledge of the internal structure of active galactic nuclei. The single largest portion of this program had to do with the development and application of techniques for "reverberation mapping", the use of spectral monitoring of several different bands related by radiation reprocessing to infer the internal geometry of sources. Major steps were taken in this regard, particularly in establishing the distribution in radius of emission line material, and in relating the apparent reprocessing of continuum bands to the underlying structure of the accretion disk. Another major effort built directly upon these results. Once the case for continuum reprocessing was made by the monitoring, it next behooved us to understand the spectral output of AGN as a result of this reprocessing. As a result, our view of continuum production in AGN is now much better focussed on the key problems. A third focus of effort had to do with the nature of X-ray variability in AGN, and what it can tell us about the dynamics of extremely hot material in the immediate outskirts of the supermassive black holes that form the central engines of active galactic nuclei. In addition to these primary efforts, this grant also supported many other, smaller projects. Several of these were demonstrations of how the material spewed out of AGN in relativistic.ets generate the radiation by which we observe them. J Finally, the portion of this study that had to do with continuum production by accretion disks in AGN led naturally to several papers in which new developments were presented having to do with "advection-dominated accretion disks", those disks in which accretion appears to proceed at a substantial rate, but in which radiation processes are weak.

Krolik, Julian H.↗
NASA NTRS1998

Variability Analysis and the Structure of Active Galactic Nuclei

This five-year Long-Term Space Astrophysics grant provided the support for several major steps in advancing our knowledge of the internal structure of active galactic nuclei. The single largest portion of this program had to do with the development and application of techniques for 'reverberation mapping, the use of spectral monitoring of several different bands related by radiation reprocessing to infer the internal geometry of sources. Major steps were taken in d-ds regard, particularly in establishing the distribution in radius of emission line material, and in relating the apparent reprocessing of continuum bands to the underlying structure of the accretion disk. Another major effort built directly upon these results. Once the case for continuum reprocessing was made by the monitoring, it next behooved us to understand the spectral output of AGN as a result of this reprocessing. As a result, our view of continuum production in AGN is now much better focussed on the key problems. A third focus of effort had to do with the nature of X-ray variability in AGN, and what it can tell us about the dynamics of extremely hot material in the immediate outskirts of the supermassive black holes that form the central engines of active galactic nuclei. In addition to these primary efforts, this grant also supported many other, smaller projects. Several of these were demonstrations of how the material spewed out of AGN in relativistic jets generate the radiation by which we observe them. Finally, the portion of this study that had to do with continuum production by accretion disks in AGN led naturally to several papers in which new developments were presented having to do with 'advection-dominated accretion disks', those disks in which accretion appears to proceed at a substantial rate, but in which radiation processes are weak.

Krolik, Julian H.↗
NASA NTRS2000

SeaWiFS Postlaunch Calibration and Validation Analyses

The effort to resolve data quality issues and improve on the initial data evaluation methodologies of the SeaWiFS Project was an extensive one. These evaluations have resulted, to date, in three major reprocessings of the entire data set where each reprocessing addressed the data quality issues that could be identified up to the time of the reprocessing. Three volumes of the SeaWiFS Postlaunch Technical Report Series (Volumes 9, 10, and 11) are needed to document the improvements implemented since launch. Volume 10 continues the sequential presentation of postlaunch data analysis and algorithm descriptions begun in Volume 9. Chapter 1 of Volume 10 describes an absorbing aerosol index, similar to that produced by the Total Ozone Mapping Spectrometer (TOMS) Project, which is used to flag pixels contaminated by absorbing aerosols, such as, dust and smoke. Chapter 2 discusses the algorithm being used to remove SeaWiFS out-of-band radiance from the water-leaving radiances. Chapter 3 provides an itemization of all significant changes in the processing algorithms for each of the first three reprocessings. Chapter 4 shows the time series of global clear water and deep-water (depths greater than 1,000m) bio-optical and atmospheric properties (normalized water-leaving radiances, chlorophyll, atmospheric optical depth, etc.) based on the eight-day composites as a check on the sensor calibration stability. Chapter 5 examines the variation in the derived products with scan angle using high resolution data around Hawaii to test for residual scan modulation effects and atmospheric correction biases. Chapter 6 provides a methodology for evaluating the atmospheric correction algorithm and atmospheric derived products using ground-based observations. Similarly, Chapter 7 presents match-up comparisons of coincident satellite and in situ data to determine the accuracy of the water-leaving radiances, chlorophyll a, and K(490) products.

Hooker, Stanford B.↗
NASA NTRS2003

Iron K Lines from Gamma Ray Bursts

We present models for reprocessing of an intense flux of X-rays and gamma rays expected in the vicinity of gamma ray burst sources. We consider the transfer and reprocessing of the energetic photons into observable features in the X-ray band, notably the K lines of iron. Our models are based on the assumption that the gas is sufficiently dense to allow the microphysical processes to be in a steady state, thus allowing efficient line emission with modest reprocessing mass and elemental abundances ranging from solar to moderately enriched. We show that the reprocessing is enhanced by down-Comptonization of photons whose energy would otherwise be too high to absorb on iron, and that pair production can have an effect on enhancing the line production. Both "distant" reprocessors such as supernova or wind remnants and "nearby" reprocessors such as outer stellar envelopes can reproduce the observed line fluxes with Fe abundances 30-100 times above solar, depending on the incidence angle. The high incidence angles required arise naturally only in nearby models, which for plausible values can reach Fe line to continuum ratios close to the reported values.

Kallman, T. R.↗
DOE OSTI2022

Impact of f-element complexation on the radiolytic robustness of separations ligands

Impact of f-element complexation on the radiolytic robustness of separations ligands Gregory P. Horne, Makayla R. Baxter, Corey D. Pilgrim, Travis S. Grimes, Center for Radiation Chemistry Research, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID, 83415, USA Cristian Celis Barros, Department of Chemistry and Biochemistry, Florida State University, Tallahassee, FL 32306, USA. E-mail: ccelisbarros@fsu.edu Andrew R. Cook, Department of Chemistry, Brookhaven National Laboratory, Upton, New York, 11973, USA Stephen P. Mezyk, Department of Chemistry and Biochemistry, California State University Long Beach, 1250 Bellflower Boulevard, Long Beach, California, 90840-9507, USA The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. However, the complexity and intensity of these effects are greatest during the management of used nuclear fuel, owing to the presence of a wide spectrum of radionuclides from neutron capture and fission processes. With regards to used nuclear fuel (UNF) reprocessing, radiation-induced processes typically promote the destruction of active compounds (e.g., complexants and additives) with the concomitant formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of a given reprocessing system. Concerning UNF complexants, radiation chemistry studies have historically focused on their radiation robustness in the absence of the metal ions they were designed to selectively complex. This knowledge gap is worrisome as previous studies on aqueous phase complexants have demonstrated significant changes in radiolytic behavior upon metal ion complexation.1-4 More recently, the rate of reaction of the n-dodecane radical cation—believed to be the major organic phase radiation-induced transient species responsible for complexant radiolysis in n-dodecane based solvent systems—with hexa-n-octylnitrilo-triacetamide (HONTA) was shown to increase by an order-of-magnitude upon complexation of europium or americium.5 These findings have significant implications on the projected longevity of complexants in UNF reprocessing solvent systems. Consequently, a thorough understanding of metal ion complexation effects on the radiolytic integrity of UNF complexants is essential to evaluate their potential for process application. Presented here are two recent studies from the Idaho National Laboratory Center for Radiation Chemistry Research group that demonstrate the various impacts of f-element complexation (uranium, americium, and lanthanides) on the radiolytic integrity (gamma and electron pulse) of tributyl phosphate (TBP), N,N-di-(2-ethylhexyl)butyramide (DEHBA), N,N-di-2-ethylhexylisobutryamide (DEHiBA), and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) under UNF reprocessing conditions. References 1) Bhattacharyya and Kundu, Int. J. Radiat. Phys. Chem., 1971, 3, 1. 2) Kundu and Matuura, Int. J. Radiat. Phys. Chem., 1975, 7, 565. 3) Ilan and Czapski, Biochimica et Biophysica Acta, 1977, 498, 386. 4) Buettner, Doherty, and Patterson, Fed. Euro. Biochem. Soc., 1983, 158 (1), 143. 5) Toigawa, Peterman, Meeker, Grimes, Zalupski, Mezyk, Cook, Yamashita, Kumagai, Matsumura, Horne, PCCP, 2021, 23, 1343.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗