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Impacts of Lanthanide Ion Complexation on the Radiation Robustness of Diglycolamide Extractants

Nuclear power reactors represent a clean and reliable source of baseload energy. However, nuclear reactors produce used nuclear fuel (UNF), which, if not recycled/reprocessed, must be disposed of as high-level radioactive waste, necessitating long-term storage options. UNF contains approximately a third of the periodic table, including the radioactive minor actinides (MA) americium and curium. Removal of these MA from UNF would greatly reduce the radiotoxic burden, volume, and cost of a storage facility or geological repository. Thus, a significant global effort has been devoted to the design of reprocessing strategies for the clean separation of the MA from UNF. As MA separations are difficult, due to the presence of lanthanide elements in UNF and their remarkably similar chemical properties, many extractants have been studied. The diglycolamide (DGA) class of extractants are promising for this separation as they exhibit high distribution coefficients for the MAs, high metal loading capacities, and are robust in highly acidic radiation environments.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Monodisperse porous polymer particles containing macrocyclic ether as a new class of sorbent for SR(II) separation

Strontium{sup 90} is one of the typical fission products that may be found in high level liquid waste (HLLW). Separation of Sr{sup 90} prior to the vitrification is beneficial to the final treatment of solid radioactive waste. In this study, a new class of sorbent for Sr(II) was developed by loading the macrocyclic ether DtBuCH18C6 into the monodisperse porous polymer particles (MPPPs). The MPPPs are well-known as a promising chromatographic material due to the uniform particle size, porous morphology, good compatibility with organic extractants, and rigid matrix. The structure and micro-morphology of the sorbent particles were characterized. The adsorption behavior towards Sr(II) in HNO{sub 3} media was investigated by both batch and column experiments. High adsorption efficiency and selective separation of Sr(II) was obtained. The sorbent particles can be recycled for at least several times before obvious lose of the adsorption ability. This kind of sorbent possesses the potential to be used for strontium separation in radioactive liquid waste.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Xe/Kr Selectivity Measurements using AgZ-PAN at Various Temperatures

In preparation for planned FY-15 Xe/Kr multi-column testing, a series of experiments were performed to determine the selectivity of Xe over Kr using the silver converted mordenite-polyacrylonitrile (AgZ-PAN) sorbent. Results from these experiments will be used for parameter selection guidelines to define test conditions for Kr gas capture purity evaluations later this year. The currently configured experimental test bed was modified by installing a new cooling apparatus to permit future multi-column testing with independent column temperature control. The modified test bed will allow for multi-column testing to facilitate a Xe separation followed by a Kr separation using engineered form sorbents. Selectivity experiments were run at temperatures of 295, 250 and 220 K. Two feed gas compositions of 1000 ppmv Xe, 150 ppmv Kr in either a He or an air balance were used. AgZ-PAN sorbent selectivity was calculated using Xe and Kr capacity determinations. AgZ-PAN sorbent selectivities for Xe over Kr of 72 were calculated at room temperature (295 K) using the feed gas with a He balance and 34 using the feed gas with an air balance. As the test temperatures were decreased the selectivity of Xe over Kr also decreased due to an increase in both Xe and Kr capacities. At 220 K, the sorbent selectivities for Xe over Kr were 22 using the feed gas with a He balance and 28 using the feed gas with an air balance. The selectivity results indicate that AgZ-PAN used in the first column of a multi-column configuration will provide adequate partitioning of Xe from Kr in the tested temperature range to produce a more pure Kr end product for collection.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Tropical Rainfall Measuring Mission (TRMM)

Recognizing the importance of rain in the tropics and the accompanying latent heat release, NASA for the U.S. and NASDA for Japan have partnered in the design, construction and flight of an Earth Probe satellite to measure tropical rainfall and calculate the associated heating. Primary mission goals are 1) the understanding of crucial links in climate variability by the hydrological cycle, 2) improvement in the large-scale models of weather and climate 3) improvement in understanding cloud ensembles and their impacts on larger scale circulations. The linkage with the tropical oceans and landmasses are also emphasized. The Tropical Rainfall Measuring Mission (TRMM) satellite was launched in November 1997 with fuel enough to obtain a four to five year data set of rainfall over the global tropics from 37 N to 37 S. This paper reports progress from launch date through the spring of 1999. The data system and its products and their access is described, as are the algorithms used to obtain the data. Some exciting early results from TRMM are described. Some important algorithm improvements are shown. These will be used in the first total data reprocessing, scheduled to be complete in early 2000. The reader is given information on how to access and use the data.

Simpson, Joanne↗

The Tropical Rainfall Measuring Mission (TRMM) Progress Report

Recognizing the importance of rain in the tropics and the accompanying latent heat release, NASA for the U.S. and NASDA for Japan have partnered in the design, construction and flight of an Earth Probe satellite to measure tropical rainfall and calculate the associated heating. Primary mission goals are 1) the understanding of crucial links in climate variability by the hydrological cycle, 2) improvement in the large-scale models of weather and climate 3) Improvement in understanding cloud ensembles and their impacts on larger scale circulations. The linkage with the tropical oceans and landmasses are also emphasized. The Tropical Rainfall Measuring Mission (TRMM) satellite was launched in November 1997 with fuel enough to obtain a four to five year data set of rainfall over the global tropics from 37'N to 37'S. This paper reports progress from launch date through the spring of 1999. The data system and its products and their access is described, as are the algorithms used to obtain the data. Some exciting early results from TRMM are described. Some important algorithm improvements are shown. These will be used in the first total data reprocessing, scheduled to be complete in early 2000. The reader is given information on how to access and use the data.

Simpson, Joanne↗

The Tropical Rainfall Measuring Mission (TRMM)

Recognizing the importance of rain in the tropics and the accompanying latent heat release, NASA for the U.S. and NASDA for Japan have partnered in the design, construction and flight of an Earth Probe satellite to measure tropical rainfall and calculate the associated heating. Primary mission goals are: 1) the understanding of crucial links in climate variability by the hydrological cycle, 2) improvement in the large-scale models of weather and climate, and 3) improvement in understanding cloud ensembles and their impacts on larger scale circulations. The linkage with the tropical oceans and landmasses are also emphasized. The Tropical Rainfall Measuring Mission (TRMM) satellite was launched in November 1997 with fuel enough to obtain a four to five year data set of rainfall over the global tropics from 37 deg N to 37 deg S. This paper reports progress from launch date through the spring of 1999. The data system and its products and their access is described, as are the algorithms used to obtain the data. Some exciting early results from TRMM are described. Some important algorithm improvements are shown. These will be used in the first total data reprocessing, scheduled to be complete in early 2000. The reader is given information on how to access and use the data.

Simpson, Joanne↗

Integration of Nuclear Material Accounting Data and Process Monitoring Data for Improvement on Detection Probability in Safeguarding Electrochemical Processing Facilities (Final Technical Report)

The KAERI advanced spent fuel conditioning process (ACP) process is a critical component of the US- South Korean nuclear cooperation and the following “123 Agreement.” Its development has received considerable attention in both countries. The ACP is an electrochemical processing (pyroprocessing) that recycles over 96% of the used nuclear fuel (UNF). It is also intrinsically proliferation-resistant in theory. In normal operation, the U/TRU product is very hot radiologically. In addition, the Cm provides a high level of spontaneous neutrons, making the product unsuitable for weapon use. However, as pointed in some study, “the need for safeguards to protect against the diversion and misuse of separated plutonium applies essentially equally to all grades of plutonium.” As pointed by many studies, the well-established traditional Nuclear Material Accounting (NMA) approach cannot be directly applied to electrochemical processing because of the lack of an input accountability tank, the non-continuous material flow, and the unsatisfactory level of confidence in sampling methods. Therefore, nuclear safeguards remain a grand challenge in the developing of commercial electrochemical separations facilities, especially around the heart of such facilities, the electrorefiner (ER) systems. In contrast to NMA data, process monitoring (PM) data is normally an indirect measurement of the SNM and is acquired much more frequently. In a broad sense, PM includes monitoring by various types of equipment, e.g. radiation detectors, cameras, voltage, current sensors. Because it is already being collected by the operator, the additional cost to safeguards is low. It has long been believed that PM data can supplement NMA data and help improve safeguards, although the benefits are hard to quantify. The U.S. DOE’s Material Protection, Accounting, and Control Technology (MPACT) campaign has made substantial investments into innovative PM sensor technology and predictive model development for real- or near real-time measurement and prediction of molten salt density and level, salt composition and actinide concentration especially Pu, the cell voltage, and the cell current to supplement traditional NMA. For aqueous-based reprocessing facilities, it is reported that PM, integrated with traditional NMA, have a high detection probability for specific diversions. For electrochemical reprocessing, preliminary studies have shown that PM data can support traditional NMA in various ways by providing a basis to estimate some of the in-processing nuclear material inventories. Despite early success, further studies on fusion of PM data and NMA data are still needed, which is the goal of this proposed work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Hydroxypyridinone-based stabilization of Np(IV) enabling efficient U/Np/Pu separations in the Adapted PUREX process

The classical process to recover uranium (U) and plutonium (Pu) from used nuclear fuel using tributyl phosphate (TBP), namely the Plutonium Uranium Redox EXtraction (PUREX) process, is complicated by the persistent presence of neptunium (Np) and thus requires extra purification steps. The concept of Adapted PUREX seeks to achieve Np recovery by adjusting the valence of the metal more effectively, thereby controlling its behavior more precisely. This study introduces the use of an aqueous hydroxypyridinone chelator, 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO), to dictate the behavior of Np for recovery and meanwhile simplify cumbersome reprocessing steps. The interactions between Np and HOPO were probed mechanistically by way of absorption spectrophotometry, in conjunction with cyclic voltammetry. UV–Vis-NIR spectra illustrated the reduction of NpO 2 2+ to Np 4+ , with a fast reaction rate. Cyclic voltammetry revealed quasi-reversible processes between the oxidized and reduced forms of the ligand and its Np complexes. The corresponding heterogeneous rate constants (k 0 ) were estimated from the peak-to-peak separation potentials (ΔE p ), at ~ 4 – 35 μm/s for both HOPO and NpHOPO, with scan rates of 0.01 – 0.4 V/s. Meanwhile, the electromotive force (E MF ) as well as the change of Gibbs free energy (ΔG) were assessed from the half-wave potential (E 1/2 ), demonstrating the completeness of NpO 2 2+ reduction to Np 4+ by HOPO. The cumulative formation constant of the resulting NpHOPO complex (logβ 101 ) was determined by metal competition titration to be 42.0 ± 0.6, corroborating the extraordinarily high affinity of HOPO to tetravalent metal ions. Here, the prowess of valence control by HOPO and the high stability of the formed complex resulted in enhanced separations of Np from U and of Pu from U, with a maximum separation factor of ~7000 for both, nearly 90- and 10300-fold higher, respectively, than the values obtained using conventional PUREX formulae.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Remediation of uranium in-situ leaching area at Straz Pod Ralskem, Czech Republic

A large-scale development in exploration and production of uranium ores in the Czech Republic was done in the 2nd half of the 20. century. Many uranium deposits were discovered in the territory of the Czech Republic. One of the most considerable deposits in the Czech Republic is the site Hamr na Jezere - Straz pod Ralskem where both mining methods - the underground mining and the acidic in-situ leaching - were used. The extensive production of uranium led to widespread environmental impacts and contamination of ground waters. Over the period of 'chemical' leaching of uranium (ca. 32 years), a total of more than 4 million tons of sulphuric acid and other chemicals have been injected into the ground. Most of the products (approx. 99.5 %) of the acids reactions with the rocks are located in the Cenomanian aquifer. The contamination of Cenomanian aquifer covers the area larger then 27 km{sup 2}. The influenced volume of groundwater is more than 380 million m{sup 3}. The total amount of dissolved SO{sub 4}{sup 2-} is about 3.6 million tons. After 1990 a large-scale environmental program was established and the Czech government decided to liquidate the ISL Mine and start the remediation in 1996. The remediation consists of contaminated groundwater pumping, removing of the contaminants and discharging or reinjection of treated water. Nowadays four main remedial technological installations with sufficient capacity for reaching of the target values of remedial parameters in 2037 are used - the 'Station for Acid Solutions Liquidation No. One', the 'Mother liquor reprocessing' station, the 'Neutralization and Decontamination Station NDS 6' and the 'Neutralization and Decontamination Station NDS 10'. It is expected that the amount of withdrawn contaminants will vary from 80 000 to 120 000 tons per year. Total costs of all remediation activities are expected to be in excess of 2 billion EUR. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Collaborative working is driving progress in hazard and risk reduction delivery at Sellafield - 16387

A new way of working has been adopted at the Sellafield site in the United Kingdom which is delivering benefits in terms of accelerating hazard and risk reduction safely and securely at the site. This new way of working involves a collaborative approach on crucial aspects of the plan of work for Sellafield between: - Sellafield Ltd (the site's management and operations contractor), - The Nuclear Decommissioning Authority (the site's owner and Sellafield Ltd's customer), - The Office for Nuclear Regulation (the UK's nuclear safety and security regulator), - The Environment Agency (England's environmental regulator), - The UK Government's Department of Energy and Climate Change, - The UK Government's Shareholder Executive, part of the Department of Business, Innovation and Skills. The new way of working is founded upon fully aligning the individual strategies of each of these six organisations towards the common goal of accelerated risk and hazard reduction and then ensuring good communications so these strategies remain fully aligned. To this end a number of issues were identified by the six organisations which were considered to be slowing the progress of the risk and hazard reduction work, from which a set of 'strategic themes' was developed to facilitate different ways of thinking and so solve these issues. The strategic themes are: - Looking for blockers and how they can be removed, - Avoiding overly complex solutions by utilising the concept of fit for purpose, - The effective use of resources, - Prioritisation arrangements, - Incentivisation, - The appetite for risk, - Avoiding distractions and diversions, - Effective use of communications so that the more effective and efficient ways of working, and the improvements that are generated, are promulgated throughout Sellafield Ltd. These strategic themes have been applied with great effect in a number of areas delivering risk reduction benefits. For example: - The removal of ageing fuel from Sellafield's oldest pond, the Pile Fuel Storage Pond; a significant milestone in the site's hazard and risk reduction agenda. - Implementing an alternative ILW approach. - Managing stocks of Highly Active Liquor (HAL). - 'Re-purposing' existing Waste Management Facilities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Periodic Accretion-powered Flares from Colliding EMRIs as TDE Imposters

When a main-sequence star undergoes Roche lobe overflow onto a supermassive black hole (SMBH) in a circular extreme mass ratio inspiral (EMRI), a phase of steady mass transfer ensues. Over millions of years, the binary evolves to a period minimum before reversing course and migrating outward as a brown dwarf. Because the time interval between consecutive EMRIs is comparable to the mass-transfer timescale, the semimajor axes of two consecutive mass-transferring EMRIs will cross on a radial scale of less than a few au. We show that such EMRI crossing events are inevitably accompanied by a series of mildly relativistic, grazing physical collisions between the stars. Each collision strips a small quantity of mass, primarily from the more massive star, which generally increases their radial separation to set up the next collision after a delay of decades to centuries (or longer) set by further gravitational radiation. Depending on the mass of the SMBH, this interaction can result in N{sub c}∼1--10{sup 4} gas production events of mass ∼M{sub ⊙}/N{sub c}, thus powering a quasi-periodic sequence of SMBH accretion-powered flares over a total duration of thousands of years or longer. Although the EMRI rate is 2–3 orders of magnitude lower than the rate of tidal disruption events (TDEs), the ability of a single interacting EMRI pair to produce a large number of luminous flares—and to make more judicious use of the available stellar fuel—could make their observed rate competitive with the TDE rate, enabling them to masquerade as “TDE imposters.” Gas produced by EMRI collisions is easier to circularize than the highly eccentric debris streams produced in TDEs. We predict flares with bolometric luminosities that decay both as power laws shallower than t{sup −5/3} and as decaying exponentials in time. Viscous spreading of the gaseous disks produced by the accumulation of previous mass-stripping events will place a substantial mass of gas on radial scales ≳10--100 au at the time of a given flare, providing a possible explanation for the “reprocessing blanket” required to explain the unexpectedly high optical luminosities of some candidate TDE flares.

79 ASTRONOMY AND ASTROPHYSICS↗

Quantify Water Extraction by TBP/Dodecane via Molecular Dynamics Simulations

The purpose of this project is to quantify the interfacial transport of water into the most prevalent nuclear reprocessing solvent extractant mixture, namely tri-butyl- phosphate (TBP) and dodecane, via massively parallel molecular dynamics simulations on the most powerful machines available for open research. Specifically, we will accomplish this objective by evolving the water/TBP/dodecane system up to 1 ms elapsed time, and validate the simulation results by direct comparison with experimentally measured water solubility in the organic phase. The significance of this effort is to demonstrate for the first time that the combination of emerging simulation tools and state-of-the-art supercomputers can provide quantitative information on par to experimental measurements for solvent extraction systems of relevance to the nuclear fuel cycle. Results: Initially, the isolated single component, and single phase systems were studied followed by the two-phase, multicomponent counterpart. Specifically, the systems we studied were: pure TBP; pure n-dodecane; TBP/n-dodecane mixture; and the complete extraction system: water-TBP/n-dodecane two phase system to gain deep insight into the water extraction process. We have completely achieved our goal of simulating the molecular extraction of water molecules into the TBP/n-dodecane mixture up to the saturation point, and obtained favorable comparison with experimental data. Many insights into fundamental molecular level processes and physics were obtained from the process. Most importantly, we found that the dipole moment of the extracting agent is crucially important in affecting the interface roughness and the extraction rate of water molecules into the organic phase. In addition, we have identified shortcomings in the existing OPLS-AA force field potential for long-chain alkanes. The significance of this force field is that it is supposed to be optimized for molecular liquid simulations. We found that it failed for dodecane and/or longer chains for this particular solvent extraction application. We have proposed a simple way to circumvent the artificial crystallization of the chains at ambient temperature.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A NICER Thermonuclear Burst from the Millisecond X-Ray Pulsar SAX J1808.4–3658

The Neutron Star Interior Composition Explorer (NICER) has extensively monitored the 2019 August outburst of the 401 Hz millisecond X-ray pulsar SAX J1808.4–3658. In this Letter, we report on the detection of a bright helium-fueled Type I X-ray burst. With a bolometric peak flux of (2.3 ± 0.1) × 10(exp −7) erg/s sq.cm, this was the brightest X-ray burst among all bursting sources observed with NICER to date. The burst shows a remarkable two-stage evolution in flux, emission lines at 1.0 and 6.7 keV, and burst oscillations at the known pulsar spin frequency, with ≈4% fractional sinusoidal amplitude. We interpret the burst flux evolution as the detection of the local Eddington limits associated with the hydrogen and helium layers of the neutron star envelope. The emission lines are likely associated with Fe, due to reprocessing of the burst emission in the accretion disk.

Bult, Peter↗

Development of evaluation models of manpower needs for dismantling the dry conversion process-related equipment in uranium refining and conversion plant (URCP)

Evaluation models for determining the manpower needs for dismantling various types of equipment in uranium refining and conversion plant (URCP) have been developed. The models are widely applicable to other uranium handling facilities. Additionally, a simplified model was developed for easily and accurately calculating the manpower needs for dismantling dry conversion process-related equipment (DP equipment). It is important to evaluate beforehand project management data such as manpower needs to prepare an optimized decommissioning plan and implement effective dismantling activity. The Japan Atomic Energy Agency (JAEA) has developed the project management data evaluation system for dismantling activities (PRODIA code), which can generate project management data using evaluation models. For preparing an optimized decommissioning plan, these evaluation models should be established based on the type of nuclear facility and actual dismantling data. In URCP, the dry conversion process of reprocessed uranium and others was operated until 1999, and the equipment related to the main process was dismantled from 2008 to 2011. Actual data such as manpower for dismantling were collected during the dismantling activities, and evaluation models were developed using the collected actual data on the basis of equipment classification considering the characteristics of uranium handling facility. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Artificial Neural Network Test Support Development for the Space Shuttle PRCS Thrusters

A significant anomaly, Fuel Valve Pilot Seal Extrusion, is affecting the Shuttle Primary Reaction Control System (PRCS) Thrusters, and has caused 79 to fail. To help address this problem, a Shuttle PRCS Thruster Process Evaluation Team (TPET) was formed. The White Sands Test Facility (WSTF) and Boeing members of the TPET have identified many discrete valve current trace characteristics that are predictive of the problem. However, these are difficult and time consuming to identify and trend by manual analysis. Based on this exhaustive analysis over months, 22 thrusters previously delivered by the Depot were identified as high risk for flight failures. Although these had only recently been installed, they had to be removed from Shuttles OV103 and OV104 for reprocessing, by directive of the Shuttle Project Office. The resulting impact of the thruster removal, replacement, and valve replacement was significant (months of work and hundreds of thousands of dollars). Much of this could have been saved had the proposed Neural Network (NN) tool described in this paper been in place. In addition to the significant benefits to the Shuttle indicated above, the development and implementation of this type of testing will be the genesis for potential Quality improvements across many areas of WSTF test data analysis and will be shared with other NASA centers. Future tests can be designed to incorporate engineering experience via Artificial Neural Nets (ANN) into depot level acceptance of hardware. Additionally, results were shared with a NASA Engineering and Safety Center (NESC) Super Problem Response Team (SPRT). There was extensive interest voiced among many different personnel from several centers. There are potential spin-offs of this effort that can be directly applied to other data acquisition systems as well as vehicle health management for current and future flight vehicles.

Lehr, Mark E.↗

Simultaneous quantification of uranium( VI ), samarium, nitric acid, and temperature with combined ensemble learning, laser fluorescence, and Raman scattering for real-time monitoring

In this work, laser-induced fluorescence spectroscopy (LIFS), Raman spectroscopy, and a stacked regression ensemble was developed for near real-time quantification of uranium(VI) (1–100 μg mL –1 ), samarium (0–200 μg mL –1 ) and nitric acid (0.1–4 M) with varying temperature (20 °C–45 °C). LIFS applications range from fundamental lab-scale studies to real-time process monitoring at industrial levels, such as nuclear reprocessing applications, provided the phenomena affecting the fluorescence spectrum are accounted for (e.g., absorption, quenching, complexation). Multiple chemometric models were examined and compared to a more traditional multivariate regression approach called partial least squares (PLS). Results obtained on synthetic samples selected using D-optimal experimental design indicated that a stacked regression method, which included ridge regression, random forest, PLS, and an eXtreme gradient boost algorithm, successfully measured uranium(VI) concentrations directly in nitric acid without measuring luminescence lifetimes or standard addition. The top model resulted in percent root-mean-square error of prediction values of 5.2, 1.9, 3.0, and 2.3% for U(VI), Sm 3+ , HNO 3 , and temperature, respectively. The approach may be useful for quantifying fluorescent fission products (e.g., Sm 3+ ) to provide information on burnup of irradiated nuclear fuel. This novel framework reinforces the applicability of LIFS for real-time applications in nuclear fuel cycle applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Highly Recyclable Thermosets for Lightweight Composites: CRADA 517 [Abstract only]

Lightweight composites are of increasing need to enable reduced fuel usage, reduced carbon emissions and increased range in air and ground transportation. The superior weight savings of carbon fiber thermoset composites are impeded by material and production costs and the limited options available for composite repair and recycle. The materials recovery and recycling sector is currently overwhelmed by an abundance of low-value materials and limited market opportunities for downcycled content, rendering landfilling a more attractive alternative. Vitrimers represent a new paradigm for repairable and recyclable thermosets, but this relatively new technology will require development, including government investment, to reduce risks for its adoption by aerospace and automotive OEMs. The overall goal of the project is to create recyclable carbon fiber composites using vitrimer resins that are more energy efficient to produce and have improved properties over baseline technology. The targeted composites will retain their tensile strength after multiple recycling and reprocessing steps. In addition, monomer will be recoverable through depolymerization and re-usable carbon fibers will be retrieved.

36 MATERIALS SCIENCE↗

Justification to Disregard U-234 Mass in Certain Uranium Systems

The ANSI/ANS-8.1-1998 Standard regarding nuclear criticality safety in operations with fissionable material outside reactors states certain guidelines for dealing with uranium isotopes when setting mass limits. In ANSI/ANS-8.1-1998 235 U limits apply to mixtures “with 234 U, 236 U, or 238 U, provided that 234 U is considered to be 235U” in computing mass. In this evaluation calculations coupled with benchmark data show a superior way of handling the other common uranium isotopes when setting limits for 235 U. Currently 234 U mass must be considered as 235 U mass in order to account for the fact 234 U has a k ∞ = 1.70 meaning criticality can be reached with a finite amount of 234 U mass. 236 U and 238 U have k ∞ ’s equal to 0.71 and 0.31 meaning they remain subcritical in infinite amounts and thus no mass limits are required. In fresh uranium (un-irradiated or reprocessed) enriched to 94% 235 U by weight, bounding ratios of 234 U, 236U, and 238U exist due to the enrichment process. Utilizing these ratios it is shown that 234 U accounts for less than 0.20 of the total mass fraction of 234 U, 236 U, and 238 U and the remaining 0.80 mass fraction is in a ratio of at least 1:1 for 238 U: 236 U. Creating models conservatively based on these two material limits, the resulting k ∞ = 0.91367 ± 0.00208 suggests a mass limit for 234 U is no longer required.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗