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At least 163 records · Page 9

Decay Heat Calculations for PWR and BWR Assemblies Fueled with Uranium and Plutonium Mixed Oxide Fuel using SCALE

In currently operating commercial nuclear power plants (NPP), there are two main types of nuclear fuel, low enriched uranium (LEU) fuel, and mixed-oxide uranium-plutonium (MOX) fuel. The LEU fuel is made of pure uranium dioxide (UO{sub 2} or UOX) and has been the fuel of choice in commercial light water reactors (LWRs) for a number of years. Naturally occurring uranium contains a mixture of different uranium isotopes, primarily, {sup 235}U and {sup 238}U. {sup 235}U is a fissile isotope, and will readily undergo a fission reaction upon interaction with a thermal neutron. {sup 235}U has an isotopic concentration of 0.71% in naturally occurring uranium. For most reactors to maintain a fission chain reaction, the natural isotopic concentration of {sup 235}U must be increased (enriched) to a level greater than 0.71%. Modern nuclear reactor fuel assemblies contain a number of fuel pins potentially having different {sup 235}U enrichments varying from {approx}2.0% to {approx}5% enriched in {sup 235}U. Currently in the United States (US), all commercial nuclear power plants use UO{sub 2} fuel. In the rest of the world, UO{sub 2} fuel is still commonly used, but MOX fuel is also used in a number of reactors. MOX fuel contains a mixture of both UO{sub 2} and PuO{sub 2}. Because the plutonium provides the fissile content of the fuel, the uranium used in MOX is either natural or depleted uranium. PuO{sub 2} is added to effectively replace the fissile content of {sup 235}U so that the level of fissile content is sufficiently high to maintain the chain reaction in an LWR. Both reactor-grade and weapons-grade plutonium contains a number of fissile and non-fissile plutonium isotopes, with the fraction of fissile and non-fissile plutonium isotopes being dependent on the source of the plutonium. While only RG plutonium is currently used in MOX, there is the possibility that WG plutonium from dismantled weapons will be used to make MOX for use in US reactors. Reactor-grade plutonium in MOX fuel is generally obtained from reprocessed irradiated nuclear fuel, whereas weapons-grade plutonium is obtained from decommissioned nuclear weapons material and thus has a different plutonium (and other actinides) concentration. Using MOX fuel instead of UOX fuel has potential impacts on the neutronic performance of the nuclear fuel and the design of the nuclear fuel must take these differences into account. Each of the plutonium sources (RG and WG) has different implications on the neutronic behavior of the fuel because each contains a different blend of plutonium nuclides. The amount of heat and the number of neutrons produced from fission of plutonium nuclides is different from fission of {sup 235}U. These differences in UOX and MOX do not end at discharge of the fuel from the reactor core - the short- and long-term storage of MOX fuel may have different requirements than UOX fuel because of the different discharged fuel decay heat characteristics. The research documented in this report compares MOX and UOX fuel during storage and disposal of the fuel by comparing decay heat rates for typical pressurized water reactor (PWR) and boiling water reactor (BWR) fuel assemblies with and without weapons-grade (WG) and reactor-grade (RG) MOX fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Verification of Special Nuclear Material (SNM) using Active Well Coincidence Counter (AWCC) and a High Purity Germanium (HPGe) Detector

SNM verification can be accomplished via two methods i.e. destructive analysis (DA) or nondestructive analysis (NDA). The DA modes are much more accurate compared to NDA modes; nevertheless, the sample's physical integrity is destroyed in the process. Techniques such as ICP-MS, ID-ICP-MS, TI-MS are few examples of DA, where a bulk material is ground and mixed with a solution (some form of acid) to acquire a homogenous sample. In contrast, NDA modes utilize signals emitted by the sample such as gamma, neutrons, light, or heat to analyze samples under investigation. HPGe detectors are some of the most frequently used gamma detectors to assay SNM. However, in a high activity scenario it provides a large uncertainty and sometimes becomes unfeasible to measure low energy gamma rays. Meanwhile, neutron detectors are not affected by the gamma background, therefore they can be used in addition to the gamma detectors to verify total fissile mass ({sup 235}U + {sup 239}Pu) of SNM. The AWCC is one of the thermal neutron NDA systems developed at the Los Alamos National Laboratory (LANL). It consists of 42 {sup 3}He detectors to measure gross neutrons (singles), coincidence neutrons (doubles), higher order multiplicity counting (triples, quadruples, etc.). It can effectively operate in both active and passive neutron interrogation modes. It can utilize AmLi, AmBe, or {sup 252}Cf active interrogation neutron sources. It is used to verify declared fissile mass ({sup 235}U or {sup 239}Pu) present in SNM. Objectives: Calibrate HPGe and AWCC for lightly irradiated (with enough {sup 137}Cs gamma background) ∼93% enriched HEU fuels; Verify fissile mass ({sup 235}U +{sup 239}Pu) content using AWCC and HPGe; Model and benchmark AWCC in MCNP6. Neutron coincidence and multiplicity counting: Two or more neutrons are coincident if they are detected by the system within the specified gate window; In AWCC: Gate window is 128 μsec; Induced fission in fissile material such as {sup 235}U and {sup 239}Pu - emission of time correlated neutrons - Singles, Doubles, Triples, or Quadruples; No induced fission in non-fissile materials- no correlated neutrons - only singles. SNM can be verified with high accuracy and precision using gamma and neutron NDA instruments such as HPGe and AWCC. Interaction with thermal neutrons. Non-fissile atoms - do not emit correlated neutrons. Fissile atoms - emit correlated neutrons during induced fission events. The time correlated neutrons can be detected by using coincidence or multiplicity counters such as AWCC. Likewise, {sup 235}U produces 186 keV gamma peak that can be measured by a HPGe gamma detector. Counts under 186 keV gamma peak provide information about {sup 235}U content. Combining AWCC and HPGe results can provide better understanding of special nuclear material under investigation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Limiting Surface Density Method Adapted to Large Arrays of Heterogeneous Shipping Packages with Nonlinear Responses

The classic Limiting Surface Density (LSD) method is an empirical calculation technique for analyzing and setting mass limits for fissile items in storage arrays. LSD is a desirable method because it can reduce or eliminate the need for lengthy detailed Monte Carlo models of storage arrays. The original (or classic) method was developed based on idealized arrays of bare spherical metal items in air-spaced cubic units in a water-reflected cubic array. In this case, the geometric and material-based surface densities were acceptably correlated by linear functions. Later updates to the method were made to allow for concrete reflection rather than water, cylindrical masses rather than spheres, different material forms, and noncubic arrays. However, in the intervening four decades since those updates, little work has been done to update the method, especially for use with contemporary highly heterogeneous shipping packages that are noncubic and stored in noncubic arrays. In this work, the LSD method is reevaluated for application to highly heterogeneous shipping packages for fissile material. The package modeled is the 9975 shipping package, currently the primary package used to store fissile material at Savannah River Site’s K-Area Complex. The package is neither cubic nor rectangular but resembles nested cylinders of stainless steel, lead, aluminum, and Celotex. The fissile content is assumed to be a cylinder of plutonium metal. The packages may be arranged in arrays with both an equal number of packages per side (package cubic) and an unequal number of packages per side (noncubic). The cubic arrangements are used to derive the 9975-specific material and geometry constants for the classic linear form LSD method. The linear form of the LSD, with noncubic array adjustment, is applied and evaluated against computational models for these packages to determine the critical unit fissile mass. Sensitivity equations are derived from the classic method, and these are also used to make projections of the critical unit fissile mass. It was discovered that the heterogeneous packages have a nonlinear surface density versus critical mass relationship compared to the acceptably linear response of bare spherical fissile masses. Methodology is developed to address the nonlinear response. In so doing, the solution to the nonlinear LSD method becomes decoupled from the critical mass of a single unit, adding to its flexibility. The ability of the method to predict changes in neutron multiplication due to perturbations in a parameter is examined to provide a basis for analyzing upset conditions. In conclusion, a full rederivation of the classic LSD method from diffusion theory is also included as this was found to be lacking in the available literature.

42 ENGINEERING↗

DN/DG Screening of Environmental Swipe Samples: FY2016 Report

The Delayed Neutron Delayed Gamma (DNDG) technique provides a new analytical capability to the International Atomic Energy Agency (IAEA) for detecting undeclared nuclear activities. IAEA’s Long Term R&D (LTRD) plan has a stated high urgency need to develop elemental and isotopic signatures of nuclear fuel cycle activities and processes (LTRD 2.2). The new DNDG capability is used to co-detect both uranium and plutonium as an extension of a DN only method that is already being utilized by the IAEA for the analysis of swipes to inform on undeclared nuclear activities. Analytical method involving irradiation of swipe samples potentially containing trace quantities of fissile material in a thermal neutron field, followed by the counting of delayed neutrons, is a well-known technique in the field of safeguards and nonproliferation. It is used for detecting the presence of microscopic amounts of fissile material, (typically a linear combination of 233 U, 235 U, 239 Pu, and 241 Pu)and quantifying it in terms of the equivalent mass of 235U. The delayed neutron (DN) technique is very sensitive and is been routinely employed at the High Flux Isotope Reactor (HFIR) facility at Oak Ridge National Laboratory (ORNL). Both uranium and plutonium are of high safeguards value. However, the DN technique is not well suited for distinguishing between U and Pu isotopes since the decay curves overlap closely. The delayed gamma (DG) technique will help detect the presence of 239Pu in a mixture of U and Pu. Thus the DNDG approach combines the best of both worlds; the sensitivity of DN counting and the isotopic specificity of DG counting. The present work seeks to build on the delayed neutron and delayed gamma methods that have been developed at ORNL. It is recognized that the distribution profile of heavy fission products remains fairly invariant for the fissile nuclides whereas the distribution of light fission products varies from one isotope to another. That is, the ratio of the yield of a light fission fragment to a heavy fission fragments is isotope specific. Measurement of the ratio of the net full energy peak (FEP) from low/high mass fission products is an elegant way to characterize the fraction of fissile materials present in a mixture. By empirically calibrating the ratio of the net FEP as a function of known concentration of the binary mixture, one can determine the fraction of fissile isotopes in an unknown sample. In the work done in fiscal year (FY) 2016, samples of single fissile material isotopes as well as binary mixtures were irradiated in a well thermalized irradiation field in the HFIR. Delayed neutron counting was performed using the neutron counter at the HFIR Neutron Activation Analysis (NAA) laboratory. Delayed gamma counting was performed using a shielded high purity germanium (HPGe) detector. Delayed neutron decay curve results highlighted the difficulty of distinguishing between U and Pu isotopes, and the need for including the delayed gamma component. Based on delayed gamma spectrometry, twelve ratios of low mass/high fission product gamma ray FEP have been identified as valid candidates. Linearity of the ratios, as a function of 239 Pu fraction in 235 U+ 239 Pu mixtures, was confirmed for the low mass/high mass candidates that were selected. The DNDG method we are spearheading allows not only the presence of total fissile content to be detected, but whether the material is predominantly U or predominantly Pu, or a mixture. This provides additional SG relevant information.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Use of Thorium within the Nuclear Power Industry - 13472

Thorium is 3 to 4 times more abundant than uranium and is widely distributed in nature as an easily exploitable resource in many countries. Unlike natural uranium, which contains ∼0.7% fissile {sup 235}U isotope, natural thorium does not contain any fissile material and is made up of the fertile {sup 232}Th isotope only. Therefore thorium and thorium-based fuel as metal, oxide or carbide, has been utilized in combination with fissile {sup 235}U or {sup 239}Pu in nuclear research and power reactors for conversion to fissile {sup 233}U, thereby enlarging fissile material resources. During the pioneering years of nuclear energy, from the mid 1950's to mid 1970's, there was considerable interest worldwide to develop thorium fuels and fuel cycles in order to supplement uranium reserves. Thorium fuels and fuel cycles are particularly relevant to countries having large thorium deposits but very limited uranium reserves for their long term nuclear power programme. The feasibility of thorium utilization in high temperature gas cooled reactors (HTGR), light water reactors (LWR), pressurized heavy water reactors (PHWRs), liquid metal cooled fast breeder reactors (LMFBR) and molten salt breeder reactors (MSBR) were demonstrated. The initial enthusiasm for thorium fuels and fuel cycles was not sustained among the developing countries later, due to new discovery of uranium deposits and their improved availability. However, in recent times, the need for proliferation-resistance, longer fuel cycles, higher burnup, and improved waste form characteristics, reduction of plutonium inventories and in situ use of bred-in fissile material has led to renewed interest in thorium-based fuels and fuel cycles. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Preliminary Neutronics Design and Analysis of D 2 O Cooled High Conversion PWRs

This report presents a neutronics analysis of tight-pitch D 2 O-cooled PWRs loaded with MOX fuel and focuses essentially on the Pu breeding potential of such reactors as well as on an important safety parameter, the void coefficient, which has to be negative. It is well known that fast reactors have a better neutron economy and are better suited than thermal reactors to breed fissile material from neutron capture in fertile material. Such fast reactors (e.g. sodium-cooled reactors) usually rely on technologies that are very different from those of existing water-cooled reactors and are probably more expensive. This report investigates another possibility to obtain a fast neutron reactor while still relying mostly on a PWR technology by: (1) Tightening the lattice pitch to reduce the water-to-fuel volume ratio compared to that of a standard PWR. Water-to-fuel volume ratios of between 0.45 and 1 have been considered in this study while a value of about 2 is typical of standard PWRs, (2) Using D 2 O instead of H 2 O as a coolant. Indeed, because of its different neutron physics properties, the use of D 2 O hardens the neutron spectrum to an extent impossible with H 2 O when used in a tight-pitch lattice. The neutron spectra thus obtained are not as fast as those in sodium-cooled reactor but they can still be characterized as fast compared to that of standard PWR neutron spectra. In the phase space investigated in this study we did not find any configurations that would have, at the same time, a positive Pu mass balance (more Pu at the end than at the beginning of the irradiation) and a negative void coefficient. At this stage, the use of radial blankets has only been briefly addressed whereas the impact of axial blankets has been well defined. For example, with a D 2 O-to-fuel volume ratio of 0.45 and a core driver height of about 60 cm, the fissile Pu mass balance between the fresh fuel and the irradiated fuel (50 GWd/t) would be about -7.5% (i.e. there are 7.5% fewer fissile Pu isotopes at the end than at the beginning of the irradiation) and the void coefficient would be negative. The addition of 1 cm of U-238 blanket at the top and bottom of the fuel would bring the fissile Pu mass balance from -7.5% to -6.5% but would also impact the void coefficient in the wrong way. In fact, it turns out that the void coefficient is so sensitive to the presence of axial blanket that it limits its size to only a few cm for driver fuel height of about 50-60 cm. For reference, the fissile Pu mass balance is about -35% in a standard PWR MOX fuel such as those used in France. In order to reduce the fissile Pu deficit and potentially reach a true breeding regime (i.e. a positive Pu mass balance), it would be necessary to make extensive use of radial blankets, both internal and external. Even though this was not addressed in detail here, it is reasonable to believe that at least as much U-238 blanket subassemblies as MOX driver fuel subassemblies would be necessary to breed enough Pu to compensate for the Pu deficit in the driver fuel. Hence, whereas a relatively simple D 2 O-cooled PWR core design makes it possible to obtain a near-breeder core, it may be necessary to more than double the mass of heavy metal in the core as well as the mass of heavy metal to reprocess per unit of energy produced in order to breed the few percents of Pu missing to reach a true breeding regime. It may be interesting to quantify these aspects further in the future.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Direct Measurement of U235 and Pu239 in Spent Fuel Rods with Gamma-Ray Mirrors

The amounts of fissile Pu and U in spent nuclear fuel are of primary concern to the safeguards community. In particular, there are issues when safeguards transitions from an item accountancy basis (such as fuel bundles) to a fissile material mass basis as occurs when spent fuel enters a reprocessing plant. Discrepancies occur because item accountancy requires estimating the content of fissile material using indirect techniques such as the fuel burn-up and item-level measurements of radiation emissions from fission by-products. Direct measurement of the fissile content by monitoring line emissions from fissile species themselves is impossible because the lines are much weaker than those emitted by shorter-lived isotopes in the fuel. The goal of this project is to develop a technique to directly measure these weaker lines despite the presence of overwhelming radiation from other isotopes. This is achieved by using gamma-ray mirrors as a narrow band-pass filter. The mirrors reflect only energies of interest toward a HPGe detector that is shielded from direct view of the spent fuel and its fierce emissions. This can significantly improve the reliability with which the mass of fissile material is tracked.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nuclear Criticality Safety Assessment of Criticality Control Containers without Moderation Control at the Waste Isolation Pilot Plant

The Waste Isolation Pilot Plant (WIPP) provides for safe, permanent disposal of government-owned transuranic (TRU) and TRU mixed wastes. Receipt and disposal of waste at the WIPP site began in March 1999. The Sandia report, Consideration of Nuclear Criticality When Disposing of Transuranic Waste at the Waste Isolation Pilot Plant, addressed potential nuclear criticality safety issues based on the projected inventory characteristics known at the time [1]. As designs for inventory, waste forms, and disposal packages have changed, new analyses have been performed, and updates have been made to address any potential effects to the WIPP safety basis. New analyses performed include Saylor 2017 [2] and Brickner 2019 [3], which address certain waste containers with specified loadings under post-closure conditions. Both examined several hypothetical scenarios and included analyses to bound (from a criticality potential standpoint) credible configurations that could occur at WIPP during the repository regulatory post-closure disposal time period for feature, event, and process (FEP) considerations—10,000 years. During this post-closure period at WIPP, the screening of FEPs is governed by the risk-based standards and implementing regulations of the US Environmental Protection Agency (EPA) (i.e., 40 CFR 191 and 40 CFR 194, respectively) [4,5]. An FEP screening can be based on either a low-consequence or low-probability rationale. A low-probability rationale includes either (a) a qualitative rationale that the FEP is not credible or (b) a quantitative demonstration that the probability is less than 10-4 in 104 years. In this evaluation, a qualitative lowprobability rationale of not credible is used by demonstrating that bounding configurations of the waste are not critical. The demonstration of subcriticality is through quantitative calculations, but a probability of criticality is not evaluated. Rather, the rationale for this evaluation is that bounding configurations with an effective neutron multiplication factor (keff) well below the upper subcriticality limit (USL) make criticality incredible. Reference [2] documented a nuclear criticality assessment of the WIPP repository for disposal of dilute surplus plutonium materials using the Dilute and Dispose Approach and packaging in criticality control overpacks (CCOs). The CCO is the waste disposal container recently designed to allow for up to 380 fissile gram equivalent (FGE) 239 Pu per drum, which is a higher fissile loading than typical waste containers. The CCO consists of a criticality control container (CCC) positioned by upper and lower plywood spacers within a standard 55 gal drum. The CCC is used to establish a geometry control for fissile materials during transportation and WIPP emplacement operations. The current WIPP waste acceptance criteria for CCO payloads limit beryllium to less than or equal to 1% by weight of the waste contents and require the waste form to be non-machine compacted. Reference [2] considered two scenario progressions—room closure from salt creep, hereafter referred to as the reconfigured dry scenario, and flooding with brine, hereafter referred to as the reconfigured wet scenario. The subsequent drying out of the reconfigured wet scenarios was also considered. For all scenarios, subcriticality was maintained when 50 g of B 4 C (acting as a neutron absorber) per CCC was intermixed within the plutonium disposition waste form. The analysis used a waste form description that limits the amount of moderation that could be present within the waste form (i.e., it limits the amount of water and polyethylene that could be present based on planned processing conditions). This analysis to evaluate increased limits on the amount of moderation that could be present was performed as a companion to Reference [2] to address concerns associated with verifying moisture and/or plastic contents of waste materials following packaging of dilute surplus plutonium in the CCO. To that end, this analysis used the models and methods from Reference [2] to evaluate a more generic base waste form consisting of water and polyethylene that is more similar (and nearly identical) to the generic waste forms utilized in other models/analyses supporting the TRU Package Transporter Model II (TRUPACTII) safety analysis [6] (all are without moderation controls). The waste form in this analysis uses a base mixture of 75% water and 25% polyethylene, the total amount of which is varied to determine the optimum moderation to fissile material (H/Pu) ratio. The fissile loading is maintained at up to 380 FGE 239 Pu (modeled as PuO 2 ) per CCO with an additional 545 g of beryllium (to bound the 1% by weight contents restriction) and 50 g of B 4 C intermixed per CCO. The beryllium content (1% by weight) is based on the total allowed waste weight (this does not include packaging and container weights). Figures ES-1 and ES-2 display summary results, showing that with this model including 50 g of B 4 C per CCO, the system keff remains under 0.85 for all moderator amounts and provides a significant margin against post-closure criticality under postulated bounding conditions for compaction. Figure ES-1 compares an infinite model with a room model at the initial emplacement spacing and under full radial compaction. Full radial compaction places each CCC in direct contact and does not credit any anticipated spacing associated with current post-closure geomechanical modeling of the repository [7]. The effects of variations in the H/Pu ratio were evaluated by varying the amount of the water/polyethylene component of the waste model, with fissile loading maintained at 380 239 Pu FGE. Similarly, Figure ES-2 illustrates how various amounts of B 4 C per CCO influence k eff at different radial compactions, all at the H/Pu ratio of 200 (in the room array model). Therefore, while the results from Saylor 2017 [2] modeled more realistic process limits associated with packaging of dilute surplus plutonium, this analysis demonstrates that limits on moderation (plastic and water content) are not necessary to ensure subcriticality in the WIPP repository, provided the requisite B 4 C absorber is present.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characteristics of TRU Fueled SFR Core during the Transition with Partially Loaded LEU Assemblies

The fast reactor (FR) fuels typically require higher fissile content than the thermal reactor fuels because the cross sections of the fissile isotopes are smaller relative to the fertile isotopes and higher neutron leakage from the reactor core. The medium-sized high-burnup sodium-cooled fast reactors (SFRs) in the framework of uranium-plutonium/transuranic (U/Pu or U/TRU) fuel-cycle can be optimized to operate with less than 17 % of Pu/TRU content in the driver fuel while having higher TRU conversion ratios (CR~1.0) [1]. However, possible shortage or inaccessibility to TRU based fuel could be accommodated by the use of uranium-based fuels on demand such as low enriched uranium (LEU) having significantly higher 235U content than used in the commercial light water reactors (LWRs), which is defined as high-assay LEU. The reactor systems having low TRU conversion ratio are commonly categorized as burner reactors, which include LWRs and even can be achieved by FRs with designed to utilize higher TRU fractions (e.g., increased neutron leakage and lower fuel volume fractions). Such reactor systems need to be initially loaded with high excess reactivity, which decreases toward the end of cycle, in order to achieve target burnup conditions. Therefore, in order to offset the excess reactivity, neutron absorbing materials need to be inserted into the core to compensate (e.g., control rods). By reducing the neutron leakage (e.g., increasing the fuel volume fraction or thicker blankets), the TRU conversion ratio in the FR can be increased. If the TRU conversion ratio becomes 1.0 (technically slightly greater than 1.0 to account for process losses during recycle), the reactor is in the condition known as “breakeven”, in which fuel contains the same amount of fissile material after recycling that was used to fuel the reactor. In such a condition, combined with the fact that fission products do not have strong poisoning effects in FRs, the reactivity swing becomes smaller than that of burner type reactors. For breeders, the reactivity can increase toward the end of the cycle because more fissile material is produced than consumed. In this regard, the breakeven FR core is implicitly optimized in a sense by eliminating the large insertion of control elements to offset the reactivity during the normal operation. However, the breakeven condition here is assumed to be achieved only by the TRU based fuel. Possible lack of TRU based fuel needs to be compensated by available LEU resources containing equivalent amount of fissile (i.e., 235U). The use of LEU will have some impact on important safety parameters that need to be evaluated. U-235 has a higher effective delayed neutron fraction than Pu-239. Also, the number of neutrons produced by fissions per neutron absorption (i.e. ?) of 235U in the fast energy range (>1e4 eV) is lower than that of 239Pu, which may lead to the poor fissile conversion when LEU is used as a high-conversion FR fuel. The full-paper presents the study of the impact of partially loaded LEU fuels within TRU fueled breakeven SFR on the transition of nuclide evolutions and core characteristics particularly focusing on the burnup reactivity swing. The full paper analyzes how the large reactivity swing occurs during the LEU loading and addresses possible options to reduce it to the level equivalent to that of the TRU fueled SFR core.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Experimental Steps toward a Density Law for Chlorine-Crediting Criticality Models of Aqueous Plutonium solutions

Criticality accident prevention is an essential safety consideration for all operations involving fissionable and fissile materials. Predictive criticality calculations using advanced neutron transport codes, such as Monte Carlo N-Particle Transport (MCNP), are invaluable tools for designing and implementing operational limits. While indispensable, these tools are limited by the quality and accuracy of the inputs that the user provides to define the modeled system. Parameters such as atomic composition, shape, and material density must be accurately defined to obtain a meaningful result. In the case of material property details for a plutonium model, accurate material characterization data is sometimes sparse. Thus limitations in calculation accuracy can be reduced by improving our knowledge of material properties in the targeted fissile systems. One of the biggest remaining challenges to accurately defining fissile systems is the description of aqueous fissile solutions. Even simple properties, such as density, are not well-known for fissile solutions relevant to nuclear energy and security. Described here are initial efforts undertaken to improve criticality calculation inputs for fissile plutonium chloride solutions in water. This effort is focused on experimentally determining accurate solution characteristics for ternary plutonium chloride/hydrochloric acid/water systems, by measurement of water activity and solution density. The effect of inputting experimental densities for these solutions into MCNP criticality calculations is compared to the traditional approach of modeling an idealized (and fictitious) plutonium-water mixture. Expansion of these efforts to a working density law for aqueous plutonium chloride solutions is also discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Checkerboard seed-blanket thorium fuel core concepts for heavy water moderated reactors

New reactor concepts to implement thorium-based fuel cycles have been explored to achieve maximum resource utilization. Pressure tube heavy water reactors (PT-HWR) are highly advantageous for implementing the use of thorium-based fuels because of their high neutron economy and on-line re-fuelling capability. The use of heterogeneous seed-blanket core concepts in a PT-HWR where higher-fissile-content seed fuel bundles are physically separate from lower-fissile-content blanket bundles allows more flexibility and control in fuel management to maximize the fissile utilization and conversion of fertile fuel. The lattice concept chosen was a 35-element bundle made with a homogeneous mixture of reactor grade Pu (about 67 wt% fissile) and Th, and with a central zirconia rod to help reduce coolant void reactivity. Several checkerboard heterogeneous seed-blanket core concepts with plutonium-thorium-based fuels in a 700-MWe-class PT-HWR were analyzed, using a once-through thorium (OTT) cycle. Different combinations of seed and blanket fuel were tested to determine the impact on core-average burnup, fissile utilization, power distributions, and other performance parameters. It was found that various checkerboard core concepts can achieve a fissile utilization that is up to 26% higher than that achieved in a PT-HWR using more conventional natural uranium fuel bundles. Up to 60% of the Pu is consumed; up to 43% of the energy is produced from thorium, and up to 303 kg/year of Pa-233/U-233/U-235 are produced. Checkerboard cores with about 50% of low-power blanket bundles may require power de-rating (65% to 74%) to avoid exceeding maximum limits for channel and bundle powers and linear element ratings. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Adding Realism to Nuclear Material Dissolving Analysis

Two new criticality modeling approaches have greatly increased the efficiency of dissolver operations in H-Canyon. The first new approach takes credit for the linear, physical distribution of the mass throughout the entire length of the fuel assembly. This distribution of mass is referred to as the linear density. Crediting the linear density of the fuel bundles results in using lower fissile concentrations, which allows higher masses to be charged to the dissolver. Also, this approach takes credit for the fact that only part of the fissile mass is wetted at a time. There are multiple assemblies stacked on top of each other in a bundle. On average, only 50-75% of the mass (the bottom two or three assemblies) is wetted at a time. This means that only 50-75% (depending on operating level) of the mass is moderated and is contributing to the reactivity of the system. The second new approach takes credit for the progression of the dissolving process. Previously, dissolving analysis looked at a snapshot in time where the same fissile material existed both in the wells and in the bulk solution at the same time. The second new approach models multiple consecutive phases that simulate the fissile material moving from a high concentration in the wells to a low concentration in the bulk solution. This approach is more realistic and allows higher fissile masses to be charged to the dissolver.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of Synergistic Fuel Cycle Options with Thorium and Heavy Water Reactors

Fuel cycle options (FCOs) with thorium-based fuels have characteristics that may have benefits for meeting certain objectives, such as transuranic actinide inventory management and overall natural resource utilization. Neutron irradiation of thorium and uranium-233 results in negligible production of transuranic actinides. This advantage is compromised, to a degree, when thorium fuels are used in conjunction with uranium-238; however, strategic reprocessing and fuel use (e.g., recycle of plutonium and/or minor actinides) can be used to manage this problem. Furthermore, thorium FCOs with reprocessing can extend the availability of natural nuclear resources by breeding new fissile material, recovering and recycling unused material, and achieving high burnups. In instances where natural thorium is more readily available than uranium, FCOs which use thorium may be preferable from sustainability and energy security perspectives. However, many hybrid uranium-thorium FCOs struggle to perform well in this regard, since large amounts of external fissile material (and therefore natural uranium) are required to breed the required uranium-233. DOE's evaluation and screening effort reports that for every metric ton (MT) of U-233 bred in a light water reactor for reuse, about 1000 MT of natural uranium are required to support such breeding, much of which is used inefficiently due to enrichment. The combination of HWRs and thorium-based fuels has the potential to reduce this consumption of natural uranium resources. Because heavy water moderates neutrons without significant absorption, fissile material requirements are lower compared to those of LWRs. This has enabled conventional 'once-through' HWRs to operate with only slightly-enriched or even natural uranium. Also, HWRs can be combined with LWRs in multistage FCOs where used LWR fuel can be processed and the remaining fissile content is sufficient to support use as fuel in HWRs in spite of the presence of neutron poisons (e.g., uranium-236); this concept has been demonstrated at a research scale in Korea. Thus, additional energy is extracted from the same initial natural uranium feed and uranium enrichment effort. Another consideration with using thorium-based fuels in HWRs is the current limited operational experience of the reactors and associated fuel cycle facilities using these fuels. However, work continues internationally towards gaining further experience. For example, at equilibrium the third stage of India's planned Three-Stage Nuclear Power Program uses thorium/uranium-233 or thorium/plutonium fuels with a fissile supply from second-stage fast reactors. Further, China plans to experiment with low-enriched uranium (LEU)-Th CANFLEX fuel bundles in a once-through configuration in its HWRs and a long-term objective is to transition to thorium use in a closed HWR FCO. Vanderbilt University (VU) and Oak Ridge National Laboratory (ORNL) are characterizing multi-stage, thermal-reactor FCOs that incorporate thorium and examining their potential performance. This paper presents insights from the examination of FCOs which consider the synergy of HWRs and thorium. Two multi-stage FCOs which incorporate thorium-based fuels in HWRs have been examined for their potential, one which uses recycled PWR uranium oxide fuel in conjunction with thorium in an HWR, and another that uses recycled HWR fuel in an MSR which also includes thorium. Both of the systems studied offer resource utilization improvements as compared to a once-through LWR fueled with low-enrichment uranium and highlight the potential synergy of thorium and HWRs. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Chemistry Based Criticality Safety Evaluation of the HM-Process Mixer Settlers

The criticality safety of Savannah River Site's H Canyon two cycle uranium extraction and purification process, called the HM process, is examined. Explicit Monte Carlo models of the multi-stage mixer-settlers are generated for the first time using the KENO-VI module of the SCALE 6.1 code package and spanning normal operating conditions and a wide range of potential upset conditions with stagewise compositions based directly on SEPHIS Mod-4 chemistry models of the same conditions. To achieve industrial scale processing, mixer-settlers are often not geometrically favorable to prevent criticality so other means must be used for criticality safety, namely control of fissile concentration and mass. Historically, the worst case upset is a reflux condition resulting from a stream flow rate, temperature, or composition that is off from the normal operating conditions. A reflux is considered to be the state in which the fissile material is not proceeding in the desired direction, i.e. is stripping rather than extracting or vice versa. The criticality safety analyses which set the current operational limits were conducted many years ago with less sophisticated codes and only loosely tied criticality to chemistry. Those analyses conservatively assumed that a reflux changed the behavior of the mixer-settler such that the fissile content collected continuously in only three stages of the mixer-settler, at a rate based on the SEPHIS modeling, until criticality occurred. This implies that under some condition the distribution coefficient of the fissile material either goes to infinity or zero, which is not physically achievable. In such a scenario, the operator would have some amount of time to react and correct the problem before sufficient fissile material built up in the mixer-settler and caused a criticality. In reality, an upset in a stream would cause the process to transition to a new, though undesired, equilibrium state of operation. The distribution coefficients would change, but would not diverge. In this work, aqueous and organic streams are modeled for both the mixer and the settler region of each stage of each bank using chemical distribution data from SEPHIS and solving the chemical equations for a wide range of operational parameters spanning normal and upset conditions. Conservative assumptions are made regarding enrichment and reflection and the whole bank multiplication factor is evaluated using discrete stage-wise compositions. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

C-400 and C-409 Criticality Incredible Road Map

Many guides and standards describe a process for evaluating process operations with known quantities of fissile material. The accepted industry guides and standards for performing criticality evaluations for fissile material operations are not well suited for operating systems that may contain residual fissile material. The Paducah Site deactivation activities includes large process components that have unfavorable geometries for the {sup 235}U enrichment levels present. The fissile material holdup in these components can range from negligible residual quantities to significant deposits weighing several hundred pounds. The purpose of this white paper is to outline a methodology that can be used to declare a facility as criticality incredible (CI). For the purpose of this paper, criticality incredible means that the inventory and its form and distribution within the facility does not need Nuclear Criticality Safety Evaluation (NCSE) type (e.g., administrative or engineered) controls. This assumes of course that certain project assumptions are maintained. For example in the facilities that will be discussed within this paper, wet decontamination is not part of the planned demolition and disposal operations. The proposed methodology for deactivation of a facility to the point that criticality incredible can be declared will be applied to the C-400 Chemical Cleaning Building and to the C-409 Decontamination Facility at the Paducah Gaseous Diffusion Plant (PGDP). The purpose and intent of the CI declaration is to release a facility from Nuclear Criticality Safety (NCS) requirements and simplify the demolition of the facility. In practical terms, this means the facility can be re-categorized as < a Hazard Category 3 facility per DOE-STD-1027-92 Hazard Categorization and Accident Analysis Techniques for compliance with DOE Order 5480.23, Nuclear Safety Analysis Reports, NCS controls are not needed, and the Criticality Accident Alarm Systems (CAAS) can be removed from service. The only involvement from the site NCS program following the declaration would be to ensure that the underlying assumptions are not violated through discovered conditions or project changes. This includes the institutional control of preventing new fissile material from being introduced into the facility. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Review of non destructive assay techniques utilised for decommissioning of plutonium facilities at AWE - 14418

Over the past fifteen years AWE has decommissioned and size reduced a large number of glove boxes that contained a wide spectrum of equipment that ranged from highly radiation attenuating structures, such as furnaces and lathes, to other less radiation attenuating apparatus, such as small discrete tools or simple work benches. In order to generate meaningful glove box residual fissile material inventory data, which can constructively inform the selection of measures needed to underwrite the criticality safety of size reduction and consignment to waste activities, several different types of Non Destructive Assay (NDA) measurement techniques are available at AWE. These are deployed for the estimate of the residual fissile material inventory prior to decommissioning activities and for the final NDA of waste containers, post decommissioning. The techniques range from the Decommissioning In-Situ Plutonium Inventory Monitor (DISPIM), through other Neutron Coincidence Counting (NCC) techniques (Neutron Panel monitoring) and gamma measurements to consideration of Thermo Luminescent Detector (TLD) data. This paper will present a comparison of the fissile material identified in the waste generated post decommissioning operations to the NDA estimate of the residual fissile material inventory for the glove boxes, as well as provide a direct comparison between the different NDA techniques available at AWE. The findings to date indicate that the glove box residual fissile material inventory used for criticality safety purposes bounds the decommissioning process, subject to the suitable deployment of the NDA technique and the inclusion of appropriate uncertainties. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Methodology for defining intermediate level waste package characteristics that ensure criticality safety in a geological disposal facility - 14599

Radioactive Waste Management (RWM) is responsible for implementing geological disposal of the UK's higher activity radioactive wastes. These wastes include fissile nuclides and, therefore, demonstration of the criticality safety of the wastes under disposal conditions forms an important component of RWM's disposal system safety case. The basis for ensuring criticality safety of intermediate level waste (ILW) packages is to specify controls on the fissile material content of individual packages through the application of deterministic criticality safety assessments (CSAs). The approach is defined and controlled through RWM's Disposability Assessment process, which aims to ensure that: criticality is prevented during waste package transport to a GDF; the risk of criticality is tolerable and as low as reasonably practicable (ALARP) during GDF operations; and the likelihood and consequences of criticality arising from the evolution of waste packages after GDF closure are low. The most restrictive phase determines the package fissile material limit and, until now, in many cases the GDF post-closure phase has provided the most restrictive limit. Currently, the GDF post-closure limits are derived deterministically using highly stylised and conservative assumptions about fissile material accumulations occurring on very long timescales into the future. RWM, waste producers and regulators do not currently consider this approach to be yielding an appropriate balance of risk. Therefore, RWM is modifying the process for setting fissile material limits on ILW packages by making use of the outcomes of its recent research projects to establish the likelihood of post-closure criticality in a GDF and the consequences of hypothetical post-closure criticality events (presented in companion papers). This paper presents the revised methodology, which is based on the requirement that criticality in a GDF can be demonstrated to be of low and tolerable consequences with regard the performance of a GDF. A probabilistic 'low-likelihood package envelope' is proposed that establishes the packaging and disposal facility conditions under which post-closure criticality is considered to be of low likelihood and low consequence. The bounding conditions for establishing the extent of the package envelope have been evaluated through application of the methodologies and models developed in RWM's Likelihood of Criticality research project. It is expected that the vast majority of ILW packages would meet the package envelope requirements. The methodology also allows the use of other options, such as deterministic CSAs, for waste packages that fall outside the low-likelihood package envelope. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Annular seed-blanket thorium fuel core concepts for heavy water moderated reactors

New reactor concepts to implement thorium-based fuel cycles have been explored to achieve maximum resource utilization. Pressure tube heavy water reactors (PT-HWR) are highly advantageous for implementing the use of thorium-based fuels because of their high neutron economy and on-line re-fuelling capability. The use of heterogeneous seed-blanket core concepts in a PT-HWR where higher-fissile-content seed fuel bundles are physically separate from lower-fissile-content blanket bundles allows more flexibility and control in fuel management to maximize the fissile utilization and conversion of fertile fuel. The lattice concept chosen is a 35-element bundle made with a homogeneous mixture of reactor grade Pu and Th, and with a central zirconia rod to help reduce coolant void reactivity. Several annular heterogeneous seed-blanket core concepts with plutonium-thorium-based fuels in a 700-MWe-class PT-HWR were analyzed, using a once-through thorium (OTT) cycle. Different combinations of seed and blanket fuel were tested to determine the impact on core-average burnup, fissile utilization, power distributions, and other performance parameters. It was found that the various core concepts can achieve a fissile utilization that is up to 30% higher than is currently achieved in a PT-HWR using conventional natural uranium fuel bundles. Up to 67% of the Pu is consumed; up to 43% of the energy is produced from thorium, and up to 363 kg/year of U-233 is produced. Seed-blanket cores with ∼50% content of low-power blanket bundles may require power de-rating (∼58% to 65%) to avoid exceeding maximum limits for peak channel power, bundle power and linear element ratings. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗