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Assessment of the quality of nuclear data for stable oxygen isotopes for Intentional Forensics applications

The Intentional Forensics (IF) project seeks to design a suite of tagging materials that can be used to unobtrusively “barcode” nuclear fuel. The idea being that, if the fuel leaves institutional controls and is later recovered, the “barcode” can be used to determine the provenance of the fuel. The IF project is investigating several schemes for this “barcode” and taggants with tailored isotopic compositions are once leading concept. Recently 18 O was suggested as a potential taggant [IF2023]. This report assesses the quality of 16,17,18 O evaluations in the ENDF/B-VIII.0 library [ENDF8.0]. In a neutron-rich environment such as a nuclear reactor, we are interested in two main processes – neutron scattering and neutron absorption (or capture). For the typical neutron energies encountered in a reactor, absorption is determined exclusively by the neutron radiative capture cross section (in which a neutron is absorbed, and the residual nucleus emits one or more gamma rays). The capture cross sections are described by and can be completely determined from R-matrix parameters in the ENDF evaluations. Therefore, it is sufficient to consider the quality of the neutron resonance part of these evaluations. Neutron scattering is determined mainly by the elastic scattering cross section which is very similar for all oxygen isotopes and is essentially constant until around 100 keV. The cross section varies from 3-4 barns, depending on the isotope, and 16 O has the largest elastic cross section of all isotopes. Therefore, we expect that significant amounts of 17 O and 18 O could diminish the moderating role of oxygen in fuel. We note that, in traditional power reactor, the hydrogen in the coolant water provides the vast majority of the moderation in the reactor, so the impact of 17 O and 18 O in any taggant would be minimal. At higher energies, neutron resonances start to play a role and the R-matrix parameters determine the cross sections. Fig. 1 shows the mass region near stable oxygen isotopes. As nuclei capture neutrons, they transmute into a different isotope, one unit to the right. In particular, 16 O transmutes to 17 O, 17 O transmutes to 18 O and 18 O transmutes to 19 O. 19 O, being unstable, beta decays in 27 s to 19 F. So, even if the 18 O neutron capture data is good, the fact that it transmutes into 19 F may be problematic and needs investigation. Fig. 2 from [NuDat] shows the thermal neutron capture cross sections for all nuclei in the ENDF/B-VII.1 library [ENDF7.1]. Clearly oxygen thermal capture values are quite small compared to other nuclei. Note, there is no 18 O evaluation in the ENDF/B-VII.1 library. In any event, given that neutron capture events lower the reactor reactivity and potentially induce chemical changes in the fuel, we will focus our attention on the capture part of the neutron resonances.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Transuranic Waste Burning Potential of Thorium Fuel in a Fast Reactor - 12423

Westinghouse Electric Company (referred to as 'Westinghouse' in the rest of this paper) is proposing a 'back-to-front' approach to overcome the stalemate on nuclear waste management in the US. In this approach, requirements to further the societal acceptance of nuclear waste are such that the ultimate health hazard resulting from the waste package is 'as low as reasonably achievable'. Societal acceptability of nuclear waste can be enhanced by reducing the long-term radiotoxicity of the waste, which is currently driven primarily by the protracted radiotoxicity of the transuranic (TRU) isotopes. Therefore, a transition to a more benign radioactive waste can be accomplished by a fuel cycle capable of consuming the stockpile of TRU 'legacy' waste contained in the LWR Used Nuclear Fuel (UNF) while generating waste which is significantly less radio-toxic than that produced by the current open U-based fuel cycle (once through and variations thereof). Investigation of a fast reactor (FR) operating on a thorium-based fuel cycle, as opposed to the traditional uranium-based is performed. Due to a combination between its neutronic properties and its low position in the actinide chain, thorium not only burns the legacy TRU waste, but it does so with a minimal production of 'new' TRUs. The effectiveness of a thorium-based fast reactor to burn legacy TRU and its flexibility to incorporate various fuels and recycle schemes according to the evolving needs of the transmutation scenario have been investigated. Specifically, the potential for a high TRU burning rate, high U-233 generation rate if so desired and low concurrent production of TRU have been used as metrics for the examined cycles. Core physics simulations of a fast reactor core running on thorium-based fuels and burning an external TRU feed supply have been carried out over multiple cycles of irradiation, separation and reprocessing. The TRU burning capability as well as the core isotopic content have been characterized. Results will be presented showing the potential for thorium to reach a high TRU transmutation rate over a wide variety of fuel types (oxide, metal, nitride and carbide) and transmutation schemes (recycle or partition of in-bred U-233). In addition, a sustainable scheme has been devised to burn the TRU accumulated in the core inventory once the legacy TRU supply has been exhausted, thereby achieving long-term virtually TRU-free. A comprehensive 'back-to-front' approach to the fuel cycle has recently been proposed by Westinghouse which emphasizes achieving 'acceptable', low-radiotoxicity, high-level waste, with the intent not only to satisfy all technical constraints but also to improve public acceptance of nuclear energy. Following this approach, the thorium fuel cycle, due to its low radiotoxicity and high potential for TRU transmutation has been selected as a promising solution. Additional studies not shown here have shown significant reduction of decay heat. The TRU burning potential of the Th-based fuel cycle has been illustrated with a variety of fuel types, using the Toshiba ARR to perform the analysis, including scenarios with continued LWR operation of either uranium fueled or thorium fueled LWRs. These scenarios will afford overall reduction in actinide radiotoxicity, however when the TRU supply is exhausted, a continued U- 235 LWR operation must be assumed to provide TRU makeup feed. This scenario will never reach the characteristically low TRU content of a closed thorium fuel cycle with its associated potential benefits on waste radiotoxicity, as exemplified by the transition scenario studied. At present, the cases studied indicate ThC as a potential fuel for maximizing TRU burning, while ThN with nitrogen enriched to 95% N-15 shows the highest breeding potential. As a result, a transition scenario with ThN was developed to show that a sustainable, closed Th-cycle can be achieved starting from burning the legacy TRU stock and completing the transmutation of the residual TRU remaining in the core inventory after the legacy TRU external supply has been exhausted. The radiotoxicity of the actinide waste during the various phases has been characterized, showing the beneficial effect of the decreasing content of TRU in the recycled fuel as the transition to a closed Th-based fuel cycle is undertaken. Due to the back-to-front nature of the proposed methodology, detailed designs are not the first step taken when assessing a fuel cycle scenario potential. As a result, design refinement is still required and should be expected in future studies. Moreover, significant safety assessment, including determination of associated reactivity coefficients, fuel and reprocessing feasibility studies and economic assessments will still be needed for a more comprehensive and meaningful comparison against other potential solutions. With the above considerations in mind, the potential advantages of thorium fuelled reactors on HLW management optimization lead us to believe that thorium fuelled reactor systems can play a significant role in the future and deserve further consideration. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Postirradiation Examination of FUTURIX-FTA metallic alloy experiments

Two different metallic nuclear fuel alloys intended for transmutation applications in fast neutron spectrum nuclear reactors have been irradiated, and their performance has been evaluated after irradiation. These alloys contained elevated levels of plutonium and other minor actinides (Am, Np) compared to historically irradiated fast reactor fuel to ascertain the impact of these isotopes on fuel performance. The irradiation of these alloys was performed at the Phénix fast reactor in France to facilitate comparisons between true fast spectrum irradiations and pseudo-fast spectrum irradiations performed at the thermal neutron spectrum Idaho National Laboratory Advanced Test Reactor. The irradiation tests were designated FUTURIX-FTA DOE1 which contained a low-fertile alloy and FUTURIX-FTA DOE2 which contained a non-fertile alloy. The DOE1 fuel was irradiated to a measured burnup of 9.5 % fissions per initial heavy metal atom (FIMA), and the DOE2 fuel was irradiated to a measured burnup of 12.7 % fissions per initial heavy metal atom. This work reports baseline Postirradiation Examination (PIE) results for DOE1 and DOE2. Fuel swelling, fission product distribution, cladding strain, fission gas release, fuel microstructure, fuel cladding chemical interaction and minor actinide transmutation were all evaluated. Cladding strain was negligible and fission gas release was 52% for DOE1 and 69% for DOE2. The exams show the 2 pins behaved very similar to EBR-II metallic fuel experience. Minor actinides seem to not affect the performance of this candidate transmutation fuel. As a result, performance data from these irradiations can be used to inform the feasibility of minor actinide transmutation in future reactor systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Competing effects of electronic and nuclear energy loss on microstructural evolution in ionic-covalent materials

Ever increasing energy needs have raised the demands for advanced fuels and cladding materials that withstand the extreme radiation environments with improved accident tolerance over a long period of time. Ceria (CeO2) is a well known ionic conductor that is isostructural with urania and plutonia-based nuclear fuels. In the context of nuclear fuels, immobilization and transmutation of actinides, CeO2 is a model system for radiation effect studies. Covalent silicon carbide (SiC) is a candidate for use as structural material in fusion, cladding material for fission reactors, and an inert matrix for the transmutation of plutonium and other radioactive actinides. Understanding microstructural change of these ionic-covalent materials to irradiation is important for advanced nuclear energy systems. While displacements from nuclear energy loss may be the primary contribution to damage accumulation in a crystalline matrix and a driving force for the grain boundary evolution in nanostructured materials, local non-equilibrium disorder and excitation through electronic energy loss may, however, produce additional damage or anneal pre-existing defects. At intermediate transit energies where electronic and nuclear energy losses are both significant, synergistic, additive or competitive processes may evolve that affect the dynamic response of materials to irradiation. The response of crystalline and nanostructured CeO2 and SiC to ion irradiation are studied under different nuclear and electronic stopping powers to describe some general material response in this transit energy regime. Although fast radiation-induced grain growth in CeO2 is evident with no phase transformation, different fluence and dose dependence on the growth rate is observed under Si and Au irradiations. While grain shrinkage and amorphization are observed in the nano-engineered 3C SiC with a high-density of stacking faults embedded in nanosize columnar grains, significantly enhanced radiation resistance is attributed to stacking faults that promote efficient point defect annihilation. Moreover, competing effects of electronic and nuclear energy loss on the damage accumulation and annihilation are observed in crystalline 4H-SiC. Systematic experiments and simulation effort are needed to understand the competitive or synergistic effects.

36 MATERIALS SCIENCE↗

Nuclear Considerations for the Application of Lanthanum Telluride in Future Radioisotope Power Systems

Thermoelectric-based radioisotope power systems (RPSs) produced in the United States convert the heat generated by the radioactive emission of alpha particles from plutonium dioxide ( 238 puO 2 ) into electricity by means of the Seebeck effect [1]. Certain designs for thermoelectric convertors propose the use of lanthanum telluride (La 3 Te 4 ) materials due to their significant conversion capabilities [2]. The generation of neutrons from spontaneous fission and alpha-neutron (α,n) reactions is also associated with the decay of 238 PuO 2 . A portion of these neutrons will interact with the thermoelectric materials and induce trace amounts of transmutation reactions in various lanthanum and tellurium isotopes. While very small quantities of several transmutation products are predicted, the most significant reaction channels are expected to produce trace amounts of iodine which will accumulate over time. Although iodine is classified as a halogen, it is the least reactive of the halogens, and as such, it is the most likely to be able to chemically convert back into the molecule I 2 . Since I 2 is a gas at RPS temperatures, it may be possible for iodine to attack other components in the thermoelectric cavity of an RPS system. Iodine reacts easily with metals to produce a wide variety of salts. This behavior could affect the performance of La 3 Te 4 thermoelectric devices, particularly the segmented architectures that include multiple sets of bonding and metallization layers. In this type of architecture, several segments of different thermoelectric materials are joined to increase the average thermoelectric figure of merit over a relatively large temperature gradient. It is plausible that sophisticated bonding/metallization layers could be required to join the segment interfaces to each other and to the cold- and hot-shoe materials. The long-term stability and performance of these segmented material combinations could degrade as a result of the potential formation and reactions of metal-iodide compounds at the segment interfaces. This paper (1) investigates the degree to which, if any, this process may threaten potential La 3 Te 4 thermoelectric technologies, (2) presents calculations of the amount of iodine generated over the operational life of a radioisotope thermoelectric generator design, and (3) discusses the potential effects of the resulting material's chemical reactions in a segmented couple-level architecture containing La 3 Te 4 . Conclusions drawn from combined particle transport, transmutation, and thermochemical calculations for La 3 Te 4 thermoelectric materials undergoing a notional 20-year mission scenario suggest that there is no significant potential for transmutation-induced thermoelectric (TE) performance degradation.

Smith, Michael↗

NUCLEAR ENERGY SYSTEM COST MODELING

The U.S. Department of Energy’s Fuel Cycle Technologies (FCT) Program is preparing to perform an evaluation of the full range of possible Nuclear Energy Systems (NES) in 2013. These include all practical combinations of fuels and transmuters (reactors and sub-critical systems) in single and multi-tier combinations of burners and breeders with no, partial, and full recycle. As part of this evaluation, Levelized Cost of Electricity at Equilibrium (LCAE) ranges for each representative system will be calculated. To facilitate the cost analyses, the 2009 Advanced Fuel Cycle Cost Basis Report is being amended to provide up-to-date cost data for each step in the fuel cycle, and a new analysis tool, NE-COST, has been developed. This paper explains the innovative “Island” approach used by NE-COST to streamline and simplify the economic analysis effort and provides examples of LCAE costs generated. The Island approach treats each transmuter (or target burner) and the associated fuel cycle facilities as a separate analysis module, allowing reuse of modules that appear frequently in the NES options list. For example, a number of options to be screened will include a once-through uranium oxide (UOX) fueled light water reactor (LWR). The UOX LWR may be standalone, or may be the first stage in a multi-stage system. Using the Island approach, the UOX LWR only needs to be modeled once and the module can then be reused on subsequent fuel cycles. NE-COST models the unit operations and life cycle costs associated with each step of the fuel cycle on each island. This includes three front-end options for supplying feedstock to fuel fabrication (mining/enrichment, reprocessing of used fuel from another island, and/or reprocessing of this island’s used fuel), along with the transmuter and back-end storage/disposal. Results of each island are combined based on the fractional energy generated by each islands in an equilibrium system. The cost analyses use the probability distributions of key parameters and employs Monte Carlo sampling to arrive at an island’s cost probability density function (PDF). When comparing two NES to determine delta cost, strongly correlated parameters can be cancelled out so that only the differences in the systems contribute to the relative cost PDFs. For example, one comparative analysis presented in the paper is a single stage LWR-UOX system versus a two-stage LWR-UOX to LWR-MOX system. In this case, the first stage of both systems is the same (but with different fractional energy generation), while the second stage of the UOX to MOX system uses the same type transmuter but the fuel type and feedstock sources are different. In this case, the cost difference between systems is driven by only the fuel cycle differences of the MOX stage.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization of a minor actinides bearing metallic fuel pin irradiated in EBR-II

The X501 transmutation experiment irradiated in Experimental Breeder Reactor II (EBR-II) was intended to evaluate the safety and performance of the addition of minor actinides (Am, Np) into the metallic nuclear fuel system. The irradiation of this experiment is also of paramount importance for comparisons between true fast spectrum irradiations (e.g. EBR-II) and shrouded irradiation capsules performed at the thermal neutron spectrum Idaho National Laboratory Advanced Test Reactor. The X501 experimental fuel pins were irradiated to a peak measured burnup of 6.2% fission per initial heavy metal atom. This paper reports and discusses Postirradiation Examination results for one of two minor actinide bearing pins from the EBR-II X-501 experiment (X501-G591) with a focus on fuel microstructure evolution. Additionally, fuel swelling, fission product distribution, cladding strain, fission gas release, fuel microstructure and fuel cladding chemical interaction were all evaluated. The fission gas release was 79.9% and the microstructure along the fuel pin presented several characteristics very similar to other EBR-II U-Pu-Zr ternary metallic fuel experience. Minor actinides seem to not dramatically affect the overall performance of this candidate transmutation fuel. Scanning Electron Microscopy was also performed and an in-depth characterization of the different regions and phases is presented. Performance data from these irradiations can be used to inform the feasibility of minor actinide transmutation in future reactor systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Actinide management with commercial fast reactors

The capability of plutonium-breeding and minor-actinide (MA) transmutation in the Japanese commercial sodium-cooled fast reactor offers one of practical solutions for obtaining sustainable energy resources as well as reducing radioactive toxicity and inventory. The reference core design meets the requirement of flexible breeding ratio from 1.03 to 1.2. The MA transmutation amount has been evaluated as 50-100 kg/GW{sub e}y if the MA content in fresh fuel is 3-5 wt%, where about 30-40% of initial MA can be transmuted in the discharged fuel.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Apres ORIENT, a PT-based new resource strategy in nuclear fuel cycle

The 'Apres ORIENT' research program, recently initiated in 2011, will deal with the transmutation of radioactive fission products (FP) to create rare metals / rare earth (RE) elements (NRM) by neutron capture on the FP followed by beta- decay. Target are radioactive FP and any created NRM should be more valuable and non-, or significantly less, radioactive than the initial FP. In the case of transmutation of radioactive Ba (i.e., non RE element) to La (i.e., light RE), the yield of {sup 139}La was low (< 3.5 %) with 5 years irradiation at thermal neutron energy conditions. However, by neutron irradiation in the fast reactor blanket region corresponding to a resonance energy range of 10 - 100 keV with an expected cross section, σ{sub γ}=0.27 b, of {sup 139}Ba a higher transmutation rate of more than 12 % over 5 years is obtained when the neutron flux is 1.0*10{sup 15} n/cm{sup 2}*s. Created La will be non-radioactive (< 0.001 Bq/g) despite natural La is slightly radioactive ca. 1 Bq/g. To facilitate Ba/La separation various kinds of crown ether (CE) resins were tested. The highest separation of Ba{sup 2+}/La{sup 3+} was obtained by a newly synthesized Benzo-18-Crown-6 (BC18) -substituted resin indicating SF(Ba/La) > 1,000 at 5 mol/l HCl medium. To confirm the scientific feasibility on such new program, actual irradiation tests by various target materials in a test reactor and separation/analysis of the products are required. While the test reactor available at the University of California Irvine has a steady state flux in the order of 10{sup 12} n/cm{sup 2}*s which is at least 2 orders of magnitude lower than a conventional power reactor, proof-of-concept investigations will be carried out since the production of nuclides should scale up linearly with the neutron flux. (author)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Irradiation performance of nonfertile (Pu-MA-Zr) fast reactor metal fuels

This work was part of a program begun in 2001 to develop advanced nuclear fuels, originally as carriers for plutonium and minor actinides (neptunium, curium, and americium) taken from spent commercial light-water reactors (LWR) so that the plutonium and minor actinides could be ‘burned’ or transmuted in an accelerator or a fast nuclear reactor. A central part of these experiment programs has been the development of advanced fast reactor fuels, because a fast reactor was considered the most efficient vehicle to transmute the actinide waste products, and metallic fuels is a central focus of these tests. An experiment design was developed in which a thermal test reactor, the Advanced Test Reactor (ATR), was used to test small fuel pin prototypes, by creating areas in the core shielded by cadmium filters to produce a largely epithermal and fast neutron spectrum environment in which the pins could be irradiated. The results of non-fertile metallic fuel (no uranium) tests are presented here. Pu-Am-Np-Zr fuels were irradiated to fission densities up to 33 × 10 20 fission/cm 3 and Pu-239 depletions of up to 39%. The depletions were created by roughly 2/3 by fission and 1/3 by transmutation neutron capture. Up to five fuel ‘rodlets’ were irradiated in three sealed capsules stacked axially in the core, and the peak cladding temperatures ranged from 300°C to 500°C, depending on axial location as those near the core centerline are operating hotter and to higher fission densities. Several post-irradiation examinations (precision gamma scanning and fission gas release) were similar to other historical metal fuel experiments in fast reactors. However, optical metallography indicated that two of the rodlets had breached. The exact reasons are unclear. Due to the design of this irradiation experiment a rodlet breach could have increased the temperature in others in the same capsule by contaminating the thermal gap helium with heavier and less conductive fission product gases. Finally, some of those rodlets showed high amounts of fuel/cladding chemical interaction (FCCI).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of Phosphorous-doping and High Temperature Annealing on CVD grown 3C-SiC

The integrity and property behavior of the SiC layer of the Tri-isotropic (TRISO) coated particle (CP) for high temperature reactors (HTR) are very important as the SiC layer is the main barrier for gaseous and metallic fission product release. This study describes the work done on un-irradiated SiC samples prepared with varying phosphorus levels to simulate the presence of phosphorus due to transmutation. 30Si transmutes to phosphorous (31P) and other transmutation products during irradiation, which may affect the integrity of the SiC layer. The P-doping levels of the SiC samples used in this study cover the range from 1.1x1015 to 1.2x1019 at/cm3 and are therefore relevant to the PBMR operating conditions. Annealing from 1000 C to 2100 C was performed to study the possible changes in nanostructures and various properties due to temperature. Characterization results by X-ray diffraction (XRD), secondary ion mass spectrometry (SIMS), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and high resolution transmission electron microscopy (HRTEM), are reported in this article. As grain boundary diffusion is identified as a possible mechanism by which 110mAg, one of the fission activation products, might be released through intact SiC layer, grain size measurements is also included in this study. Temperature is evidently one of the factors/parameters amongst others known to influence the grain size of SiC and therefore it is important to investigate the effect of high temperature annealing on the SiC grain size. The ASTM E112 method as well as electron back scatter diffraction (EBSD) was used to determine the grain size of various commercial SiC samples and the SiC layer in experimental PBMR Coated Particles (CPs) after annealing at temperatures ranging from 1600 C to 2100 C. The HRTEM micrograph of the decomposition of SiC at 2100 C are shown and discussed. Nanotubes were not identified during the TEM and HRTEM analysis although graphitic structures were identified. The preliminary conclusion reached is that the P-content at these experimental levels (1.1x1015 - 1.2x1019 atom/cm3) does not have a significant influence on the nanostructure of SiC at high temperatures without irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Understanding Boron through Size-Selected Clusters: Structure, Chemical Bonding, and Fluxionality

Conspectus Boron is an interesting element with unusual polymorphism. While three-dimensional (3D) structural motifs are prevalent in bulk boron, atomic boron clusters are found to have planar or quasi-planar structures, stabilized by localized two-center–two-electron (2c–2e) σ bonds on the periphery and delocalized multicenter–two-electron (nc–2e) bonds in both σ and π frameworks. Electron delocalization is a result of boron’s electron deficiency and leads to fluxional behavior, which has been observed in B13+ and B19–. A unique capability of the in-plane rotation of the inner atoms against the periphery of the cluster in a chosen direction by employing circularly polarized infrared radiation has been suggested. Such fluxional behaviors in boron clusters are interesting and have been proposed as molecular Wankel motors. The concepts of aromaticity and antiaromaticity have been extended beyond organic chemistry to planar boron clusters. The validity of these concepts in understanding the electronic structures of boron clusters is evident in the striking similarities of the π-systems of planar boron clusters to those of polycyclic aromatic hydrocarbons, such as benzene, naphthalene, coronene, anthracene, or phenanthrene. Chemical bonding models developed for boron clusters not only allowed the rationalization of the stability of boron clusters but also lead to the design of novel metal-centered boron wheels with a record-setting planar coordination number of 10. The unprecedented highly coordinated borometallic molecular wheels provide insights into the interactions between transition metals and boron and expand the frontier of boron chemistry. Another interesting feature discovered through cluster studies is boron transmutation. Even though it is well-known that B–, formed by adding one electron to boron, is isoelectronic to carbon, cluster studies have considerably expanded the possibilities of new structures and new materials using the B–/C analogy. It is believed that the electronic transmutation concept will be effective and valuable in aiding the design of new boride materials with predictable properties. The study of boron clusters with intermediate properties between those of individual atoms and bulk solids has given rise to a unique opportunity to broaden the frontier of boron chemistry. Understanding boron clusters has spurred experimentalists and theoreticians to find new boron-based nanomaterials, such as boron fullerenes, nanotubes, two-dimensional boron, and new compounds containing boron clusters as building blocks. Here, a brief and timely overview is presented addressing the recent progress made on boron clusters and the approaches used in the authors’ laboratories to determine the structure, stability, and chemical bonding of size-selected boron clusters by joint photoelectron spectroscopy and theoretical studies. Specifically, key findings on all-boron hydrocarbon analogues, metal-centered boron wheels, and electronic transmutation in boron clusters are summarized.

Environmental Molecular Sciences Laboratory↗

Heterogeneous recycling in fast reactors

Current sodium fast reactor (SFR) designs have avoided the use of depleted uranium blankets over concerns of creating weapons grade plutonium. While reducing proliferation risks, this restrains the reactor design space considerably. This project will analyze various blanket and transmutation target configurations that could broaden the design space while still addressing the non-proliferation issues. The blanket designs will be assessed based on the transmutation efficiency of key minor actinide (MA) isotopes and also on mitigation of associated proliferation risks. This study will also evaluate SFR core performance under different scenarios in which depleted uranium blankets are modified to include minor actinides with or without moderators (e.g. BeO, MgO, B 4 C, and hydrides). This will be done in an effort to increase the sustainability of the reactor and increase its power density while still offering a proliferation resistant design with the capability of burning MA waste produced from light water reactors (LWRs). Researchers will also analyze the use of recycled (as opposed to depleted) uranium in the blankets. The various designs will compare MA transmutation efficiency, plutonium breeding characteristics, proliferation risk, shutdown margins and reactivity coefficients with a current reference sodium fast reactor design employing homogeneous recycling. The team will also evaluate the out-of-core accumulation and/or burn-down rates of MAs and plutonium isotopes on a cycle-by-cycle basis. This cycle-by-cycle information will be produced in a format readily usable by the fuel cycle systems analysis code, VISION, for assessment of the sustainability of the deployment scenarios.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Advanced Burner Reactor with Breed-and-Burn Thorium Blankets for Improved Economics and Resource Utilization

This study assesses the feasibility of designing Seed and Blanket (S&B) Sodium-cooled Fast Reactor (SFR) to generate a significant fraction of the core power from radial thorium fueled blankets that operate on the Breed-and-Burn (B&B) mode without exceeding the radiation damage constraint of presently verified cladding materials. The S&B core is designed to maximize the fraction of neutrons that radially leak from the seed (or “driver”) into the subcritical blanket and reduce neutron loss via axial leakage. The blanket in the S&B core makes beneficial use of the leaking neutrons for improved economics and resource utilization. A specific objective of this study is to maximize the fraction of core power that can be generated by the blanket without violating the thermal hydraulic and material constraints. Since the blanket fuel requires no reprocessing along with remote fuel fabrication, a larger fraction of power from the blanket will result in a smaller fuel recycling capacity and lower fuel cycle cost per unit of electricity generated. A unique synergism is found between a low conversion ratio (CR) seed and a B&B blanket fueled by thorium. Among several benefits, this synergism enables the very low leakage S&B cores to have small positive coolant voiding reactivity coefficient and large enough negative Doppler coefficient even when using inert matrix fuel for the seed. The benefits of this synergism are maximized when using an annular seed surrounded by an inner and outer thorium blankets. Among the high-performance S&B cores designed to benefit from this unique synergism are: (1) the ultra-long cycle core that features a cycle length of ~7 years; (2) the high-transmutation rate core where the seed fuel features a TRU CR of 0.0. Its TRU transmutation rate is comparable to that of the reference Advanced Burner Reactor (ABR) with CR of 0.5 and the thorium blanket can generate close to 60% of the core power; but requires only one sixth of the reprocessing and fabrication capacity per unit of core power. Nevertheless, these high-performance cores were designed to set upper bounds on the S&B core performance by using larger height and pressure drop than those of typical SFR design. A study was subsequently undertaken to quantify the tradeoff between S&B core design variables and the core performance. This study concludes that a viable S&B core can be designed without significant deviation from SFR core design practices. For example, the S&B core with 120cm active height will be comparable in volume, HM mass and specific power with the S-PRISM core and could fit within the S-PRISM reactor vessel. 43% of this core power will be generated by the once-through thorium blanket; the required capacity for reprocessing and remote fuel fabrication per unit of electricity generated will be approximately one fifth of that for a comparable ABR. The sodium void worth of this 120cm tall S&B core is significantly less positive than that of the reference ABR and the Doppler coefficient is only slightly smaller even though the seed uses a fertile-free fuel. The seed in the high transmutation core requires inert matrix fuel (TRU-40Zr) that has been successfully irradiated by the Fuel Cycle Research & Development program. An additional sensitivity analysis was later conducted to remove the bias introduced by the discrepancy between radiation damage constraints -- 200 DPA applied for S&B cores and fast fluence of 4x1023 n(>0.1MeV)/cm2 applied for ABR core design. Although the performance characteristics of the S&B cores are sensitive to the radiation damage constraint applied, the S&B cores offer very significant performance improvements relative to the conventional ABR core design when using identical constraint.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

MANTA. An Integral Reactor Physics Experiment to Infer the Neutron Capture Cross Sections of Actinides and Fission Products in Fast and Epithermal Spectra

Neutron cross-sections characterize the way neutrons interact with matter. They are essential to most nuclear engineering projects and, even though theoretical progress has been made as far as the predictability of neutron cross-section models, measurements are still indispensable to meet tight design requirements for reduced uncertainties. Within the field of fission reactor technology, one can identify the following specializations that rely on the availability of accurate neutron cross-sections: (1) fission reactor design, (2) nuclear fuel cycles, (3) nuclear safety, (4) nuclear safeguards, (5) reactor monitoring and neutron fluence determination and (6) waste disposal and transmutation. In particular, the assessment of advanced fuel cycles requires an extensive knowledge of transuranics cross sections. Plutonium isotopes, but also americium, curium and up to californium isotope data are required with a small uncertainty in order to optimize significant features of the fuel cycle that have an impact on feasibility studies (e.g. neutron doses at fuel fabrication, decay heat in a repository, etc.). Different techniques are available to determine neutron cross sections experimentally, with the common denominator that a source of neutrons is necessary. It can either come from an accelerator that produces neutrons as a result of interactions between charged particles and a target, or it can come from a nuclear reactor. When the measurements are performed with an accelerator, they are referred to as differential since the analysis of the data provides the cross-sections for different discrete energies, i.e. σ(E i ), and for the diffusion cross sections for different discrete angles. Another approach is to irradiate a very pure sample in a test reactor such as the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The precise characterization of the nuclide densities before and after neutron irradiation allows to infer energy-integrated neutron cross sections, i.e. ∫₀ ∞ σ(E)φ(E)dE, where φ(E) is the neutron flux “seen” by the sample. This approach, which is usually defined and led by reactor physicists, is referred to as integral and is the object of this report. These two sources of information, i.e. differential and integral, are complementary and are used by the nuclear physicists in charge of producing the evaluated nuclear data files used by the nuclear community (ENDF, JEFF…). The generation of accurate nuclear data files requires an iterative process involving reactor physicists and nuclear data evaluators. This experimental program has been funded by the ATR National Scientific User Facility (ATR-NSUF) and by the DOE Office of Science in the framework of the Recovery Act. It has been given the name MANTRA for Measurement of Actinides Neutron TRAnsmutation.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Initial Testing of the Microscopic Depletion Implementation in the MAMMOTH Reactor Physics Application

Present and new nuclear fuels that will be tested at the Transient Reactor Test (TREAT) facility will be analyzed with the MAMMOTH reactor physics application, currently under development, at Idaho National Laboratory. MAMMOTH natively couples the BISON, RELAP-7, and Rattlesnake applications within the MOOSE framework. This system allows the irradiation of fuel from beginning of life in a nuclear reactor until it is placed in TREAT for fuel testing within the same analysis mesh and, thus, retaining a very high level of resolution and fidelity. The calculation of the isotopic distribution in fuel requires the solution to the decay and transmutation equations coupled to the neutron transport equation. The Chebyshev Rational Approximation Method (CRAM) is the current state-of-the-art in the field, as was chosen to be the solver for the decay and transmutation equations. This report shows that the implementation of the CRAM solver within MAMMOTH is correct with various analytic benchmarks for decay and transmutation of nuclides. The results indicate that the solutions with CRAM order 16 achieve the level of precision of the benchmark. The CRAM solutions show little sensitivity to the time step size and consistently produce a high level of accuracy for isotopic decay for time steps of 1x10^11 years. Comparisons to DRAGON5 with 297 isotopes yield comparable results, but some differences need to be further analyzed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Architecture for the Performance of Nuclear Fuel Depletion Calculations

Computational analysis of the depletion of nuclear fuel is crucial to the accurate modeling of the time-dependent behavior of nuclear reactors. The reactor physics application MAMMOTH is modified to compute radioactive decay and neutron transmutation in order to model physical processes which occur within nuclear reactors as reactor fuel is burned. The ability to read decay and cross-section data files of other codes are also added and the addition of a standardized decay and transmutation XML file format for MAMMOTH, known as ISOXML. Comparisons between MAMMOTH and the Oak Ridge Isotope Generation (ORIGEN) code are performed to demonstrate the improved precision possible with MAMMOTH. In addition, several tests are run to demonstrate the ability of MAMMOTH to model decay and transmutation processes involving hundreds of isotopes. Future work will focus on solving depletion problems with multiple neutron energy groups and the implementation of predictor-corrector methods, several of which are described in this work.

07 ISOTOPE AND RADIATION SOURCES↗