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At least 163 records · Page 9

Neutron resonance transmission analysis prototype system for thorium fuel cycle safeguards

Emerging thorium-based reactor designs and fuel cycles present challenges to traditional non-destructive assay techniques used in international safeguards. Specifically, assaying the masses of 233 U and 235 U when they are present together in samples with high gamma ray backgrounds is difficult because of similar passive neutron signatures and relatively weak gamma-ray emissions of 233 U. The Pacific Northwest National Laboratory (PNNL) and the Massachusetts Institute of Technology (MIT) are developing a compact neutron resonance transmission analysis (NRTA) system as one potential solution to these challenges. The NRTA technique provides isotopic information for a sample via neutron time-of-flight (TOF) measurements that exploit a sample’s epithermal neutron resonance cross-sections. A recently developed portable NRTA system uses a commercially available, pulsed deuterium-tritium neutron generator with a ~2 m flight path and a GS20 lithium glass scintillator detector. Finally, this paper describes the prototype NRTA system design, a refined radiation transport model of the system, preliminary measurements with thorium and uranium sources, and demonstration of a quantitative isotopic estimation algorithm.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thorium nanochemistry: the solution structure of the Th(IV)-hydroxo pentamer

Tetravalent thorium exhibits a strong tendency towards hydrolysis and subsequent polymerization. Polymeric species play a crucial role in understanding thorium solution chemistry, since their presence causes apparent solubility several orders of magnitude higher than predicted by thermodynamic data bases. Although electrospray mass spectrometry (ESI MS) identifies Th(IV) dimers and pentamers unequivocally as dominant species close to the solubility limit, the molecular structure of Th 5 (OH) y polymers was hitherto unknown. In the present study, X-ray absorption fine structure (XAFS) spectroscopy, high energy X-ray scattering (HEXS) measurements, and quantum chemical calculations are combined to solve the pentamer structure. The most favourable structure is represented by two Th(IV) dimers linked by a central Th(IV) cation through hydroxide bridges.

36 MATERIALS SCIENCE↗

Preliminary design study of small long life boiling water reactor (BWR) with tight lattice thorium nitride fuel

Neutronic performance of small long-life boiling water reactors (BWR) with thorium nitride based fuel has been performed. A recent study conducted on BWR in tight lattice environments (with a lower moderator percentage) produces small power reactor which has some specifications, i.e. 10 years operation time, power density of 19.1 watt/cc and maximum excess reactivity of about 4%. This excess reactivity value is smaller than standard reactivity of conventional BWR. The use of hexagonal geometry on the fuel cell of BWR provides a substantial effect on the criticality of the reactor to obtain a longer operating time. Supported by a tight concept lattice where the volume fraction of the fuel is greater than the moderator and fuel, Thorium Nitride give good results for fuel cell design on small long life BWR. The excess reactivity of the reactor can be reduced with the addition of gadolinium as burnable poisons. Therefore the hexagonal tight lattice fuel cell design of small long life BWR that has a criticality more than 20 years of operating time has been obtained.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Advantages of liquid fluoride thorium reactor in comparison with light water reactor

Liquid Fluoride Thorium Reactor (LFTR) is an innovative design for the thermal breeder reactor that has important potential benefits over the traditional reactor design. LFTR is fluoride based liquid fuel, that use the thorium dissolved in salt mixture of lithium fluoride and beryllium fluoride. Therefore, LFTR technology is fundamentally different from the solid fuel technology currently in use. Although the traditional nuclear reactor technology has been proven, it has perceptual problems with safety and nuclear waste products. The aim of this paper is to discuss the potential advantages of LFTR in three aspects such as safety, fuel efficiency and nuclear waste as an alternative energy generator in the future. Comparisons between LFTR and Light Water Reactor (LWR), on general principles of fuel cycle, resource availability, radiotoxicity and nuclear weapon proliferation shall be elaborated.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Theoretical analysis of uranium-doped thorium dioxide: Introduction of a thoria force field with explicit polarization

Thorium dioxide is used industrially in high temperature applications, but more insight is needed into the behavior of the material as part of a mixed-oxide (MOX) nuclear fuel, incorporating uranium. We have developed a new interatomic potential model including polarizability via a shell model, and commensurate with a prominent existing UO{sub 2} potential, to conduct configurational analyses and to investigate the thermophysical properties of uranium-doped ThO{sub 2}. Using the GULP and Site Occupancy Disorder (SOD) computational codes, we have analyzed the distribution of low concentrations of uranium in the bulk material, where we have not observed the formation of uranium clusters or the dominance of a single preferred configuration. We have calculated thermophysical properties of pure thorium dioxide and Th{sub (1−x)}U{sub x}O{sub 2} which generated values in very good agreement with experimental data.

36 MATERIALS SCIENCE↗

Optimization of small long-life PWR based on thorium fuel

A conceptual design of small long-life Pressurized Water Reactor (PWR) using thorium fuel has been investigated in neutronic aspect. The cell-burn up calculations were performed by PIJ SRAC code using nuclear data library based on JENDL 3.2, while the multi-energy-group diffusion calculations were optimized in three-dimension X-Y-Z geometry of core by COREBN. The excess reactivity of thorium nitride with ZIRLO cladding is considered during 5 years of burnup without refueling. Optimization of 350 MWe long life PWR based on 5% {sup 233}U & 2.8% {sup 231}Pa, 6% {sup 233}U & 2.8% {sup 231}Pa and 7% {sup 233}U & 6% {sup 231}Pa give low excess reactivity.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Antineutrino monitoring of thorium reactors

Various groups have demonstrated that antineutrino monitoring can be successful in assessing the plutonium content in water-cooled nuclear reactors for nonproliferation applications. New reactor designs and concepts incorporate nontraditional fuel types and chemistry. Understanding how these properties affect the antineutrino emission from a reactor can extend the applicability of antineutrino monitoring. Thorium molten salt reactors breed 233 U, that if diverted constitute a direct use material as defined by the International Atomic Energy Agency (IAEA). The antineutrino spectrum from the fission of 233 U has been estimated for the first time, and the feasibility of detecting the diversion of 8 kg of 233 U, within a 30 day timeliness goal has been evaluated. The antineutrino emission from a thorium reactor operating under normal conditions is compared to a diversion scenario by evaluating the daily antineutrino count rate and the energy spectrum of the detected antineutrinos at a 25 m standoff. It was found that the diversion of a significant quantity of 233 U could not be detected within the current IAEA timeliness detection goal using either tests. In conclusion, a rate-time based analysis exceeded the timeliness goal by 23 days, while a spectral based analysis exceeds this goal by 31 days.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Hybrid fusion–fission reactor with a thorium blanket: Its potential in the fuel cycle of nuclear reactors

Discussions are currently going on as to whether it is suitable to employ thorium in the nuclear fuel cycle. This work demonstrates that the {sup 231}Pa–{sup 232}U–{sup 233}U–Th composition to be produced in the thorium blanket of a hybrid thermonuclear reactor (HTR) as a fuel for light-water reactors opens up the possibility of achieving high, up to 30% of heavy metals (HM), or even ultrahigh fuel burnup. This is because the above fuel composition is able to stabilize its neutron-multiplying properties in the process of high fuel burnup. In addition, it allows the nuclear fuel cycle (NFC) to be better protected against unauthorized proliferation of fissile materials owing to an unprecedentedly large fraction of {sup 232}U (several percent!) in the uranium bred from the Th blanket, which will substantially hamper the use of fissile materials in a closed NFC for purposes other than power production.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Determination of the Galaxy age by the method of uranium–thorium–plutonium isotopic ratios

The dependence of the Galaxy age (Т{sub G}), as determined by the method of uranium–thorium isotopic ratios, on the parameters of the nucleosynthesis model is studied within the theory of galactic nucleosynthesis. It is shown that ТG depends strongly both on the scenario of the production of nuclei in the r-process and those features of neutron-rich nuclei that are used in the respective analysis and on galactic-nucleosynthesis parameters. The effect of a sudden nucleosynthesis spike before the formation of a solar system on the Galaxy age is evaluated. The region of admissible values of the parameters of galacticnucleosynthesis theory is discussed. The method of uranium–thorium isotopic ratios is supplemented with the {sup 244}Pu/{sup 238}U ratio for yet another cosmochronometer pair, and the Galaxy age is estimated on the basis of the model modified in this way.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium–Uranium–Plutonium Fuel Cycle

It is shown for a closed thorium–uranium–plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain ~54 kg of fission products, ~0.8 kg of thorium, ~0.10 kg of uranium isotopes, ~0.005 kg of plutonium isotopes, ~0.002 kg of neptunium, and “trace” amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Trace Elemental Analysis of Bulk Thorium Using an Automated Separation–Inductively Coupled Plasma Optical Emission Spectroscopy Methodology

Presented here is a novel automated method for determining the trace element composition of bulk thorium by inductively coupled plasma–optical emission spectroscopy (ICP-OES). ICP-OES is a universal approach for measuring the trace elemental impurities present in actinide-rich materials; however, due to the emission rich spectrum of the actinide, a separation from the trace elements is warranted for spectrochemical analysis. Here, AG MP-1 ion exchange resin was utilized for retention of the Th matrix, while allowing the trace element impurities to be separated prior to subsequent analysis using ICP-OES. After demonstrating the separation on traditional gravity-driven columns, the methodology was transitioned to an automated platform for comparison. This automated platform utilizes syringe-driven sample and solvent flow and can collect the trace element and thorium fractions in separate locations. Finally, while reducing the sample size (500 µL, 1.5 mg of Th), maintaining the overall separation efficiency (recoveries >95%), and illustrating the sample throughput ability (n = 10+), this automated methodology could be readily adopted to nuclear facilities in which the determination of trace elemental impurities in Th samples is warranted.

47 OTHER INSTRUMENTATION↗

New NDA Methods for Thorium Fuel Cycle Safeguards (Final Report)

This project developed portable Neutron Resonance Transmission Analysis (pNRTA) as a new non-destructive assay (NDA) method for thorium fuel cycles safeguards and other applications where multiple isotopes must be measured when present together. pNRTA leverages epithermal neutron resonances to assay multiple safeguards-relevant isotopes (e.g., 233 U and 235 U) when they are present together in a sample. Existing techniques are challenged by this task, driving the need for new active interrogation methods. With selected detectors, pNRTA works in high gamma-ray backgrounds from fission and activation products and 232 U progeny expected in thorium fuel cycle samples. This project leveraged a pNRTA system developed at Pacific Northwest National Laboratory (PNNL) and collaboration with the Massachusetts Institute of Technology (MIT). The system uses a commercially available deuterium-tritium (DT) neutron generator at short standoff (2 m). Key achievements in this project included: first-of-a-kind pNRTA quantitative measurements of 233 U oxide samples, an assessment of neutron detector technologies suitable for pNRTA in high gamma-ray background environments, experimentally demonstrating quantitative assay of samples containing 233 U and 235 U, and modeling studies showing the applicability of pNRTA to a wide range of material forms. Further, a custom algorithm was developed at MIT, which provided mean bias of 9% and relative standard deviation of 36% in assaying 233 U, 235 U, 238 U, and 232 Th content in eight measured samples. These outcomes form a solid technical basis for pNRTA as a new promising capability for international safeguards verification that is portable, non-destructive, quantitative, and isotopic specific.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

IMPACT OF URANIUM AND THORIUM ON HIGH TIO2 CONCENTRATION NUCLEAR WASTE GLASSES

This study focused on the potential impacts of the addition of Crystalline Silicotitanate (CST) and Monosodium Titanate (MST) from the Small Column Ion Exchange (SCIX) process on the Defense Waste Processing Facility (DWPF) glass waste form and the applicability of the DWPF process control models. MST from the Salt Waste Processing Facility (SWPF) is also considered in the study. The KT08-series of glasses was designed to evaluate any impacts of the inclusion of uranium and thorium in glasses containing the SCIX components. All but one of the study glasses were found to be amorphous by X-ray diffraction (XRD). One of the slowly cooled glasses contained a small amount of trevorite, which is typically found in DWPF-type glasses and had no practical impact on the durability of the glass. The measured Product Consistency Test (PCT) responses for the study glasses and the viscosities of the glasses were well predicted by the current DWPF models. No unexpected issues were encountered when uranium and thorium were added to the glasses with SCIX components.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

THE ATTRACTIVENESS OF MATERIAS ASSOCIATED WITH THORIUM-BASED NUCLEAR FUEL CYCLES FOR PHWRS

This paper reports the continued evaluation of the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with thorium based nuclear fuel cycles. Specifically, this paper examines a thorium fuel cycle in which a pressurized heavy water reactor (PHWR) is fueled with mixtures of natural uranium/233U/thorium. This paper uses a PHWR fueled with natural uranium as a base fuel cycle, and then compares material attractiveness of fuel cycles that use 233U/thorium salted with natural uranium. The results include the material attractiveness of fuel at beginning of life (BoL), end of life (EoL), and the number of fuel assemblies required to collect a bare critical mass of plutonium or uranium. This study indicates what is required to render the uranium as having low utility for use in nuclear weapons; in addition, this study estimates the increased number of assemblies required to accumulate a bare critical mass of plutonium that has a higher utility for use in nuclear weapons. This approach identifies that some fuel cycles may be easier to implement the International Atomic Energy Agency (IAEA) safeguards approach and have a more effective safeguards by design outcome. For this study, approximately one year of fuel is required to be reprocessed to obtain one bare critical mass of plutonium. Nevertheless, the result of this paper suggests that all spent fuel needs to be rigorously safeguarded and provided with high levels of physical protection. This study was performed at the request of the United States Department of Energy /National Nuclear Security Administration (DOE/NNSA). The methodology and key findings will be presented.

CANDU↗

Modeling CANDU-6 liquid zone controllers for effects of thorium-based fuels

We use the DRAGON code to model the CANDU-6 liquid zone controllers and evaluate the effects of thorium-based fuels on their incremental cross sections and reactivity worth. We optimize both the numerical quadrature and spatial discretization for 2D cell models in order to provide accurate fuel properties for 3D liquid zone controller supercell models. We propose a low computer cost parameterized pseudo-exact 3D cluster geometries modeling approach that avoids tracking issues on small external surfaces. This methodology provides consistent incremental cross sections and reactivity worths when the thickness of the buffer region is reduced. When compared with an approximate annular geometry representation of the fuel and coolant region, we observe that the cluster description of fuel bundles in the supercell models does not increase considerably the precision of the results while increasing substantially the CPU time. In addition, this comparison shows that it is imperative to finely describe the liquid zone controller geometry since it has a strong impact of the incremental cross sections. This paper also shows that liquid zone controller reactivity worth is greatly decreased in presence of thorium-based fuels compared to the reference natural uranium fuel, since the fission and the fast to thermal scattering incremental cross sections are higher for the new fuels. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Status of the Norwegian thorium light water reactor (LWR) fuel development and irradiation test program

Thorium based fuels offer several benefits compared to uranium based fuels and should thus be an attractive alternative to conventional fuel types. In order for thorium based fuel to be licensed for use in current LWRs, material properties must be well known for fresh as well as irradiated fuel, and accurate prediction of fuel behavior must be possible to make for both normal operation and transient scenarios. Important parameters are known for fresh material but the behaviour of the fuel under irradiation is unknown particularly for low Th content. The irradiation campaign aims to widen the experience base to irradiated (Th,Pu)O{sub 2} fuel and (Th,U)O{sub 2} with low Th content and to confirm existing data for fresh fuel. The assumptions with respect to improved in-core fuel performance are confirmed by our preliminary irradiation test results, and our fuel manufacture trials so far indicate that both (Th,U)O{sub 2} and (Th,Pu)O{sub 2} fuels can be fabricated with existing technologies, which are possible to upscale to commercial volumes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Parametric analyses of single-zone thorium-fueled molten salt reactor fuel cycle options

Analyses of fuel cycle options based on thorium-fueled Molten Salt Reactors (MSRs) have been performed in support of fuel cycle screening and evaluation activities for the United States Department of Energy. The MSR options considered are based on thermal spectrum MSRs with 3 different separations levels: full recycling, limited recycling, and 'once-through' operation without active separations. A single-fluid, single-zone 2250 MWth (1000 MWe) MSR concept consisting of a fuel-bearing molten salt with graphite moderator and reflectors was used as the basis for this study. Radiation transport and isotopic depletion calculations were performed using SCALE 6.1 with ENDF/B-VII nuclear data. New methodology developed at Oak Ridge National Laboratory (ORNL) enables MSR analysis using SCALE, modeling material feed and removal by taking user-specified parameters and performing multiple SCALE/TRITON simulations to determine the resulting equilibrium operating conditions. Parametric analyses examined the sensitivity of the performance of a thorium MSR to variations in the separations efficiency for protactinium and fission products. Results indicate that self-sustained operation is possible with full or limited recycling but once-through operation would require an external neutron source. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗