Fuels comprised of the element thorium have become increasingly popular with researchers and the public as the next generation fuel due to its ability to produce its own fissile element (U-233) and generate lower concentrations of heavy actinides. The use of thorium can possibly lead to a self-sustaining cycle whereby the addition of fissile material is not required and that the fuel can breed sufficient amounts of U-233 for a continuous supply. Research into thorium use in CANDU reactors has mainly been focused on using driver elements such as U-235 or Pu-239 to initiate the nuclear reaction by taking advantage of bundle design or by mixing the thorium and driver fuel together; however, these methods have added complexities and may not lead to a pure thorium fuel cycle, but extend the life of current nuclear fuels used. This thesis will investigate a simpler means of utilizing thorium for the intent of breeding U-233 through the use of pure thorium bundles in a once-through cycle by the ways of a heterogeneous core loading in a CANDU-6 reactor model. A 3x3 multi-cell model using DRAGON 3.06K will simulate the dual fuel model by having the centre lattice enclosing the thorium bundle and the outer eight lattices enclosing the enriched uranium bundles as the driver fuel. Next, the diffusion code DONJON 3.02E is used to produce time-average, instantaneous, and initial startup full-core simulations. As well, a brief look at the refuelling operations on the thorium channels will be done. The presence of a thorium bundle places a negative reactivity load on the multi-cell, but causes a positive insertion of reactivity for a coolant void and shutdown scenario. In the full-core modelling, the final core configuration chosen shows that thorium channels should be located in the inner core rather than in the most outer channels to produce a flattening effect on the radial profile. Thorium channels will require a combination of SEU and thorium bundles in an attempt to maintain channel power levels. Specifically, the use of 4, 6, or 8 Th bundles were investigated. The most optimal core performance shown has a radial form factor of 0.816, a total average core burnup of 18.32 GWd/t, and operates within designed power limits. It is possible to implement pure thorium bundles into a reactor set in a dual fuel mode. A careful consideration of where thorium bundles should be located in the core can help flatten the radial power distribution and help the reactor operate within the operating licensing parameters without the use of adjuster rods while breeding U-233 for a future thorium fuel cycle. / Thesis / Master of Applied Science (MASc)

Part B of two Project Reports; Part A can be found at: http://hdl.handle.net/11375/16881 / <p> Procedures have been set up to calculate the reactor kinetics parameters for thorium fuelled CANDU reactors using the perturbation option of the 2-dimensional diffusion code EXTERMINATOR. The procedures are believed to be very accurate. </p> <p> Representative cases of a CANDU thorium converter at different stages during the reactor life have been used to test the developed procedures. Results are presented and discussed. </p> / Thesis / Master of Engineering (ME)

<p>Thorium complexes primarily exist in the thermodynamically stable (IV) oxidation state with only a few low-valent thorium(III) and thorium(II) complexes having been isolated. As a result, redox chemistry with thorium at the metal center is synthetically challenging without carefully selected ligand systems. This redox-restricted nature of thorium(IV) makes redox-active ligands (RALs) an attractive option to facilitate multi-electron redox chemistry with thorium. In this work, first, a series of thorium(IV) complexes featuring the redox-active iminoquinone ligand and its derivatives, including the iminosemiquinone and amidophenolate species, were synthesized and characterized. Rare thorium oxygen multiple bonds were then accessed by exploiting the RALs on the thorium center and using dioxygen in dry air. Other oxidation chemistry was attempted with the thorium amidophenolate complexes as well. Second, armed with the knowledge of synthesizing multiple bonds with thorium(IV) complexes, similar chemistry was explored with cerium as it is in the same group as thorium. A series of cerium(III) and cerium(IV) complexes featuring the redox-active iminoquinone ligand and its derivatives were synthesized. Oxidation chemistry was explored with the cerium amidophenolate complexes and a rare cerium oxo was isolated. Finally, with interest in expanding and addressing a gap in the literature related to the synthesis, characterization, and utility of thorium alkyls, several tetrabenzylthorium complexes were synthesized, characterized, and some reactivity was explored. A highlight of this work involved the isolation of the first crystal structure of ligand and solvent free tetrabenzylthorium since its first synthesis in 1974. Full spectroscopic and structural characterization of the complexes was performed via ¹H NMR spectroscopy, X-ray crystallography, EPR spectroscopy, electronic absorption spectroscopy, and SQUID magnetometry, which all confirmed the identity and electronic structure of these complexes. </p>

<p>Due to the strong interest in thorium fuels in CANDU reactors rooting back to 1970’s and 1980’s, four experiments were done in the ZED-2 critical facility at Chalk River Laboratories to test the properties of (Th,Pu)O­₂ fuel. The fuel was placed in five bundles with a typical CANDU design, stacked vertically in the center of the core (K0 site) and surrounded by natural uranium fuel.</p> <p>The simulation of these experiments using the transport code DRAGON coupled with the diffusion code DONJON is presented. DRAGON is initially used to model two lattices and the full cores in 2D. These models are designed to calculate direct/adjoint flux, k_∞ and k_eff values using the collision probability method. Furthermore, the models determine a set of homogenized and condensed cross sections in two energy groups. Subsequently, DONJON is used to model the full core facility in three dimensions. Using the homogenized and condensed macroscopic cross section libraries obtained from the DRAGON models, DONJON is able to calculate the flux alongside with the k_eff values for the specific cases in two energy groups. The results are then compared to those from the experiments and will further validate the accuracy of the simulations.</p> <p>Sensitivity and uncertainty results for the infinite lattices and the 2D full core model using DRAGON and SUSD3D code are discussed. The direct and adjoint flux values determined by DRAGON for the lattices and the full core model are used by SUSD3D to calculate the sensitivity profiles for specific reactions of the isotopes present. The sensitivity profiles are then used alongside with the covariance matrices to calculate the uncertainty contribution of nuclear data to criticality. The sensitivity and uncertainty (S/U) results of the 2D model for full core, using the DRAGON/SUSD3D code coupling are then compared with the S/U results of a 3D model of the full core using the code TSUNAMI within the SCALE6 package in reference. The comparisons will show an excellent degree of consistency between the two methods, while reasons for possible differences in the results are also presented.</p> / Master of Applied Science (MASc)

<p>A study was conducted to scope the relative merits of various thorium fuel cycles in CANDU reactors. It was determined that, due to the very large reprocessing demands of the self-sustaining equilibrium thorium fuel cycle, an additional fissile driver fuel is required for a practical thorium fuel cycle. The driver fuels considered were PWR- and CANDU- derived plutonium, PWR-derived MOX fuel, and low-enriched uranium. The addition a RU-fuelled CANDU reactor with possible americium, curium, and lanthanides recycling was also considered. The fuel cycles were evaluated for natural uranium consumption and reprocessing demands as well as spent fuel characteristics such as: thermal and gamma power, radioactivity, and ingestion and inhalation hazards.</p> <p>The two-dimensional multigroup code, WIMS-AECL, was used to calculate the burnup and some controllability properties of the CANDU reactors. ORIGEN, a depletion and decay module, was used to evaluate the spent fuel characteristics and the systems code, DESAE, was used to simulate the introduction of the thorium fuel cycle to a growing global reactor park.</p> <p>It was determined that ²³³U production in the thorium fuels is optimized at lower exit burnups. Therefore, less external fissile driver material is required for the operation of the thorium reactors and natural uranium savings of the overall fuel cycle are increased. Furthermore, it was determined that driving the thorium fuel cycle with low-enriched uranium is the most efficient way to minimize natural uranium consumption. Assuming that a 40 MWd/kg exit burnup was achieved in the CANDU reactors, the fuel cycle yielded an 82% savings of natural uranium, compared to a scenario in which all power came from PWRs, while a 20 MWd/kg exit burnup increased the savings to 94%. The savings ranged over those exit burnups from 55%-69% for the variant with PWR-derived plutonium, 60%-73% for PWR-derived MOX fuel, and 78%-87% for CANDU-derived plutonium. The thermal power, radioactivity, and health hazards of the spent fuel were the highest for the case with MOX fuel driver but americium recycling proved effective for decreasing the long term dangers. In a global reactor park, the introduction of the thorium fuel cycle was hampered by the availability of fissile resources and, for a PWR-derived driver, natural uranium consumption was only reduced by 22% over 100 years relative to the PWR only scenario.</p> / Master of Applied Science (MASc)

Fuel comprised of thorium has been explored since the early development of nuclear energy in the 1960s. In the last decade, there has been a renewed interest in thorium fuel and it has now become a primary focus in studies and proposed in next-generation nuclear reactors. This has been prompted by a limited supply of uranium in the foreseeable future and an abundance of thorium resources. Additionally, when compared to natural uranium (NU), thoria (ThO$_2$) produces substantially less long-lived radioactive waste and the fissile content can be reprocessed for additional fuel cycles. The CANDU 6 reactor has a unique ability to harvest thorium fuels because of its superior neutron economy. Thorium requires a driving isotope to sustain neutron fission until the long absorption chain produces viable amounts of U-233. Previous studies have investigated many different practical fissile isotopes and core modeling techniques that would make thorium feasible in a CANDU 6 reactor. This thesis focuses on a safety evaluation of thorium fuel compared to NU fuel in a lattice cell and full core configuration. \\ DRAGON 3.06 and SERPENT 2 are used to examine the infinite lattice cell containing NU and homogeneous thorium fuel enriched with 2.0\% U-235, emphasizing the relationship between multiple nuclear libraries. This configuration is used to determine the enrichment concentration, temperature coefficient, coolant void reactivity, and the power relationship. Thorium fuel exhibits a higher negative temperature coefficient, a lower coolant void reactivity, and a greater reactivity change when simulated at different powers. If the lattice cell is simulated at 75\% nominal power there is an 11 mk adjustment for thorium fuel, whereas the adjustment is only three mk for NU fuel. This is related to the extensive cross section of Th-232 and the long fertile absorption chain results in a sizeable inventory of the intermediate isotope Pa-233. The fissile content of the fuel bundle after exiting the reactor will continue to accumulate U-233 and should be monitored and properly stored. \\ A full core evaluation in a CANDU 6 reactor is performed in DONJON 4. Thorium fuel has an inferior reactivity worth for the control mechanism than does NU fuel in an operating CANDU 6 reactor. The reactivity worth of leakage and absorption in the reactor is estimated to be slightly lower for the thorium fuel. \\ This thesis presents a new computational model for analyzing full core power transients built upon previous results. The approximation model utilizes many assumptions to develop an expeditious code for analyzing the infinite square lattice retaining the isotopic densities. This model has demonstrated the ability to accurately emulate the reactivity of a lattice cell at different powers and power transients formed in DRAGON. The model is coupled with a point kinetic code to perform power transients in a CANDU 6 reactor. \\ Load following operations are performed in cycles of 24 hours examined at 80\%, 60\%, and 40\% full power. Power adjustments are performed in increments of 10 minutes, two hour, or four hour periods with a constant reactivity input. The power adjustment time has minimal effect on the reactivity perturbations and only influences the rate of reactivity. Thorium fuel has enhanced load following capabilities compared to conventional NU fuel.\\ The long-lasting effects of Pa-233 introduces safety concern when reducing power or reactor shutdown scenarios. Reactivity transformation within the first two days of immediate power reduction will yield similar results for both fuels. Excess reactivity in the thorium fuel will continue to accumulate and eventually double the reactivity peak of NU fuel in the following 90 to 120 days. A shutdown simulation is performed in incremental power reduction steps of 20\% for a range of different days. It is found that NU fuel can adequately control the additional reactivity in this simulation. Thorium fuel maintains a disconcerting amount of excess reactivity that will need to be addressed accordingly. The protactinium transient highlights the need to adequately monitor the buildup of Pa-233 for thorium-based fuels in a reactor. / Thesis / Master of Applied Science (MASc)

La présence naturelle de la radioactivité dans les rejets des industries, notamment minières, soulève des enjeux en termes de gestion et de réutilisation. La teneur en radioéléments permet d’établir le potentiel radioactif, essentiel pour attester de leur innocuité, ouvrant ainsi des voies de valorisation. La quantification des principaux éléments des chaînes de désintégration du thorium et de l’uranium, principales causes naturelles de la radioactivité, permet de prédire le potentiel radioactif. Dans le cas des résidus miniers, les méthodes existantes de quantification ne sont pas toujours fiables, car l’incertitude analytique qu’elles engendrent ne permet pas toujours de statuer quant au respect des limites gouvernementales. Afin de pallier ce problème, il est nécessaire de développer des méthodes rapides, précises et robustes afin d’analyser adéquatement ces matrices complexes. L’objectif et l’innovation de cette thèse résident dans le développement d’une méthode unique combinant plusieurs résines de manière séquencée afin d’extraire sélectivement le thorium, l’uranium, le radium, le plomb et le polonium. L’individualisation des résines après le chargement de l’échantillon permet la séparation des analytes, soit les cinq éléments d’intérêt, dans des fractions distinctes. Leur séparation, notamment des éléments interférents, rend leur analyse possible sur des instruments sensibles, tels que la spectrométrie alpha ou la spectrométrie de masse couplée au plasma inductif. Afin de garantir la fiabilité de l’analyse, une attention particulière est également portée sur la mise en solution des analytes de manière totale. Ainsi, cette thèse propose un complément aux techniques actuelles, telle que la spectrométrie gamma, pour établir un diagnostic juste et précis de la radioactivité naturelle, que ce soit pour une application industrielle ou en institut de recherche. Pour accompagner le lecteur, une partie théorique sera consacrée aux propriétés physiques et chimiques des éléments d’intérêt. De même, l’ensemble des méthodologies permettant leur quantification sera détaillé afin de comprendre tous les tenants et aboutissants de cette thèse. / Natural radioactivity is ubiquitous and reported in industrial wastes, such as mining residues. Its presence raises the issue of the management and the sustainability of such wastes. The content in radioactive elements allows to establish the radioactive potential of the residues, necessary to demonstrate their safety for an eventual revalorization. The quantification of the main elements of the thorium and uranium decay series, mainly responsible of natural radioactivity, allows to predict the radioactive potential. In the case of mining residues, current methodologies are not always reliable due to analytical uncertainties, often flirting with governmental limitations. To overcome this issue, new methods must be developed to handle complex matrices as well as being fast, precise and robust. The aim of this thesis is to develop a unique innovative method that combine several sequential resins to selectively extract thorium, uranium, radium, lead and polonium. The targeted analyte can be recovered after selective elution on a single resin. The segregation of the elements from interfering elements originating from the matrix allows their precise measurement on instruments such as alpha spectrometry or inductively coupled plasma mass spectrometry. To ensure the reliability of the analysis, total sample dissolution techniques have also been investigated. This thesis brings a valuable complement to current techniques such as gamma spectrometry, to screen natural radioactivity with accuracy and precision. Thus, the proposed technique could be applied in both industrial support laboratories and research laboratories. To guide the reader, a theorical part dealing with the chemical and physical properties of elements of interest will be provided. In addition, standard methodologies on their quantification will also be detailed in order demonstrate the novelty of the work presented in this thesis.

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