Uranium

Résumé

L’uranium est l'élément chimique de numéro atomique 92, de symbole U. Il fait partie de la famille des actinides. L'uranium est le naturel le plus abondant dans la croûte terrestre, son abondance est supérieure à celle de l'argent, comparable à celle du molybdène ou de l'arsenic, mais quatre fois inférieure à celle du thorium. Il se trouve partout à l'état de traces, y compris dans l'eau de mer. C'est un métal lourd radioactif (émetteur alpha) de période très longue ( d'années pour l' et pour l'). Sa radioactivité, additionnée à celle de ses descendants dans sa chaîne de désintégration, développe une puissance de par tonne d'uranium, ce qui en fait, avec le thorium 232 (quatre fois plus abondant, mais trois fois moins radioactif) et le potassium 40, la principale source de chaleur qui tend à maintenir les hautes températures du manteau terrestre, en ralentissant de beaucoup son refroidissement. L'isotope U est le seul isotope fissile naturel. Sa fission libère une énergie voisi

Source officielle

https://fr.wikipedia.org/wiki/Uranium

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Chargement

Conceptual Design of a Sustainable Waste Burning Molten Salt Reactor

Boris Aviv Hombourger

For an energy source to qualify as sustainable, it must maximize the efficiency with which it uses natural resources while minimizing the amounts of waste it produces. Currently deployed nuclear power plants however use a very limited amount of the energy contained in natural nuclear fuels such as Uranium and Thorium and produce long-lived nuclear waste that must be dealt with. Molten Salt Reactors (MSRs) are one family of advanced reactors designs with the potential for safe and sustainable energy production due to their use of a liquid molten salt fuel. This thesis aimed at reviewing MSR designs that have been proposed in the past, investigating alternative design possibilities and proposing a concept capable of disposing of existing waste in a sustainable manner. One possibility to do so is to design a reactor to run on an isobreeding closed fuel cycle while using existing actinide waste as a start-up inventory, which is the route investigated in this thesis. For this purpose, the EQL0D fuel cycle procedure was developed using the MATLAB environment and the Serpent 2 Monte Carlo neutron transport code to simulate the start-up, transition and equilibrium of MSRs. The procedure was then applied to investigate the performance at equilibrium of several candidate fuel salts and moderators in an infinite lattice and in a closed Uranium-Plutonium and Thorium-Uranium fuel cycle. The results showed that only an isobreeding closed Uranium-Thorium fuel cycle can be achieved in moderated MSRs, while both isobreeding Uranium-Plutonium and Thorium-Uranium closed fuel cycles can be sustained in fast-spectrum MSRs, which additionally show a substantial reactivity margin that enable them to dispose of poorly fissile nuclides. The transition behavior of selected fluoride- and chloride-fueled reactors was then investigated. The fluoride-fueled cores all feature a closed Thorium-Uranium fuel cycle and included two historical graphite-moderated designs (the single- and two-fluid Molten Salt Breeder Reactors) and a modern fast-spectrum design (Molten Salt Fast Reactor). The chloride-fueled cores were proposed based on the results obtained in the infinite lattice study. The results obtained indicated that the transuranic-burning capabilities of fluoride-fueled reactors are substantially limited by the low solubility of transuranic trifluorides in fluoride salt mixtures, while no such limitation was found in chloride salts. On the other hand, chloride salts necessitate substantially larger cores and inventories. Finally, the possibility of operating MSRs on two types of open cycles without fuel processing, breed-and-burn and once-through, was investigated to alleviate concerns related to the uncertainties related to the technical feasibility of molten salt fuel processing in closed fuel cycles. The results obtained show that it is possible to operate chloride-fueled MSRs in a sustainable breed-and-burn fuel cycle and also on an open cycle with appreciable burn-ups achieved.

EPFL2018

Chargement

Small Molecule Activation by Multimetallic Uranium Complexes

Marta Falcone

The development of new processes for the selective and sustainable transformation of abundant small molecules constitutes one of the major research areas in inorganic and organometallic chemistry. These molecules as CO2, CO, N2 and H2 are abundant reservoirs of chemical energy, readily available sources of carbon, nitrogen and hydrogen. In a patent from 1909, Haber reported that uranium and uranium nitride were very efficient catalysts for ammonia synthesis. In order to perform multi-electron transfer, multimetallic complexes need to be designed. Reactivity of uranium bridging nitride remained unexplored since we investigated the nitride based reactivity of a dinuclear uranium(IV) bridging nitride complex towards small molecules such as CO2, yielding the first example of a uranium complex containing a bridging dicarbamate ligand, or CO, resulting in the complete cleavage in mild conditions of one of the strongest bonds in nature, or H2, yielding one of the few examples in f-elements of metal hydride, which is readily transferred to substrates such as CO2. Beyond the ligand based reactivity, we were interested in reducing the two metal centers to access a diuranium(III) bridging nitride, to pursue nitrogen activation. This complex was shown to have high flexibility, provided by the siloxide ligands, high reducing power and a bridging atom, the nitride, that holds together the uranium centers, with the possibility to bend upon nitrogen activation. This approach led us to the isolation of a hydrazido complex, resulting from the four-electron reduction of dinitrogen by the two metal centers. Moreover, complete cleavage of the NâN single bond was achieved by addition of CO to give two cyanate ligands or by addition of H2 to give ammonia. The nitride atom linker is nonetheless, too reactive to act as a spectator and it is involved in reactivity. Hence, we target the isolation of the analogue dinuclear U(III) complex with an oxide ligand as linker. This complex showed the same reactivity towards nitrogen but DFT revealed a more ionic character of the UâO bond nature with respect to the UâN bond, leading to different reactivity of the hydrazido fragment upon addition of CO and upon addition of H2, showing a smaller extent of activation in the oxo complex with respect to the nitride. The diuranium(III) bridging oxide complex showed interesting reactivity with H2, forming a bis-hydride complex capable of reducing CO2 beyond the formate level, to methanol.

EPFL2019

Chargement

Decades of uranium (U) mining, milling and military use left a legacy of U contamination around the world. The radioactivity and chemical toxicity of U at contaminated sites pose an acute and long-term hazard to human health and the surrounding environment. In order to diminish the risk, in situ bioremediation methods, which contribute to contaminant immobilization, are proposed. Nevertheless, the reported prevalent formation of labile and non-crystalline U(IV) species as a result of microbial U(VI) reduction, in contrast to more stable and crystalline uraninite, undermines the effectiveness of the applied bioremediation. Therefore, a holistic understanding of the controls and mechanisms that govern the formation of non-crystalline U(IV) in the environment is at the core of this thesis. Presence of common groundwater solutes (sulfate, silicate and phosphate) were shown to induce the production of bacterial extracellular polymeric substances (biofilm matrix components), which in turn increases the formation of non-crystalline U(IV) as a result of microbial U reduction. In contrast, a field study suggested that non-crystalline U(IV) was a product of abiotic U reduction followed by the sequestration of U(IV) ions by the biofilm matrix. Those contrasting theories, motivated us to look for an indicator capable of differentiating between biotic and abiotic U reduction in the environment. Uranium isotope fractionation proved to be an excellent tool. Based on our results, the isotopic signature of biotic U reduction (accumulation of 238U in the reduced phase) is easily distinguishable from the abiotic U reduction signature (either no isotopic fractionation or fractionation in the opposite direction). When contrasted with U isotope signatures recorded in the sediments, the findings of this study indicated that biological activity contributed to the formation of many ancient and modern U(IV) deposits. Equipped with a tool capable of assessing the origin of the U(IV) product, and with an understanding of the relationship between the biofilm matrix and the formation of non-crystalline U(IV), we embarked on a project to validate the mechanism responsible for non-crystalline U(IV) formation in the subsurface. Results show that regardless whether U is reduced enzymatically or though abiotic agents, the formed U(IV) species are always non-crystalline if the biofilm matrix is present. However, according to our experiments, biological U reduction resulted in better immobilization and overall reduction of U. The mechanism of U reduction in our systems was shown to be controlled by U speciation, which in turn, is govern by the presence of bicarbonate. Under low carbonate concentrations, the majority of U(VI) adsorbs onto the mineral phase thus promoting abiotic U reduction mediated by redox active minerals. However, at higher carbonate concentrations, most of U(VI) is present as aqueous U(VI)-carbonate complexes precluding sorption and thus allowing for enhanced enzymatic U reduction. The results obtained here shed light on the processes occurring at U-contaminated sites and have several field implications. The effectiveness of applied bioremediation was shown to depend on the geochemical conditions at the field site. However, the injection of bicarbonate during in situ clean-up operation enhances microbial U reduction and by this, the overall reductive immobilization of U.

EPFL2015

Chargement

Conceptual Design of a Sustainable Waste Burning Molten Salt Reactor

Boris Aviv Hombourger

EPFL2018

Small Molecule Activation by Multimetallic Uranium Complexes

Marta Falcone

EPFL2019

EPFL2015