Actinide

Résumé

Les actinides sont une famille du tableau périodique comprenant les quinze éléments chimiques allant de l'actinium () au lawrencium (). Ces métaux lourds tirent leur nom de l'actinium, premier de la famille, en raison de leurs propriétés chimiques apparentées. On les désigne parfois sous le symbole chimique collectif An, qui représente alors n'importe quel actinide. Ce sont tous des éléments du bloc f, hormis le lawrencium, qui appartient au bloc d. Contrairement aux lanthanides, qui appartiennent également au bloc f, les actinides présentent un nombre de valence sensiblement plus variable. Ils ont tous un rayon atomique et un rayon ionique élevé, et leurs propriétés physiques sont particulièrement diverses. Ainsi, alors que les actinides de numéro atomique élevé se comportent chimiquement comme des lanthanides, ceux du début de la famille, allant du thorium au neptunium, ont une chimie évoquant par certains aspects celle des métaux de transition. Tous les actinides sont radioactifs

Source officielle

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

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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

The management of radioactive wastes from the nuclear fuel cycle has become an important issue in the development of future, more sustainable nuclear energy systems. Partitioning and transmutation (P&T) of actinides and some long-lived fission products could reduce the mass and radiotoxicity of highlevel wastes and possibly ease repository licensing requirements. Influenced by political and technological developments, an increasing number of countries employing nuclear power have become interested in P&T technology which involves the development of new types of critical and/or sub-critical reactors and very efficient fuel cycle strategies. The present thesis is closely connected to two P&T related projects of the OECD Nuclear Energy Agency in Paris, a numerical benchmark exercise for an accelerator-driven minor actinides burner and a calculational system study on the role of accelerator-driven systems (ADS) and advanced fast reactors (FR) in advanced nuclear fuel cycles. The author co-coordinated the benchmark exercise and performed the comparative analysis of the different "fuel cycle schemes" investigated in the system study. The benchmark exercise contributed to a greater understanding of the physical phenomena characteristic of the transmutation of actinides in a closed fuel cycle, and allowed to test and improve the tools used for modeling ADSs and corresponding advanced fuel cycles. This work thus effectively led to the development of an efficient and more complete calculational scheme, which has permitted an in-depth and reliable analysis of different transmutation scenarios to be carried out. To quantitatively assess the advantages and drawbacks of transmutation, we considered a limited number of "base" transmutation scenarios which constitute an envelope for various possible transmutation strategies employing fast spectrum systems. We then evaluated, for an equilibrium situation, the main aspects which characterise the different transmutation strategies, such as the nuclear park composition, the mass and toxicity of the waste, the need for natural uranium, the in-pile and out-pile mass inventories and, finally, the fuel cycle requirements. Thus, this study has allowed for the reliable comparison of performances of the three main options in the nuclear waste management, viz. open cycle, recycling of plutonium alone and recycling of all the actinides, as well as an evaluation of the advantages and disadvantages of ADSs in comparison to advanced critical reactors in the management of minor actinides or transuranics. The last part of the dissertation is dedicated to a phase-out study for two schemes employing either ADSs or critical reactors. It has been shown thereby that advanced systems, optimised for an equilibrium fuel composition, can indeed be used to reduce the inventory of transuranics. A comparison of ADS and FR performances has been made in this context, and the relative benefits of transmutation have been quantified in each case taking into consideration, more realistically, the residual mass inventory after the shutdown of all nuclear installations.

EPFL2003

Chargement

A Uranium-Based UO2+-Mn2+ Single-Chain Magnet Assembled trough Cation-Cation Interactions

Lucile Sylvie Danielle Chatelain, Marinella Mazzanti

Single-chain magnets (SCMs) are materials composed of magnetically isolated one-dimensional (1D) units exhibiting slow relaxation of magnetization. The occurrence of SCM behavior requires the fulfillment of stringent conditions for exchange and anisotropy interactions. Herein, we report the synthesis, the structure, and the magnetic characterization of the first actinide-containing SCM. The 5f-3d heterometallic 1D chains [[UO2(salen)(py)]M(py) 4]n, (M=Cd (1) and M=Mn (2); py=pyridine) are assembled trough cation-cation interaction from the reaction of the uranyl(V) complex [UO2(salen)py][Cp2Co] (Cp=pentamethylcyclopentadienyl) with Cd(NO3)2 or Mn(NO3)2 in pyridine. The infinite UMn chain displays a high relaxation barrier of 134±0.8 K (93±0.5 cm-1), probably as a result of strong intra-chain magnetic interactions combined with the high Ising anisotropy of the uranyl(V) dioxo group. It also exhibits an open magnetic hysteresis loop at T<6 K, with an impressive coercive field of 3.4 T at 2 K. Uranium in chains: 5f-3d heterometallic 1D chains are assembled from the reaction of pentavalent uranyl and CdII or MnII. The Mn-UO2-Mn coordination polymer exhibits slow relaxation of magnetization with a high relaxation barrier, and shows an open hysteresis cycle, thus affording the first example of an actinide-based single-chain magnet. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

2014

Chargement

Conceptual Design of a Sustainable Waste Burning Molten Salt Reactor

Boris Aviv Hombourger

EPFL2018

EPFL2003