Bibliografie tematiche / Actinides – Structure

Letteratura scientifica selezionata sul tema "Actinides – Structure"

Autore: Grafiati

Pubblicato: 1 giugno 2024

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Articoli di riviste sul tema "Actinides – Structure":

Saha, Saumitra, e Udo Becker. "A first principles study of energetics and electronic structural responses of uranium-based coordination polymers to Np incorporation". Radiochimica Acta 106, n. 1 (26 gennaio 2018): 1–13. http://dx.doi.org/10.1515/ract-2016-2732.

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AbstractRecently developed coordination polymers (CPs) and metal organic frameworks (MOFs) may find applications in areas such as catalysis, hydrogen storage, and heavy metal immobilization. Research on the potential application of actinide-based CPs (An-CP/MOFs) is not as advanced as transition metal-based MOFs. In order to modify their structures necessary for optimizing thermodynamic and electronic properties, here, we described how a specific topology of a particular actinide-based CP or MOF responds to the incorporation of other actinides considering their diverse coordination chemistry associated with the multiple valence states and charge-balancing mechanisms. In this study, we apply a recently developed DFT-based method to determine the relative stability of transuranium incorporated CPs in comparison to their uranium counterpart considering both solid and aqueous state sources and sinks to understand the mechanism and energetics of charge-balanced Np5+incorporation into three uranium-based CPs. The calculated Np5++H+incorporation energies for these CPs range from 0.33 to 0.52 eV, depending on the organic linker, when using the solid oxide Np source Np2O5and U sink UO3. Incorporation energies of these CPs using aqueous sources and sinks increase to 2.85–3.14 eV. The thermodynamic and structural analysis in this study aides in determining, why certain MOF topologies and ligands are selective for some actinides and not for others. This means that once this method is extended across a variety of CPs with their respective linker molecules and different actinides, it can be used to identify certain CPs with certain organic ligands being specific for certain actinides. This information can be used to construct CPs for actinide separation. This is the first determination of the electronic structure (band structure, density of states) of these uranium- and transuranium-based CPs which may eventually lead to design CPs with certain optical or catalytic properties. While the reduction of the DFT-determined-bandgap goes from 3.1 eV to 2.4 eV when going from CP1 to CP3, showing the influence of the linker, Np6+incorporation reduces the bandgap for CP1 and CP3, while increasing it for CP2. The coupled substitution of U6+→Np5++H+reduces the bandgap significantly, but only for CP3.

Nadykto, B. A. "Electronic structure of actinides". Journal of Nuclear Science and Technology 39, sup3 (novembre 2002): 221–24. http://dx.doi.org/10.1080/00223131.2002.10875449.

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Laatiaoui, Mustapha, e Sebastian Raeder. "New Developments in the Production and Research of Actinide Elements". Atoms 10, n. 2 (8 giugno 2022): 61. http://dx.doi.org/10.3390/atoms10020061.

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This article briefly reviews topics related to actinide research discussed at the virtual workshop Atomic Structure of Actinides & Related Topics organized by the University of Mainz, the Helmholtz Institute Mainz, and the GSI Helmholtz Centre for Heavy Ion Research, Darmstadt, Germany, and held on the 26–28 May 2021. It includes references to recent theoretical and experimental work on atomic structure and related topics, such as element production, access to nuclear properties, trace analysis, and medical applications.

Kwon, Youngjin, Hee-Kyung Kim e Keunhong Jeong. "Assessment of Various Density Functional Theory Methods for Finding Accurate Structures of Actinide Complexes". Molecules 27, n. 5 (23 febbraio 2022): 1500. http://dx.doi.org/10.3390/molecules27051500.

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Density functional theory (DFT) is a widely used computational method for predicting the physical and chemical properties of metals and organometals. As the number of electrons and orbitals in an atom increases, DFT calculations for actinide complexes become more demanding due to increased complexity. Moreover, reasonable levels of theory for calculating the structures of actinide complexes are not extensively studied. In this study, 38 calculations, based on various combinations, were performed on molecules containing two representative actinides to determine the optimal combination for predicting the geometries of actinide complexes. Among the 38 calculations, four optimal combinations were identified and compared with experimental data. The optimal combinations were applied to a more complicated and practical actinide compound, the uranyl complex (UO2(2,2′-(1E,1′E)-(2,2-dimethylpropane-1,3-dyl)bis(azanylylidene)(CH3OH)), for further confirmation. The corresponding optimal calculation combination provides a reasonable level of theory for accurately optimizing the structure of actinide complexes using DFT.

Silva, Ricardo F., Jorge M. Sampaio, Pedro Amaro, Andreas Flörs, Gabriel Martínez-Pinedo e José P. Marques. "Structure Calculations in Nd III and U III Relevant for Kilonovae Modelling". Atoms 10, n. 1 (7 febbraio 2022): 18. http://dx.doi.org/10.3390/atoms10010018.

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The detection of gravitational waves and electromagnetic signals from the neutron star merger GW170817 has provided evidence that these astrophysical events are sites where the r-process nucleosynthesis operates. The electromagnetic signal, commonly known as kilonova, is powered by the radioactive decay of freshly synthesized nuclei. However, its luminosity, colour and spectra depend on the atomic opacities of the produced elements. In particular, opacities of lanthanides and actinides elements, due to their large density of bound–bound transitions, are fundamental. The current work focuses on atomic structure calculations for lanthanide and actinide ions, which are important in kilonovae modelling of ejecta spectra. Calculations for Nd III and U III, two representative rare-earth ions, were achieved. Our aim is to provide valuable insights for future opacity calculations for all heavy elements. We noticed that the opacity of U III is about an order of magnitude greater than the opacity of Nd III due to a higher density of levels in the case of the actinide.

Kovács, Attila. "Theoretical Study of Complexes of Tetravalent Actinides with DOTA". Symmetry 14, n. 11 (18 novembre 2022): 2451. http://dx.doi.org/10.3390/sym14112451.

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1,4,7,10-Tetraazacyclododecane-N,N′,N″,N‴-tetraacetic acid (H4DOTA) is a prominent chelating ligand with potential applications in various fields, from radiotherapy to the separation of fission products. The present study explores the stability, structure, and bonding properties of its complexes with tetravalent actinides (An = Th, U, Np, Pu) using density functional theory and relativistic multireference calculations. Neutral complexes prefer to form symmetric (C4) structures with DOTA. The first coordination sphere of the actinide ions is readily saturated by a weakly bonded H2O ligand. The latter ligand reduces the molecular symmetry while exerting only marginal effects on the properties of the parent complex. An-ligand bonding is mainly electrostatic, but there are also significant charge-transfer contributions from DOTA to the An 6d/5f orbitals. The charge-transfer interactions and the covalent character of bonding increase gradually in the order of Th < U < Np < Pu, as indicated by analysis of the electron density distribution using the Quantum Theory of Atoms in Molecules.

Bai, Li Jun, Ping Qian, Yao Wen Hu e Jiu Li Liu. "Atomistic Study on the Structure and Thermodynamic Properties of Afe₂al₁₀ (A = Th, U)". Advanced Materials Research 261-263 (maggio 2011): 735–39. http://dx.doi.org/10.4028/www.scientific.net/amr.261-263.735.

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An atomistic study is presented on the phase stability, interatomic distances and lattice parameters of the new actinide intermetallic compounds AFe2Al10(A = Th, U). Calculations are based on a series of interatomic pair potentials related to the actinides and transition metals, which are obtained by lattice inversion method. The cohesive energy of AFe2Al10with two possible structures of YbFe2Al10-type and ThMn12-type are calculated and compared with each other. Calculated lattice parameters of AFe2Al10are found to agree with reports in the literatures. In particular, the phonon densities of states, vibrational entropy and Debye temperature related to dynamic phenomena are evaluated for the first time.

Livshits, Tatiana, Sergey Yudintsev, Sergey V. Stefanovsky e Rodney Charles Ewing. "New Actinide Waste Forms with Pyrochlore and Garnet Structures". Advances in Science and Technology 73 (ottobre 2010): 142–47. http://dx.doi.org/10.4028/www.scientific.net/ast.73.142.

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Cubic oxides with pyrochlore and garnet structures are promising matrices for long-lived actinides immobilization. Their isomorphic capacity with respect to An and REE was determined. To predict the long-term behavior of these matrices under their underground disposal radiation stability of synthetic pyrochlores and garnets was studied. Most of titanate phases have the critical (amorphization) doses close to 0.2 displacements per atom at 298 K. This value is significantly higher for Sn- and Zr-rich pyrochlores. Corrosion behavior of the pyrochlore- and garnet-composed matrices was investigated. The lowest actinides leach rates were observed in water and alkaline solutions most typical for underground waste repositories. Amorphization of the phases has a low influence on their corrosion behavior in solutions. Possibility for joint incorporation of actinides and Tc into zirconate- and titanate-based matrices with the pyrochlore structure is discussed.

Block, Michael. "Direct mass measurements and ionization potential measurements of the actinides". Radiochimica Acta 107, n. 9-11 (25 settembre 2019): 821–31. http://dx.doi.org/10.1515/ract-2019-3143.

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Abstract The precise determination of atomic and nuclear properties such as masses, differential charge radii, nuclear spins, electromagnetic moments and the ionization potential of the actinides has been extended to the late actinides in recent years. In particular, laser spectroscopy and mass spectrometry have reached the region of heavy actinides that can only be produced only at accelerator facilities. The new results provide deeper insight into the impact of relativistic effects on the atomic structure and the evolution of nuclear shell effects around the deformed neutron shell closure at N = 152. All these experimental activities have also opened the door to extend such measurements to the transactinide elements in the near future. This contribution summarizes recent achievements in Penning trap mass spectrometry and laser spectroscopy of the late actinides and addresses future perspectives.

PETIT-MAIRE, D., J. PETIAU, G. CALAS e N. JACQUET-FRANCILLON. "LOCAL STRUCTURE AROUND ACTINIDES IN BOROSILICATE GLASSES". Le Journal de Physique Colloques 47, n. C8 (dicembre 1986): C8–849—C8–852. http://dx.doi.org/10.1051/jphyscol:19868163.

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Più fonti

Tesi sul tema "Actinides – Structure":

Hilaire, Sandrine. "Etude de la stabilisation des hauts degrés d'oxydation des actinides". Paris 11, 2005. http://www.theses.fr/2005PA112031.

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Les actinides du début de série, de l'uranium au curium, peuvent exister sous des degrés d'oxydation pouvant aller de +III jusqu'à +VII. Les propriétés des orbitales 5f permettent la formation d'un système de liaison où les oxygènes se placent en trans par rapport au métal en comparaison du placement en cis des pour les éléments d. En effet, elles sont accessibles en énergie et peuvent, faire parti des orbitales de valence. Dans la suite de la série, les orbitales 5f sont moins accessibles en énergie et la stabilité de la structure actinyle décroît. Dans le but d'étudier ce comportement, une étude des structures électronique et géométrique de composés actinyles combinée à une étude théorique a été effectuée : - une modélisation de la géométrie et des fréquences de vibration de composés du type AnO2L2n+(H2O)3 (An= U(VI) 5f0, Np(V) 5f2, Np(VI) 5f1 and Np(VII) 5f°, L=CI-, Br-, F-, CO32- and OH-) ont été effectués en utilisant des méthodes de DFT sur les logiciel Gaussian et ADF. Les occupations et les compositions orbitalaire ont été essentiellement étudiées ; - des complexes hydroxydes, carbonate et oxalate de Np(V) et Np(VI) ont été synthétisés afin d'être caractérisés électroniquement par des mesures vibrationnelles, de susceptibilité magnétique, de spectroscopie photoélectronique et Mössbauer ; - l'étude sur les complexes uranyles s'est focalisée sur les composés organométtaliques UO2Cl2(THF)3, UO2(OPPh3)4(Otf)2 et UO2(OTf)2 exhibant des liaisons au caractère plus covalent dans le plan équatorial
Early actinides (U, Np, Pu, Am) in a high oxidation state show a particular linear structure in bonding with pi-donor ligands (O, NR,. . . ). The diminution of the charge on the metallic centre due to the electronic donation from the equatorial and axial ligands allow the existence of high oxidation states for the light actinide. The particularity of the actinide stands in the fact that An 5f orbitals can take part in chemical bonding because of a partial delocalisation. In order to understand this behaviour, a study of the electronic and the geometric structure is undertaken using both theorical and experimental approaches : - Modelling of geometry and IR vibrational frequencies of compounds with formula AnO2L2n+(H2O)3 (An= U(VI) 5f0, Np(V) 5f2, Np(VI) 5f1 and Np(VII) 5f°, L=CI-, Br-, F-, CO32- and OH-) were performed by the density functional theory (DFT) using Gaussian and ADF software. Bond population and molecular orbitals composition were essentially studied. - Hydroxide, carbonate and oxalate of Neptunium (+V) and (+VI) were synthesized with the aim to study the electronic properties by different experimental way: magnetism susceptibility (SQUID), Mossbauer, XPS measurements and vibrationals spectroscopy's. - Uranium studies are focused on the water free compounds UO2Cl2(THF)3, UO2(OPPh3)4(Otf)2 and UO2(OTf)2, exhibiting more covalent bonds in the equatorial plane

O'Brien, Kieran. "Electronic structure and bonding in pyrrolic macrocycle-supported complexes of actinides". Thesis, University of Manchester, 2018. https://www.research.manchester.ac.uk/portal/en/theses/electronic-structure-and-bonding-in-pyrrolic-macrocyclesupported-complexes-of-actinides(9c8ab96e-0e0d-4cca-aaa2-ef30102fbcc2).html.

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Chemistry of the early actinides has undergone a lot of developments in recent years, and due to the need of specialised laboratories to handle these often highly radioactive complexes, computational chemistry has become a powerful aid in understanding the physical properties of these unique systems. This thesis describes a systematic computational study of organoactinide and organometallic model complexes of the form [LAnX]n+ where L is the macrocyclic trans- calix[2]benzene[2]pyrrolide ligand using density functional theory (DFT) in conjunction with a variety of partition-based methods â Mulliken populations analysis (MPA), Hirshfield population analysis (HPA), natural population analysis (NPA) and the quantum theory of atoms in molecules (QTAIM) â with the aim of probing the electronic structure of the An-X and An-arene bonds as a function of the X ligand. Natural bond orbital (NBO) analysis was also used to study the nature of the An-X bonds, with these results compared to the QTAIM descriptions of covalency and ionicity in the [LAnX]n+ complexes. Analogous transition metal complexes of the form [LMX]n+ (M = Hf, W) have also been studied with the QTAIM and NBO approaches to compare with the actinide-based systems. Nucleus independent chemical shift (NICS) analysis was carried out to probe the extent of aromaticity of the arene rings of the L2- ligand in the closed-shell [LThX]+ complexes as a function of X ligand, and was compared with QTAIM measurements of aromaticity. The MPA also revealed Î ́-bonding to the arene rings of the L2- ligand and was compared to the NICS data. Bond energies and bond energy decomposition analysis (EDA) of An-X were further analysed and compared to the QTAIM data. These same analyses were carried out on complexes where the X-type ligand series was extended to include a larger set of first and second-row p-block based ligands. Finally, other, bi-metallic actinide-based complexes including the L2-/4- ligand were studied with the aim of understanding the thermal stabilities of these experimentally-characterised complexes, with analogous model complexes modelled to find potential synthetic targets. The Kohn-Sham molecular orbitals (KS-MOs) of some of these complexes were also analysed to try and find a rationale, based on their electronic structure, for the energetic preference for one binding mode of L-An over another.

Ye, Gaoyang. "Thermodynamic and structural investigations on the interactions between actinides and phosphonate-based ligands". Thesis, Université Paris-Saclay (ComUE), 2018. http://www.theses.fr/2018SACLS286/document.

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En cas d’accidents nucléaires (Tchernobyl, Fukushima) ou d’exposition à de l'uranium appauvri dans des zones de conflit, la décontamination est nécessaire pour réduire au mieux les conséquences de l’ingestion de radionucléides. Après une contamination externe ou interne, les actinides solubilisées sont distribués dans les organes cibles (squelette, foie, tissus, reins, etc.) via la circulation sanguine. Compte tenu de cette dispersion, la chélation de ces radionucléides par des ligands biologiques est une méthode efficace de décorporation pour favoriser l'excrétion de ces métaux déposés et ainsi réduire les risques pour la santé. En raison du faible taux de distribution dans les organes cibles (os, foie, reins) de l'acide diéthylènetriaminepentaacétique (DTPA), des agents de chélation ont été synthétisés et testés in vitro ou in vivo. Dans ce projet, plusieurs ligands polyaminophosphonates, (conçus à l'origine pour être des agents de contraste), ont été synthétisés selon leurs propriétés de bio-distribution, de leurs groupes fonctionnels, de leur potentiel site de coordination et de leur lipophilie. Des études structurales et thermodynamiques ont ensuite été effectuées sur les complexes entre l'uranium (VI) et l’europium (III) (comme analogue de l’américium (III) et curium (III)) et les ligands polyaminophosphonates. La sphère de coordination de ces cations a été observée par spectroscopie UV-visible, TRLFS, FT-IR et la spectroscopie d’absorption X (EXAFS). L'étude de l’affinité a été réalisée par spectroscopie UV-visible. Enfin, les spectroscopies UV-visible et TRLFS ont été utilisées d’une part pour tester la stabilité du complexe ligand/uranyle en présence d’un ion métallique et d’autre part pour étudier le système ternaire : ion uranyle/ligand/calmoduline. Ces résultats ont permis de mieux comprendre les mécanismes de chélation et d’évaluer l'affinité chimique de ces ligands polyaminophosphonates pour l'uranium (VI) et l’europium (III). Cela devrait ainsi aider à la conception de nouveaux agents de chélation de plus en plus efficaces du point de vue de la décorporation
For exposed person who suffers from contamination from nuclear accidents (Chernobyl, Fukushima) or depleted uranium in war zones, decontamination is required to reduce the sequence damage of radionuclide intake. After an external or internal contamination, the solubilized actinides could be distributed to the target organs (skeletal, liver, kidneys tissues, etc.) via the bloodstream. Considering the dispersion, fate and health effect of the actinides, chelation therapy is an effective decorporation method to promote the excretion of deposited actinides to reduce the health risk. Due to the defect on weak distribution rate to the target organs (bone, liver, kidneys) of diethylenetriaminepentaacetic acid (DTPA) which currently used in clinics, plenty chelation agents were synthesized and tested in vitro or in vivo. In this project, several polyaminophosphonates ligands, a series ligand originally designed for MRI contrast and SPECT agents, were synthesized according to the properties of ligand bio-distribution, functional groups, coordination site and lipophilic. Then the structural and thermodynamic studies were done with the complexes between metal ion such as uranium(VI) and europium(III) (as americium/curium(III) analogue), and polyaminophosphonates ligands. The sphere of coordination of these cations was observed by UV-visible spectroscopy, TRLFS, FT-IR and Extended X-Ray Absorption Fine Structure (EXAFS). The affinity study was done with UV-visible spectroscopy. Finally, the UV-visible spectroscopy and TRLFS were used to test the stability of uranyl ligand complex with competition metal ion in biological conditions and to reveal the interactions between the ternary system, uranyl ion/ligand/calmodulin. These results allow to better understand the chemical affinity and possible chelation mechanism of the polyaminophosphonates ligands for the above actinides and therefore to promote the design of new chelation agents

Kervazo, Sophie. "Computational actinide chemistry : structure, bonding and thermodynamics". Thesis, Lille 1, 2018. http://www.theses.fr/2018LIL1R042/document.

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La question générale traitée dans cette thèse est de déterminer si, à l’heure actuelle, nous disposons d’outils théoriques efficaces pour décrire la structure, la liaison et les propriétés thermodynamiques de système comprenant un actinide. Cette large question va être abordée à l’aide de trois études différentes. Les deux premières sont directement liées à l’industrie plastique et à la sureté nucléaire. La dernière, plus fondamentale concerne une analyse comparative d’une approche théorique nouvellement développée sur des systèmes comprenant des éléments f. Tout d’abord, les cations alkyles contenant un actinide (Th, U) ou un métal de transition (Zr) coordonné à un arène se sont révélés efficaces pour la catalyse de la synthèse du polyéthylène. Étonnamment, les activités catalytiques des cations alkyles dépendent du solvant. Pour comprendre cela et confirmer la tendance qu’ont ces complexes à se lier à l’arène, une étude en DFT dans un contexte relativiste combinée à une caractérisation de liaison avec la méthode ETS-NOCV fut faite. La deuxième étude vise à étoffer les bases de données thermodynamiques qui servent à explorer numériquement les scénarios d’accidents. Notre étude in silico porte sur la détermination des enthalpies de formation des deux espèces pour lesquelles des incertitudes expérimentales subsistent (PuO3 ou PuO2(OH)2 …), en utilisant une méthode quantique multiconfigurationnelle et relativiste. La dernière partie de la théorie se concentre sur l’estimation de la précision de la fonctionnelle B2-PLYP pour les éléments f, qui s'avère assez précise en comparaison aux données expérimentales et à la méthode de référence CCSD(T)
The main question of this thesis is: do we have today the tools to efficiently describe the structure, the bonding and the thermodynamics of actinide systems? This broad question is answered thanks to three studies. The first two are directly applied to the plastic industry and the nuclear plant safety. The last one, more fundamental, concerns the benchmarking of newly developed theoretical approach on f-element systems.First, actinides and transition metal arene-coordinated alkyl cations have been recently proven to be efficient catalysts for ethylene polymerizations. Interestingly, thorium, uranium and zirconium alkyl cations’ catalytic activity depends on the solvent. To understand these behaviors and to confirm the tendency of these complexes to engage in unusual-arene coordination, relativistic DFT calculations combined with a characterization of the interaction thanks to the ETS-NOCV method are used. Second, in accident scenario along the reprocessing of spent nuclear fuel, plutonium can be released in various volatile forms (PuO2, PuO3 or PuO2(OH)2, …). The exploration of these scenarios by the use of simulations requires, among the various parameters, the knowledge of the thermodynamic properties of the possibly formed elements. Our in-silico study focusses on the determination of the enthalpies of formation of the former two species for which experimental uncertainties remain, using multi-configurational relativistic wavefunction method. The last part of the thesis focusses on the benchmark of the B2-PLYP functional for f-element systems, which turns out quite accurate with respect to the experimental data and the gold-standard CCSD(T) method

Gasnier, Estelle. "Etude structurale et propriétés des verres peralumineux de conditionnement des produits de fission et actinides mineurs"". Phd thesis, Université d'Orléans, 2013. http://tel.archives-ouvertes.fr/tel-00965076.

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Ce travail de thèse s'inscrit dans le cadre de la recherche de nouvelles formulations verrières pour le conditionnement des produits de fission et actinides mineurs (PFA). Il s'agit d'étudier une composition de verre dans le domaine peralumineux (défaut de compensateurs de charge en alcalins et alcalino-terreux par rapport à l'aluminium) présentant un taux de charge au moins équivalent à celui du verre R7T7 (18,5 % mass. PFA) et de statuer sur la potentialité de ces matrices vitreuses comme matrice de conditionnement. La première partie de cette étude évalue les propriétés physico-chimiques de verres peralumineux complexes en fonction de la teneur en PFA (de 18,5 à 32 % mass.) afin de vérifier leur adéquation avec le cahier des charges prédéfini. La très faible tendance à la cristallisation de ces matrices pour des teneurs en PFA allant jusqu'à 22,5 % massiques ainsi que l'excellente durabilité chimique observée jusqu'à présent sont des atouts indéniables. La seconde partie de l'étude apporte des informations sur l'incorporation des terres rares dans des verres de composition simplifiée du système SiO2-B2O3-Al2O3-Na2O-CaO-TR2O3 (TR=Nd ou La). L'homogénéité et la tendance à la dévitrification des verres sont étudiés à l'échelle micrométrique (DRX, MEB) et nanométrique (MET) et la spectroscopie RMN (MAS, MQMAS, REDOR, HMQC, DHMQC), combinée à la spectroscopie d'absorption optique du néodyme, se révèle un outil puissant pour mettre en évidence le rôle structural de la terre rare vis-à-vis de l'aluminium et décrire de façon précise l'organisation du réseau vitreux peralumineux. L'homogénéité des matrices sur une large gamme de composition et des données structurales inédites sur l'organisation du réseau vitreux à fortes teneurs en terres ont ainsi pu être mis en évidence.

Dodane, Catherine. "Dommages d'irradiation dans des céramiques de structure spinelle MGAl2O4 et ZNAl2O4- : application à la transmutation des déchets nucléaires". Paris 11, 2002. http://www.theses.fr/2002PA112013.

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Dans le cadre de la maîtrise des déchets nucléaires, une des voies de recherche est la transmutation des actinides mineurs en réacteur. Incorporer ces radioéléments dans une matrice céramique inerte est un des concepts proposés. Ce matériau support doit posséder une bonne tenue sous irradiation. Au cours de la transmutation, la principale source d'endommagement de la matrice étant les produits de fission, il convient d'étudier leurs effets en priorité. Nous avons irradié des spinelles MgAl2O4 (matrice de référence) et ZnAl2O4 par des ions rapides (par exemple : (86)Kr d'environ 400 MeV) simulant les produits de fission. Dans ces conditions, l'endommagement est essentiellement dû aux pertes d'énergie électroniques (Se). Une des caractéristiques de la structure spinelle AB2O4 est que les deux cations (A(2+) et B(3+)) peuvent échanger leur site. Ce phénomène est quantifié par le paramètre d'inversion. Nous mettons en évidence par DRX en incidence rasante que les changements structuraux observés dans MgAl2O4 correspondent à une transition ordre-désordre des sous-réseaux cationiques et non à un changement de phase comme décrit dans la littérature. A l'aide d'autres techniques caractérisant le groupe d'espace (spectroscopie Raman) ainsi que l'ordre local (RMN 27Al, spectroscopie d'absorption X aux seuils K de Al et Zn), nous confirmons cette interprétation. De plus, pour une fluence de 101̂4 ions/CM2̂, la perte de l'ordre à longue distance est observée traduisant ainsi un début d'amorphisation du matériau. Le spinelle ZnAl2O4 présente le même comportement. Pour ce dernier, une évolution du paramètre d'inversion en fonction du pouvoir d'arrêt Se, à la puissance 2 est mis en évidence après irradiation par des ions (86)Kr d'environ 20 MeV. Nous illustrons notre étude par l'analyse des résultats obtenus en DRX d'une irradiation en réacteur de combustibles composites (MgA12O4 + UO2) appelée THERMHET
The transmutation of minor actinides in-reactor is one solution currently being studied for the long time management of nuclear waste. In the heterogeneous concept the radionuclides are incorporating in an inert ceramic matrix. The support material must be insensitive to radiation damage. Fission product damage is the main radiation damage source during the transmutation process and therefore it is of the utmost importance to study their effects. We irradiated spinels MgA12O4 (matrix of reference) and ZnAl2O4 by fast ions (by example: (86)Kr of approximately 400MeV) simulating the fission products. Under these conditions, the damage is primarily due to the electronic energy losses (Se). One of the structural features of spinel AB2O4 is that the two cations (A(2+) and B(3+)) can exchange their site. This phenomenon is quantified by the inversion parameter. We highlight by XRD in grazing incidence that the structural changes observed in MgAl2O4 correspond to an order-disorder transition from the cation sub-networks and not to a phase shift as described in the literature. Using other techniques characterizing the space group (Raman spectroscopy) as well as the local order (NMR 27Al, spectroscopy of absorption X with the thresholds K of Al and Zn), we confirm this interpretation. Moreover, for a fluence of 101̂4 ions/cm2̂, the loss of the order at long distance is observed thus meaning a beginning of amorphization of material. The ZnA12O4 spinel presents the same behavior. For this last spinel, an evolution of the inversion parameter according to the stopping power to power 2 was highlighted after irradiation by ions (86)Kr from approximately 20MeV. We illustrate our study by the analysis of the results obtained in XRD of an irradiation out of composite fuel (MgAl2O4 + UO2) called THERMHET

Castro, Ludovic. "Étude théorique de la structure et de la réactivité de complexes de lanthanides et d'actinides : activation de petites molécules". Toulouse 3, 2012. http://thesesups.ups-tlse.fr/1706/.

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Cette thèse présente une étude théorique au niveau DFT de la structure et de la réactivité de complexes organométalliques de lanthanides et d'actinides. Après une introduction générale aux méthodes de chimie théorique employées pour traiter la réactivité de complexes organométalliques, une étude de la participation des électrons 5f dans la réactivité des complexes d'uranium(IV) est présentée. Il est montré qu'il est possible d'utiliser sans crainte des pseudopotentiels relativistes à grand cœur pour un certain nombre de problèmes de réactivité et qu'ainsi les électrons 5f peuvent être traités de manière implicite. Ensuite, la réactivité de complexes d'uranium(III) avec CO2 et autres molécules analogues est étudiée à travers plusieurs exemples issus de la littérature. Ces études montrent que la nature stérique des ligands impliqués est d'une importance capitale et contrôle la réactivité. Cette étude est étendue à un complexe de samarium(II). Enfin, la réactivité entre un complexe hydrure de cérium(III) et MeOSO2Me est étudiée et les résultats théoriques sont comparés aux observations expérimentales
This PhD thesis presents a theoretical study of the structure and the reactivity of organometallic complexes of lanthanides and actinides at the DFT level. After a general introduction of the methods of theoretical chemistry used for the modelling of organometallic reactivity, a study of the participation of 5f electrons in uranium(IV) reactivity is presented. The results show that the large core ECP can be used safely in order to treat the actinide and so that 5f electrons can be treated implicitly. Then, the reactivity of uranium(III) complexes with CO2 and other analogous molecules is studied via multiple examples from the literature. These studies show that the steric nature of the ligands is very important and controls the reactivity. This study is then extended to samarium(II) complex. Eventually, the reactivity of a hydride complex of cerium(III) with MeOSO2Me is investigated and theoretical results are compared with experimental observations

Lemonnier, Stéphane. "Synthèse par voie douce d'oxydes polymétalliques incluant des actinides : réactivité et structure de la solution au solide". Paris 6, 2006. http://www.theses.fr/2006PA066056.

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Lemonnier, Stéphane. "Synthèse par voie douce d'oxydes polymétalliques incluant des actinides : réactivité et structure de la solution au solide /". [Gif-sur-Yvette] : [CEA Saclay, Direction des systèmes d'information], 2007. http://catalogue.bnf.fr/ark:/12148/cb41067551t.

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Thèse de doctorat--Physique et chimie des matériaux--Paris 6, 2006.
La couv. et la p. de titre portent en plus : "Direction de l'énergie nucléaire" Bibliogr. p. 122-132. Résumé en français et en anglais.

Lutique, Stéphanie. "Etude de zirconates de structure pyrochlore en tant que matrice pour la transmutation ou le conditionnement des actinides mineurs". Paris 11, 2003. http://www.theses.fr/2003PA112080.

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La loi "Bataille" définit le cadre des études pour une gestion optimisée des déchets nucléaires, incluant la séparation des éléments les plus radiotoxiques pour les transmuter en élément moins radiotoxiques ou les stocker à long terme. Ces deux applications nécessitent l'utilisation d'une matrice répondant à plusieurs critères spécifiques. Ce travail effectué au cours de la thèse a pour but d'étudier une matrice potentielle pour la transmutation ou le stockage des actinides après leur séparation: le zirconate de type pyrochlore A2Zr2O7 (A est un lanthanide ou un actinide). Le développement d'un procédé de synthèse a conduit à la production de pastilles de zirconate de néodyme d'une densité de plus de 95 % de la densité théorique. La méthode d'infiltration de solution active dans un précurseur inactif a permis l'incorporation de plutonium et d'uranium et la production de pastilles denses de structure pyrochlore de type Nd(1,57)[Pu/U](0,43)Zr2O(7+y). A l'aide de trois techniques de calorimétrie, la capacité calorifique de zirconate de lanthanide à été déterminée dans l'intervalle de température 0,4 à 1400 K. La diffusivité thermique à été mesurée pour le zirconate de néodyme entre 400 et 1400 K et la conductivité thermique a été déduite. Une simulation numérique du comportement thermique sous irradiation d'un combustible à base de zirconate a été réalisée. La résistance à l'irradiation a été testée par implantation d'ions par accélérateur simulant les produits de fission et les noyaux de recul alpha. Enfin, après implantation d'ions d'hélium dans la matrice, le relâchement du gaz hélium a été contrôlé. Au vu de l'ensemble de ces résultats, il est apparu que les zirconates de type pyrochlore sont utilisables comme matrice pour la transmutation uniquement sous forme d'inclusions dans un composite. Une étude complémentaire du comportement de ce type de composé sous lixiviation est nécessaire pour apporter une conclusion quant à son usage comme matrice de conditionnement
The "Bataille" law gives orientations for nuclear waste management optimisation, which includes the partitioning of the most radiotoxic elements (the actinides and some fission products) in order to transmute them into less radiotoxic elements or to store for long term. For both applications a matrix with specific criteria is needed to incorporate the radionuclides. The aim of this work was the study of a potential matrix for the transmutation or the storage of actinides after their partitioning: pyrochlore zirconate, which general formula is A2Zr2O7, where A is a lanthanide or a actinide. A fabrication process was developed leading to the production of neodymium zirconate with a density higher than 95 % of the theoretical density. The method of infiltration of active solution in an inactive precursor permitted to incorporate plutonium and uranium and to produce highly dense pellet with pyrochlore structure and general formula Nd(1,57)[Pu/U](0,43)Zr2O(7+y). Using three calorimetric techniques, the lanthanide zirconate heat capacity was measured in the temperature range [0. 4 -1400 K]. The thermal diffusivity of the neodymium zirconate was determined between 400 and 1400 K and its thermal conductivity was deduced in the same temperature range, yielding to the constant value of 1,33 W. M^(-1). S^(-l). Using this value, the thermal behaviour of a zirconate based fuel was numerically simulated. The radiation resistance of the neodymium zirconate was tested using ion implanted with several energy by accelerator in order to simulate fission products and alpha recoil atoms. Finally He ions were implanted in the matrix and their release was monitored using a Knudsen cell. Basis on all those results, it appears that pyrochlore zirconates could be used as inert matrix for the transmutation only as inclusions in composites. However, a complementary study of the compound behaviour against leaching is needed before to be able to conclude concerning it use as waste form for actinides storage

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Libri sul tema "Actinides – Structure":

Flanders, David John. Structural studies of actinide compounds. [s.l.]: typescript, 1985.

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1927-, Kasuya T., a cura di. Physical properties of actinide and rare earth compounds: Search for heavy fermion characters. Tokyo, Japan: Publication Office, Japanese Journal of Applied Physics, 1993.

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Jr, Darby J. B., J. B. Darby e A. J. Freeman. Actinides: Electronic Structure and Related Properties. Elsevier Science & Technology Books, 2013.

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Freeman, A. J. Actinides: Electronic Structure and Related Properties. Elsevier Science & Technology Books, 2012.

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Manes, L. Actinides-Chemistry and Physical Properties (Structure and Bonding, Vol 59/60). Springer, 1985.

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Structural Chemistry of Inorganic Actinide Compounds. Elsevier, 2007. http://dx.doi.org/10.1016/b978-0-444-52111-8.x5000-5.

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Peter, Burns, Sergey Krivovichev e Ivan Tananaev. Structural Chemistry of Inorganic Actinide Compounds. Elsevier Science & Technology Books, 2006.

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(Editor), Sergey Krivovichev, Peter Burns (Editor) e Ivan Tananaev (Editor), a cura di. Structural Chemistry of Inorganic Actinide Compounds. Elsevier Science, 2006.

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Capitoli di libri sul tema "Actinides – Structure":

Papaconstantopoulos, Dimitris A. "Actinides". In Handbook of the Band Structure of Elemental Solids, 457–82. Boston, MA: Springer US, 2014. http://dx.doi.org/10.1007/978-1-4419-8264-3_14.

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Dudarev, S. L., D. Nguyen Manh e A. P. Sutton. "Electronic Structure and Structural Stability of Uranium Dioxide". In Actinides and the Environment, 113–20. Dordrecht: Springer Netherlands, 1998. http://dx.doi.org/10.1007/978-94-017-0615-5_7.

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Johansson, Börje. "Electronic Structure of the Actinide Elements". In Actinides and the Environment, 47–96. Dordrecht: Springer Netherlands, 1998. http://dx.doi.org/10.1007/978-94-017-0615-5_3.

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Salamakha, P. S., e O. L. Sologub. "Synthesis and Crystal Structure of New Quaternary Silicides of Uranium". In Actinides and the Environment, 121–24. Dordrecht: Springer Netherlands, 1998. http://dx.doi.org/10.1007/978-94-017-0615-5_8.

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Sorace, Lorenzo, e Dante Gatteschi. "Electronic Structure and Magnetic Properties of Lanthanide Molecular Complexes". In Lanthanides and Actinides in Molecular Magnetism, 1–26. Weinheim, Germany: Wiley-VCH Verlag GmbH & Co. KGaA, 2015. http://dx.doi.org/10.1002/9783527673476.ch1.

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Shields, Ashley E. "Advances in Structure Prediction of Lanthanides and Actinides with Genetic Algorithms". In Rare Earth Elements and Actinides: Progress in Computational Science Applications, 157–71. Washington, DC: American Chemical Society, 2021. http://dx.doi.org/10.1021/bk-2021-1388.ch007.

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Nguyen, Manh-Thuong, Jun Zhang, David C. Cantu, Roger Rousseau e Vassiliki-Alexandra Glezakou. "Tailored Computational Approaches to Interrogate Heavy Element Chemistry and Structure in Condensed Phase". In Rare Earth Elements and Actinides: Progress in Computational Science Applications, 219–45. Washington, DC: American Chemical Society, 2021. http://dx.doi.org/10.1021/bk-2021-1388.ch011.

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Papaconstantopoulos, Dimitrios A. "Actinide Hydrides". In Band Structure of Cubic Hydrides, 601–31. Cham: Springer International Publishing, 2023. http://dx.doi.org/10.1007/978-3-031-06878-2_16.

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Gutowski, Keith E., Nicholas J. Bridges e Robin D. Rogers. "Actinide Structural Chemistry". In The Chemistry of the Actinide and Transactinide Elements, 2380–523. Dordrecht: Springer Netherlands, 2010. http://dx.doi.org/10.1007/978-94-007-0211-0_22.

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Troć, R. "PuSe: X-ray Absorption Near Edge Structure (XANES)". In Actinide Monochalcogenides, 864–65. Berlin, Heidelberg: Springer Berlin Heidelberg, 2009. http://dx.doi.org/10.1007/978-3-540-47043-4_185.

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Atti di convegni sul tema "Actinides – Structure":

Delaroche, J. P. "Structure properties of even-even actinides". In FUSION06: Reaction Mechanisms and Nuclear Structure at the Coulomb Barrier. AIP, 2006. http://dx.doi.org/10.1063/1.2338412.

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MASLOV, V. M., YU V. PORODZINSKIJ, M. BABA e A. HASEGAWA. "COLLECTIVE LEVEL STRUCTURE OF EVEN-EVEN ACTINIDES". In Proceedings of the Eleventh International Symposium. WORLD SCIENTIFIC, 2003. http://dx.doi.org/10.1142/9789812795151_0110.

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Albers, R. C. "Actinide electronic structure and atomic forces". In Plutonium futures-The science (Topical conference on Plutonium and actinides). AIP, 2000. http://dx.doi.org/10.1063/1.1292349.

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GOUTTE, H., J. F. BERGER, J. P. DELAROCHE, M. GIROD, A. DOBROWOLSKI e J. LIBERT. "STRUCTURE AND FISSION PROPERTIES OF ACTINIDES WITH THE GOGNY FORCE". In Seminar on Fission VI. WORLD SCIENTIFIC, 2008. http://dx.doi.org/10.1142/9789812791061_0015.

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Haddi, Amine, François Farges, Patrick Trocellier, Enzo Curti, Messaoud Harfouche e Gordon E. Brown. "On the Coordination of Actinides and Fission Products in Silicate Glasses". In X-RAY ABSORPTION FINE STRUCTURE - XAFS13: 13th International Conference. AIP, 2007. http://dx.doi.org/10.1063/1.2644493.

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Bouchet, J. "New Pseudophase Structure for α-Pu". In PLUTONIUM FUTURES - THE SCIENCE: Third Topical Conference on Plutonium and Actinides. AIP, 2003. http://dx.doi.org/10.1063/1.1594578.

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Du, Yingzhe, Lili Li, Kunfeng Li, Peng Lin, Yugang Zhang e Juan Diwu. "Study on the Substitute Nuclides of Actinides in High-Level Radioactive Waste Liquid". In 2022 29th International Conference on Nuclear Engineering. American Society of Mechanical Engineers, 2022. http://dx.doi.org/10.1115/icone29-93771.

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Abstract (sommario):

Abstract Actinides have complex chemical properties, there are a variety of oxidation states and changeable coordination configurations, and their physical properties, electronic structure and molecular orbital theory are much more complex than other elements. On the other hand, actinides in high level liquid waste, especially transuranic elements synthesized by artificial nuclear reaction, are highly radioactive, which is critical for its stable glass solidification. At present, taking elements with similar properties as substitutes to simulate actinides and inferring the properties of actinides by analyzing the compounds formed by substitutes is one of the important works of glass solidification. This paper provides a possible way to use trivalent lanthanides as an alternative for trivalent actinides.

Demetriou, P., Th Keutgen, R. Prieels, Y. El Masri, Paraskevi Demetriou, Rauno Julin e Sotirios Harissopulos. "Proton-induced fission of actinides at energies 26.5 and 62.9 MeV—Theoretical interpretation". In FRONTIERS IN NUCLEAR STRUCTURE, ASTROPHYSICS, AND REACTIONS: FINUSTAR 3. AIP, 2011. http://dx.doi.org/10.1063/1.3628372.

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Butterfield, M. T. "Photoemission and Electronic Structure of UCoGa5 and PuCoGa5". In PLUTONIUM FUTURES - THE SCIENCE: Third Topical Conference on Plutonium and Actinides. AIP, 2003. http://dx.doi.org/10.1063/1.1594580.

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Guziewicz, E. "USb2 and PuSb2 Electronic Structure: A Photoemission Study". In PLUTONIUM FUTURES - THE SCIENCE: Third Topical Conference on Plutonium and Actinides. AIP, 2003. http://dx.doi.org/10.1063/1.1594585.

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Rapporti di organizzazioni sul tema "Actinides – Structure":

Marino, Maria, M. e Walter C. Ermler. Reliable Electronic Structure Calculations for Heavy Element Chemistry: Molecules Containing Actinides, Lanthanides, and Transition Metals. Office of Scientific and Technical Information (OSTI), gennaio 2006. http://dx.doi.org/10.2172/875418.

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Fast, L., e P. Soederlind. Crystal structure of actinide metals at high compression. Office of Scientific and Technical Information (OSTI), agosto 1995. http://dx.doi.org/10.2172/113969.

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Cort, B., T. H. Allen e A. C. Lawson. Structural and magnetic characterization of actinide materials. Office of Scientific and Technical Information (OSTI), dicembre 1998. http://dx.doi.org/10.2172/296813.

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Krishnan Balasubramanian. Electronic Structure of Transition Metal Clusters, Actinide Complexes and Their Reactivities. Office of Scientific and Technical Information (OSTI), luglio 2009. http://dx.doi.org/10.2172/959347.

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J. BERG, C. BURNS e ET AL. ACTINIDE MOLECULAR SCIENCE: F-ELECTRONIC STRUCTURE IN SYNTHESIS, SPECTROSCOPY, AND COMPUTATION. Office of Scientific and Technical Information (OSTI), novembre 2000. http://dx.doi.org/10.2172/772849.

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Schrell, Samantha K. Exploring the Actinide Series from Periodic Trends to Electronic Structure and Bonding. Office of Scientific and Technical Information (OSTI), ottobre 2018. http://dx.doi.org/10.2172/1477639.

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Gouder, T., e C. Colmenares. The effect of actinide thin films on the electronic structure and reactivity of various elements. Office of Scientific and Technical Information (OSTI), dicembre 1994. http://dx.doi.org/10.2172/86926.

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Wills, J. W., e O. Eriksson. Bulk and surface electronic structure of actinide, rare earth, and transition metal elements and compounds. Office of Scientific and Technical Information (OSTI), luglio 1996. http://dx.doi.org/10.2172/258186.

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Buesseler, K. O., M. Dai e D. J. Repeta. Speciation and structural characterization of Plutonium and Actinide-organic complexes in surface and ground waters (Sept. 1996-Sept. 1999) & Speciation, Mobility and Fate of Actinides in the Groundwater at the Hanford Site (Sept. 1999-Sept. 2002). Office of Scientific and Technical Information (OSTI), giugno 2000. http://dx.doi.org/10.2172/827049.

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Buesseler, K. O., M. Dai e D. J. Repeta. Speciation and structural characterization of Plutonium and Actinide-organic complexes in surface and ground waters. Office of Scientific and Technical Information (OSTI), giugno 1999. http://dx.doi.org/10.2172/827047.

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