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, Enthalpy increment in Nd 2 O 3 presented by Konings et al, p.27
, Solubility of rare-earths in uranium for temperatures of, pp.1273-1523
, (a) and (b) show on the extremes of the phase diagram to appreciate the low solubility of both metals [91]
, 29 1.17 Description of the U-Nd-O system made by Lambertson through the pseudo-binary diagram T vs UO 2 -Nd 2 O 3 [115]
, U-Nd-O phase diagram proposed by Wadier in [52] at 1123 K (850 ? C), p.31
, 32 1.21 XRD patterns for samples with different Nd concentration and hypostoichiometric O/M ratios [117]. All samples display a single solution except the sample U 15 Nd 85 O 1.61 , which shows a coexistence between the FCC structure and the Nd 2 O 3 hexagonal phase, and the hypo-stoichiometric U 1?y Nd y O 2?x phase, and (b) extract of the phase diagram of the (U,Nd,O) system at room temperature reported by Desgranges, p.33
, The picture on the left shows the reversible behavior of samples sintered at 1973 K and the picture on the right shows the non-reversible evolution of samples sintered at 1673 K, Isodensity maps of the HT-XRD measures reported by Dottavio et al. in [91] for samples doped with 28% Nd
, (a) Calculated U-Nd-O phase diagram from the model developed in [91] at room temperature showing the formation of two phases joined by the tie lines, and (b) pseudo-binary diagram in temperature, The yellow region stands for the miscibility gap and the blue line represents the tie line that the defines both FCC A and FCC B phase at the thermodynamic equilibrium, vol.35
, Calculated U-Nd-O ternary isotherm at 800 K from the model developed in [51]
, 37 1.27 Oxygen chemical potential for the U-Nd-O system for samples doped with 14% and 15.5% Nd (a), and 27% and 29.5% Nd at various temperatures [51]
, ) black and grey circles represent the FCC structure formed by both U and Pu cations [125], and dashed circles represent the anionic sublattice in form of a cube on U-Pu-O mixed oxides. (b) evolution of the lattice parameter for different concentrations of Pu on the U-Pu-O system published by Truphémus et al. in [56], p.40
, The dashed central region represents the transition region where the hypo-stoichiometric FCC structure becomes a BCC structure, Isotherm of the ternary diagram of the U-Pu-O system schematized in [Gunéneau, 2012.
, Grey symbols were acquired by Sari et al. and red symbols by Truphémus et al. [56, 126], vol.30
, Phase diagram of the system U-Ce-O described by Markin et al. in [43] showing the full extension of the miscibility gap at room temperature, vol.46
, Extract of the U-La-O ternary diagram at 1523 K on the sections UO 2 -U 3 O 8 -La 2 O 3 reported in [144]
, 50 1.35 Phase diagram of the U-Gd-O system at 1773 K reported by Lindemer and Sutton in [49], Phase diagram of the pseudobinary system UO 2+x -La, vol.2
, 56 2.2 SEM imaging and X-ray mapping for the samples doped with 4%Nd ((a) and (b)), 27%Nd ((c) and (d)) and 33%Nd ((e) and (f))
, 60 2.6 (a) illustrates the XRD patterns of two samples doped with 17%Nd through dry route and (b) presents a magnification of the framed region in red or blue to highlight the presence of the second crystallographic phase, FCC in sample 3 and hexagonal Nd 2 O 3 in sample 4 (black stars). 61 2.7 (a) presents the full XRD pattern of the sample doped with 27% Nd and (b) magnification of the pattern to highlight the presence of the cubic bixbyite C-Nd 2 O 3 (*), Figures (a) and (c) show the SAED corresponding to the green and orange circles and (b) TEM imaging of the sample doped with 33%. . 59 2.5 XRD patterns for the samples 1 and 2 doped with 4%Nd produced by dry route showing in both cases the presence of the FCC structure and a monophasic system
, 73 2.18 Oxygen chemical potentials for the samples doped with 17 and 25% Nd at 470 K and 670 K, respectively, p.73
, Evolution of the P O 2 in the furnace when the entering conditions of the gas vector are fixed at 10 ?27 atm and 923, Log(P O 2 ) vs O/M for the samples with 17% Nd (a) and 25%Nd (b) at, vol.74
, 76 2.22 (a) shows the evolution of the lattice parameter for all samples before and after thermal treatment, and (b) schematizes the shifting of the (1 1 1) peak for the sample doped with 25% to lower angles after the thermal treatment, vol.82
, Figure (a) and figure (b) schematize the Fourier transform of the asproduced samples (T0) and the samples treated thermally (TT), p.83
, 85 List of Figures 2.28 Distances of the first shell for all samples in comparison with the lattice parameter as a function of the concentration of Nd
, Calculation of the chemical potential as a function of the temperature for the sample doped with 25%Nd
, Selected XRD patterns of the sample doped with 25% at different times after the thermal treatment at high temperature, p.96
, 97 3.6 SEM imaging and Nd X-ray mapping of the sample after the high temperature thermal annealing. The sample remains single-phase and presents a uniform distribution of Nd
, , vol.100
, 107 3.14 HT-XRD patterns of the peak (3 1 1) for the sample doped with 20%Ce. The system remains monophasic as there is no evidence of a second crystallographic phase, The system follows Vegard's law, vol.106
, 110 3.17 HT-XRD patterns of the peak (2 0 2) for the sample doped with 45%Ce. Below T=473 K the system presents a second phase, p.111
, Extraction of the XRD pattern of the peak (2 0 2) along with the Rietveld refinement, showing a biphasic system at room temperature (a), and a monophasic system at 773 K (b) and at 1173 K (c), p.112
, 19 (a) evolution of the lattice parameter for each temperature on the sample doped with 45%Ce. (b), phase fraction of FCC 1 (red) and FCC 2 (black). The FCC 2 fraction decreases with decreasing temperatures, vol.113
, The orange section highlights the peaks (3 1 1) and (2 2 2), which will be discussed later in figure 3.21, Complete XRD patterns of the sample doped with 45%Ce
, 116 3.23 Representation of the miscibility gap in temperature on the system U-Ce-O for a sample doped with 45%. The green line stands for the evolution of the sample during the HT-XRD and the blue line for the thermal annealing at 1773 K, Evolution of the lattice parameter as a function of time of the sample doped with 45%Ce after the thermal annealing at 1773
, 126 4.2 Calculated oxygen chemical potentials for different temperatures and comparison with experimental data from [51] for a concentration of Nd of 5.5%Nd, Schematization of the regions where the interaction parameters are most relevant for the ternary phase diagram, vol.5, p.128
, Calculated oxygen chemical potentials at different temperatures for concentrations of Nd of 27, 29.5 and 30%, and comparison with experimental data from, p.129
, 6 (a) calculated isotherm at 300 K. (b) section of the isotherm at 300 K and comparison with experimental data from, vol.117, p.130
, isotherm at 1123 K. (b) section of the isotherm at 1123 K and comparison with experimental data from [52], p.130
, 8 (a) calculated isotherm at 1523 K. (b) section of the isotherm at 1523 K and comparison with experimental data from [116], p.131
, Site fractions of the sample doped with 4%Nd, p.132
, Site fractions of the sample doped with 17%Nd, p.133
, Site fractions of the sample doped with 25%Nd, p.133
, 167 1.1 Formation enthalpies, entropies and Gibbs free energies for the different uranium oxides at room temperature [37, 68], XAS spectra collected on this work at the U L 3, p.20
, types of transition and transition enthalpy and entropy for the different neodymium oxides, vol.36
, Coefficients of the polynomial expression of the heat capacity measured on temperature range of 298 K-1800 K [116], p.37
, Manufacturing processes and concentration ranges of the different authors that described the U-Pu-O phase diagram, vol.126, pp.128-131
, Manufacturing processes and concentration ranges of different authors that described the U-Ce-O phase diagram, p.45
, Manufacturing processes and concentration ranges of different authors that described the U-La-O phase diagram, vol.41, p.48
, Manufacturing processes and concentration ranges of different authors that described the U-Gd-O phase diagram, p.51
, 59 2.2 Results obtained by the Rietveld refinements for the three sintered samples
, 75 2.4 Calculated parameters obtained through the Rietveld refinement for all samples before and after the thermal treatment, p.77
, Position of the E 0 and the white line for each sample at the U M 4 -edge HERFD-XAS spectra
, Calculated concentration of U +4 , U +5 and U +6 for each sample after the linear combination fitting of the HERFD-XAS data, p.81
, 86 2.8 Results of the Nd L 3 -edge EXAFS refinements of samples with 17 and 25 %Nd, EXAFS refinements of all samples
, Theoretical and experimental concentration of U +4 , U +5 and U +6 when O/M=2, for the different ternary systems, p.89
,
, Oxygen self-diffusion parameters for stoichiometric UO 2, p.102
, Thermodynamic parameters used for the two models to describe the FCC phase [51, 91]
, The symbol "*" means all species, in this case it would include O ?2 and oxygen vacancies
, Parameters obtained after the assessment of the rhombohedral phase, vol.127
, Optimized thermodynamic parameter used on the different models to define the FCC phase [51, 91]
, Optimized thermodynamic parameter used on the different models to define the rhombohedral phase [183]