Cette thèse s’inscrit dans le cadre d’une collaboration entre le CEA et ORANO Mining, visant à améliorer la sensibilité et la précision des mesures radiométriques de l’uranium dans le cadre de l’exploration et de l’exploitation minières, notamment pour les échantillons de minerai. Dans un premier temps, les méthodes de mesure nucléaire pour la prospection de l’uranium actuellement utilisées sont présentées ainsi que leurs enjeux, avant d’exposer le développement des nouvelles méthodes de spectrométrie gamma qui font l’objet de ces travaux de thèse. Elles exploitent notamment le phénomène d’auto-fluorescence X de l’uranium, dont le signal n’est actuellement pas utilisé, pour réduire les temps de mesure et en améliorer la précision. L'auto-fluorescence X, est provoquée par les rayonnements gamma d'isotopes radioactifs présents dans le minerai, comme le 214Pb et 214Bi, créant par diffusion Compton un important continuum au-delà de la discontinuité d'absorption K de l'uranium à 115.6 keV. Il en résulte l'émission de raies X-K de fluorescence de l'uranium, autour de 100 keV, représentatives de la teneur en uranium sur une profondeur de plusieurs centimètres, ce qui est particulièrement intéressant pour la mesure des échantillons ou carottes de minerai. L'intensité de l'auto-fluorescence dépend de l'activité des isotopes radioactifs présents dans le minerai, qui peut être quantifiée par spectrométrie gamma classique via leurs raies caractéristiques, ainsi que de la densité et de la minéralogie du minerai. En plus de la teneur en uranium, il est possible de détecter une hétérogénéité, par exemple une pépite d’uranium, en comparant les teneurs déduites de la raie d’émission passive du 234Th à 92 keV et de la raie XKα1 de fluorescence de l’uranium à 98 keV. Ces premières approches par spectrométrie gamma haute résolution avec un détecteur au germanium hyper pur ont fait l’objet d’une mise au point par simulation numérique avec le code MCNP et d’une qualification expérimentale avec des spectres gamma acquis par ORANO, puis au Laboratoire de Mesures Nucléaires du CEA Cadarache avec des échantillons de minerai réels. La méthode a aussi fait l’objet d’un dépôt de demande de brevet. La thèse étudie ensuite la possibilité de caractériser la teneur en uranium et de détecter des déséquilibres potentiels avec ses descendants, comme les isotopes 214Pb et 214Bi qui sont les principaux contributeurs au signal total, par spectrométrie gamma basse résolution avec un scintillateur NaI(Tl). Une approche par analyse de zones d'énergie du spectre gamma est développée par simulation et qualifiée en laboratoire, qui a fait aussi l’objet d’une demande de brevet. Ces nouvelles approches ont débouché sur le lancement par ORANO Mining de l’industrialisation d’un nouveau dispositif de mesure d’échantillons, ainsi que d’une nouvelle sonde gamma pour les puits de forage. / This PhD thesis in the frame of CEA - ORANO Mining collaboration aimed at improving the sensitivity and precision of radiometric uranium measurements for mining exploration and exploitation, particularly for ore samples characterisation. Before explaining the development of new gamma spectrometry methods, a survey of nuclear measurement methods currently used in this field are presented as well as their limitations. The new proposed methods exploit uranium X-ray fluorescence in order to reduce measurement time and improve accuracy. Gamma radiation from radioactive isotopes of the natural uranium decay chain, such as 214Pb and 214Bi, create a large Compton scattering continuum beyond the K-absorption discontinuity at 115.6 keV, leading to X-ray fluorescence. Uranium fluorescence K lines, in the 100 keV region, are representative of the uranium concentration up to a depth of a few centimetres, which is particularly interesting for small samples and drill cores. The intensity of self-fluorescence depends on the activity of the radioactive isotopes present in the ore, which can be directly quantified by gamma spectrometry from their characteristic lines, and on the density and mineralogy of the ore. In addition to uranium content, it is possible to detect a heterogeneity, for instance a uranium nugget, by comparing the 234Th passive emission line at 92 keV and the uranium XKα1 fluorescence line at 98 keV. This high-resolution gamma spectrometry approach using a hyper-pure germanium detector has been developed by MCNP numerical simulation, and then experimentally qualified using existing gamma spectra acquired by ORANO as well as new ore sample measurements at CEA Cadarache Nuclear Measurement Laboratory. Beyond this patent pending method, the PhD thesis studies the characterization of uranium content and potential imbalances between uranium and its radioactive daughters, such as the main signal contributors 214Pb and 214Bi, by low-resolution gamma spectrometry with a NaI(Tl) scintillator. An approach based on the analysis of energy areas of the gamma spectrum has been developed by numerical simulation and experimentally qualified in the Nuclear Measurement Laboratory. This new method is also patent pending and the outcome of this PhD work is the ongoing industrialization, by ORANO Mining, of an in situ measurement system for samples, and of a new borehole gamma probe.

Dissertation

This project aims to improve research in gamma-ray spectroscopy by using advanced detector systems. These systems are designed to reduce interference inherent in gamma-ray spectroscopy by rejecting Compton scattering events from high-energy gamma-rays, as well as look at cascading decays of gamma-rays through gamma-gamma coincidence counting. By combining these methods, one is able to lower detection limits for many elements than would otherwise be possible. This work also takes advantage of neutron activation analysis, which allows stable elements to be analyzed by activating them with neutrons, causing them to become unstable and decay with radioactive signatures. By analyzing these signatures, one is able to detect trace levels of elements with relatively small samples sizes (< 1g) and in a nondestructive manner. / text

Gamma spectroscopy and gamma emission tomography are two non-destructive measurement techniques for assessing the performance of nuclear fuel which have been investigated in this thesis for existing and novel applications through theoretical studies and experimental demonstrations. For assessment of individual fuel rods using gamma spectroscopy, fuel assemblies are dismantled so that the fuel rods may be measured separately, which is time-consuming and may cause damage to the fuel. Gamma tomography is more seldom used, but its application on complete fuel assemblies would enable the assessment of individual fuel rods without the need to disassemble the fuel. Both techniques are based on recording gamma rays, emitted at characteristic energies from decaying radioactive products in the fuel. The feasibility of measuring short-lived fission gasses in the gas plenum of fuel rods with short cooling time was experimentally investigated. Based on the feasibility demonstration, a method was proposed and experimentally demonstrated for determining the fission gas release fraction of 133Xe in fuel rods with short cooling time. Additionally, a method for investigating the origin of released fission gasses based on the measured ratio of 133Xe/85Kr in the fuel rod gas plenum was demonstrated. These methods may be employed at research reactors, where fuel with short cooling time is available for measurement. A gamma emission tomography instrument has been designed, constructed and experimentally demonstrated on a Halden Reactor fuel assembly. Simulation studies showed that the instrument and the tomographic reconstruction methods employed may be useful for: identifying a leaking fuel rod in an assembly by its lack of fission gas content; reconstruction of the rod-wise fission product distributions in the fuel stack and plenum regions of the assembly; and determining the rod-wise fission gas release fractions. In the experimental demonstration, the rod-wise distributions of the fission products 137Cs and 85Kr in the fuel stack and plenum regions of the assembly were reconstructed, as well as the distributions of the activation products 60Co and 178mHf in the plenum region, revealing the plenum springs and tie rods, respectively. The reconstructed data was in the form of images, useful for qualitative assessment of the fuel.

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