Properties and recrystallization of radiation damaged pyrochlore and titanite
Notice bibliographique
Résumé
Radiation damage in minerals is caused by the alpha-decay of incorporated radionuclides, such as U and Th and their decay products. The effect of thermal annealing (400-1400 K) on radiation-damaged pyrochlores has been investigated by Raman scattering, X-ray powder diffraction (XRD), and combined differential scanning calorimetry/thermogravimetry (DSC/TG) (Zietlow et al., in print). The analysis of three natural radiation-damaged pyrochlore samples from Miass/Russia (6.4 wt% Th, 23.1·1018 α-decay events per gram (dpg)), Zlatoust/Russia (6.3 wt% Th, 23.1·1018 dpg), Panda Hill/Tanzania (1.6 wt% Th, 1.6·1018 dpg), and Blue River/Canada (10.5 wt% U, 115.4·1018 dpg), are compared with a crystalline reference pyrochlore from Schelingen (Germany). The type of structural recovery depends on the initial degree of radiation damage (Panda Hill 28 %, Blue River 85 %, Zlatoust and Miass 100 % according to XRD), as the recrystallization temperature increases with increasing degree of amorphization. Raman spectra indicate reordering on the local scale during annealing-induced recrystallization. As Raman modes around 800 cm-1 are sensitive to radiation damage (Vandenborre & Husson 1983, Moll et al. 2011), the degree of local order was deduced from the ratio of the integrated intensities of the sum of the Raman bands between 605 and 680 cm-1 devided by the sum of the integrated intensities of the bands between 810 and 860 cm-1. The most radiation damaged pyrochlores (Miass and Zlatoust) show an abrupt recovery of both, its short- (Raman) and long-range order (X-ray) between 800 and 850 K. The volume decrease upon recrystallization in Zlatoust pyrochlore was large enough to crack the sample repeatedly. In contrast, the weakly damaged pyrochlore (Panda Hill) begins to recover at considerably lower temperatures (near 500 K), extending over a temperature range of ca. 300 K, up to 800 K (Raman). The pyrochlore from Blue River shows in its initial state an amorphous x-ray diffraction pattern superimposed by weak Bragg-maxima that indicates the existence of ordered regions in a damaged matrix. Unlike the other studied pyrochlores, Raman spectra of the Blue River sample show the appearance of local modes above 560 K between 700 and 800 cm-1 resulting from its high content of U and Ta impurities. DSC measurements confirmed the observed structural recovery upon annealing. While the annealing-induced ordering of Panda Hill begins at a lower temperature (ca. 500 K) the recovery of the highly-damaged pyrochlore from Miass occurs at 800 K. The Blue-River pyrochlore shows a multi-step recovery which is similarly seen by XRD. Thermogravimetry showed a continuous mass loss on heating for all radiation-damaged pyrochlores (Panda Hill ca. 1%, Blue River ca. 1.5%, Miass ca. 2.9%). In order to elucidate local phenomena by NMR spectroscopy, a simpler structure of a metamict mineral such as titanite has been chosen. Hence, metamict titanite from Cardiff uranium mine (M28696) in Ontario, Canada, has been analysed using 29Si magic angle spinning nuclear magnetic resonance spectroscopy (MAS NMR) (Zietlow et al., 2014). A broad Gaussian shaped NMR signal at -81 ppm occurs at room temperature resulting from the mainly short range ordered metamict structural state. NMR signals were obtained at room temperature and after annealing at 600, 950, 1220 and 1470 K. Because of increasing crystallinity the full width at half maximum (FWHM) decreased from 24 ppm to 20 ppm respectively using a Pseudo-Voigt fit. For comparison well crystalline titanite from Rauris showed an NMR signal at -79.3 ppm with FWHM of 4.1 ppm and an almost Lorentzian profile because of its good long range order. Integrating synchrotron X-ray diffraction (XRD) signals of Cardiff titanite show an increase of the long range order at annealing temperatures considerably lower than the short range ordering seen by NMR.
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Comment cette classification a été obtenuedéplier
Prédiction distillée sur la base complète
Imitation des enseignantsNi prévalence calibrée, ni vérité terrain. Validation humaine à venir. Apprise à partir de 10 348 étiquettes directes de Codex et de 10 348 étiquettes directes de Gemma. Le mode candidate est l'union des têtes enseignantes seuillées; le consensus est leur intersection. Ces sorties portent le statut machine_predicted_unvalidated et ne sont ni des étiquettes humaines ni des étiquettes directes de modèles de pointe.
Scores Codex et Gemma par catégorie
| Catégorie | Codex | Gemma |
|---|---|---|
| Métarecherche | 0,000 | 0,000 |
| Méta-épidémiologie (sens strict) | 0,000 | 0,000 |
| Méta-épidémiologie (sens large) | 0,000 | 0,000 |
| Bibliométrie | 0,000 | 0,000 |
| Études des sciences et des technologies | 0,000 | 0,000 |
| Communication savante | 0,000 | 0,000 |
| Science ouverte | 0,000 | 0,000 |
| Intégrité de la recherche | 0,000 | 0,000 |
| Charge utile insuffisante (le modèle a refusé de juger) | 0,000 | 0,000 |
Scores machine (provisoires)
Les deux têtes enseignantes du modèle étudiant, lues sur ce travail. Un score ordonne la base pour la relecture; il n'affirme jamais une catégorie, et le statut de validation accompagne chaque rangée tel quel.
Scores de référence d'un modèle non mature (critères de maturité non atteints, 7 itérations). Un score ordonne; il n'affirme jamais une catégorie.
score_only:v0-immature-baseline · tel quel depuis la passe de notation : score_only signifie que le nombre peut ordonner les travaux, et qu'aucune étiquette de catégorie n'en découleClassification
machine, non validéePrédiction automatique; un appel candidat d’une seule tête enseignante, pas un consensus.
Le détail, modèle par modèle et score par score, se trouve en fin de page sous « Comment cette classification a été obtenue ».