Euradwaste '08 - EU Bookshop - Europa

Euradwaste '08 - EU Bookshop - Europa Euradwaste '08 - EU Bookshop - Europa

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elease falls typically between 1 and 2 % for all these species except Ba; the highest value for the fraction released was determined for Cs (2.3%). These values are generally lower than labile inventory values reported in literature from tests on UO2 including also gap contributions. They are in satisfactory agreement with the data reported specifically for grain boundary inventory of low to medium burnup UO2 [9]. In parallel, measurements of the species effusing from the fuel as a function of annealing temperature were performed using a Knudsen cell coupled to a mass spectrometer. The release measured at temperatures below the range where thermally activated transport dominates the fission gas release was attributed to release from surfaces and grain boundaries. The results from the two techniques showed good convergence and were in satisfactory agreement with data reported specifically for grain boundary inventory of low-medium burnup UO2. 2. Alpha decay damage evolution In order to predict the long term properties evolution of spent fuel, the effects of alpha-decay damage accumulation on spent fuel properties were investigated under accelerated alpha-decay rate conditions, using UO2 containing high activity alpha-emitters, the so-called alpha-doped UO2. Macroscopic and microstructural effects associated with the build-up of defects in the structure were studied. In particular, the correlation among annealing of defects in the microstructure, release behaviour of He, and energy stored by the defects in the material were evaluated. The limits of application of accelerated decay accumulation methods were also evaluated. The studies on alpha-doped UO2 have been performed on sol-gel producedsamples with a range of activities: from 10 wt% 233 U-doped UO2 (3.88·10 7 Bq.g -1 , with a damage level of ~ 10 -5 dpa) up to UO2 doped with 10 wt% 238 PuO2 with 3 dpa of damage, corresponding to standard irradiated UO2 fuel after 10000 years of storage. Alpha decay damage may lead to long term changes in the fuel microstructure and may further influence long term fuel leaching. A TEM analysis of the 233 U-doped UO2 has been performed, showing (Figure 1) numerous non-homogeneously distributed dislocation loops with sizes between 20 and 50 nm, indicating that the UO2 damage rapidly leads to precipitation of dislocation loops. Figure 1: TEM micrograph of 10 wt% 233 U-doped UO2 A Differential Scanning Calorimetry (DSC) study of 10 wt% 238 Pu-doped UO2 has also been performed (Figure 2). With this method the energy related to healing of lattice defects could be determined as a function of temperature, after correcting for the thermal effects due to self-irradiation in the material. 484

The Cp * (T) curve were analysed in order to identify the different parameters controlling the latent heat effects of the defects. For each stage, the quantities to be derived are concentration and energy associated to the annealing of a certain kind of defect i.e. its characteristic mobility (i.e., preexponential factor and activation energy of the diffusion coefficient). Four peaks, corresponding to different defect annealing stages were identified from the analysis. A distinct physical significance was attributed to the various stages with increasing temperature: oxygen vacancy/interstitial recombination; uranium vacancy/interstitial cluster recombination (5.1 eV); dislocation loop annealing; void growth (the void fractional volume was measured to about 0.3 0.05 %; the resulting defect annealing energy of a vacancy trio is 13.4 eV). Heat Released, J g -1 0,00 -0,02 -0,04 -0,06 -0,08 -0,10 -0,12 -0,14 400 600 800 1000 1200 1400 Annealing Temperature, K Figure 2: Analysis of the heat release for (U0.9Pu0.1)O2 3. Evolution of spent fuel in steam I II 485 III IV Fitting Experiment The aim of this study was to investigate the alteration of spent nuclear fuel (SNF) in a disposal vault under non-oxidising conditions (the behaviour of SNF under oxidizing conditions was investigated previously [10-13]). Potential alteration processes of the spent fuel during the transient phase corresponding to initial breach of the canister and first water ingress (early failure scenario) were investigated. This involved experiments in which fuel rod segments containing intentional defects in the cladding were exposed to a water-saturated atmosphere containing hydrogen to simulate nonoxidizing repository conditions. The effect of hydrogen overpressure on the corrosion behaviour of spent fuel in contact with groundwater was investigated by performing autoclave studies on irradiated fuel and analogues under conditions relevant for assessing different repository scenarios. The complete experimental equipment including an autoclave, an oven, a gas-sampling system and all the electrical connections was installed inside a hot cell during normal cell operation and adapted to remote handling by tele-manipulators. Three experiments were carried out at 90°C in humid atmosphere composed of, respectively, 1) pure Ar, 2) mixture of Ar and H2, and 3) pure H2. SEM investigations showed a significant surface change in the area of the intentionally set defect only under Ar. On both rodlets exposed to a moist hydrogen-containing atmosphere, no fuel surface alteration could be seen. Figure 3 shows SEM images of the surface exposed to different atmospheres. EDS analysis of the hydrogen-exposed surfaces showed, in addition to uranium, only the presence of fission products caesium and barium at the outer periphery of the fuel pellet, near the fuel cladding. Here also zirconium traces were found.

elease falls typically between 1 and 2 % for all these species except Ba; the highest value for the<br />

fraction released was determined for Cs (2.3%). These values are generally lower than labile<br />

inventory values reported in literature from tests on UO2 including also gap contributions. They are<br />

in satisfactory agreement with the data reported specifically for grain boundary inventory of low to<br />

medium burnup UO2 [9]. In parallel, measurements of the species effusing from the fuel as a function<br />

of annealing temperature were performed using a Knudsen cell coupled to a mass spectrometer.<br />

The release measured at temperatures below the range where thermally activated transport dominates<br />

the fission gas release was attributed to release from surfaces and grain boundaries. The results<br />

from the two techniques showed good convergence and were in satisfactory agreement with<br />

data reported specifically for grain boundary inventory of low-medium burnup UO2.<br />

2. Alpha decay damage evolution<br />

In order to predict the long term properties evolution of spent fuel, the effects of alpha-decay damage<br />

accumulation on spent fuel properties were investigated under accelerated alpha-decay rate conditions,<br />

using UO2 containing high activity alpha-emitters, the so-called alpha-doped UO2. Macroscopic<br />

and microstructural effects associated with the build-up of defects in the structure were studied.<br />

In particular, the correlation among annealing of defects in the microstructure, release behaviour<br />

of He, and energy stored by the defects in the material were evaluated. The limits of application<br />

of accelerated decay accumulation methods were also evaluated.<br />

The studies on alpha-doped UO2 have been performed on sol-gel producedsamples with a range of<br />

activities: from 10 wt% 233 U-doped UO2 (3.88·10 7 Bq.g -1 , with a damage level of ~ 10 -5 dpa) up to<br />

UO2 doped with 10 wt% 238 PuO2 with 3 dpa of damage, corresponding to standard irradiated UO2<br />

fuel after 10000 years of storage.<br />

Alpha decay damage may lead to long term changes in the fuel microstructure and may further influence<br />

long term fuel leaching. A TEM analysis of the 233 U-doped UO2 has been performed, showing<br />

(Figure 1) numerous non-homogeneously distributed dislocation loops with sizes between 20<br />

and 50 nm, indicating that the UO2 damage rapidly leads to precipitation of dislocation loops.<br />

Figure 1: TEM micrograph of 10 wt% 233 U-doped UO2<br />

A Differential Scanning Calorimetry (DSC) study of 10 wt% 238 Pu-doped UO2 has also been performed<br />

(Figure 2). With this method the energy related to healing of lattice defects could be determined<br />

as a function of temperature, after correcting for the thermal effects due to self-irradiation in<br />

the material.<br />

484

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