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Euradwaste '08 - EU Bookshop - Europa

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The Cp * (T) curve were analysed in order to identify the different parameters controlling the latent<br />

heat effects of the defects. For each stage, the quantities to be derived are concentration and energy<br />

associated to the annealing of a certain kind of defect i.e. its characteristic mobility (i.e., preexponential<br />

factor and activation energy of the diffusion coefficient).<br />

Four peaks, corresponding to different defect annealing stages were identified from the analysis. A<br />

distinct physical significance was attributed to the various stages with increasing temperature:<br />

oxygen vacancy/interstitial recombination; uranium vacancy/interstitial cluster recombination (5.1<br />

eV); dislocation loop annealing; void growth (the void fractional volume was measured to about 0.3<br />

0.05 %; the resulting defect annealing energy of a vacancy trio is 13.4 eV).<br />

Heat Released, J g -1<br />

0,00<br />

-0,02<br />

-0,04<br />

-0,06<br />

-0,08<br />

-0,10<br />

-0,12<br />

-0,14<br />

400 600 800 1000 1200 1400<br />

Annealing Temperature, K<br />

Figure 2: Analysis of the heat release for (U0.9Pu0.1)O2<br />

3. Evolution of spent fuel in steam<br />

I<br />

II<br />

485<br />

III<br />

IV<br />

Fitting<br />

Experiment<br />

The aim of this study was to investigate the alteration of spent nuclear fuel (SNF) in a disposal vault<br />

under non-oxidising conditions (the behaviour of SNF under oxidizing conditions was investigated<br />

previously [10-13]). Potential alteration processes of the spent fuel during the transient phase corresponding<br />

to initial breach of the canister and first water ingress (early failure scenario) were investigated.<br />

This involved experiments in which fuel rod segments containing intentional defects in the<br />

cladding were exposed to a water-saturated atmosphere containing hydrogen to simulate nonoxidizing<br />

repository conditions. The effect of hydrogen overpressure on the corrosion behaviour of<br />

spent fuel in contact with groundwater was investigated by performing autoclave studies on irradiated<br />

fuel and analogues under conditions relevant for assessing different repository scenarios.<br />

The complete experimental equipment including an autoclave, an oven, a gas-sampling system and<br />

all the electrical connections was installed inside a hot cell during normal cell operation and<br />

adapted to remote handling by tele-manipulators. Three experiments were carried out at 90°C in<br />

humid atmosphere composed of, respectively, 1) pure Ar, 2) mixture of Ar and H2, and 3) pure H2.<br />

SEM investigations showed a significant surface change in the area of the intentionally set defect<br />

only under Ar. On both rodlets exposed to a moist hydrogen-containing atmosphere, no fuel surface<br />

alteration could be seen. Figure 3 shows SEM images of the surface exposed to different<br />

atmospheres.<br />

EDS analysis of the hydrogen-exposed surfaces showed, in addition to uranium, only the presence<br />

of fission products caesium and barium at the outer periphery of the fuel pellet, near the fuel<br />

cladding. Here also zirconium traces were found.

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