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Chlorine is present as an impurity in the UO2 nuclear fuel. 35Cl is activated into 36Cl by thermal neutron capture. In case of interim storage or deep geological disposal of the spent fuel, this isotope is known to be able to contribute significantly to the instant release fraction because of its mobile behavior and its long half life (around 300000 years). It is therefore important to understand its migration behavior within the fuel rod. During reactor operation, chlorine diffusion can be due to thermally activated processes or can be favoured by irradiation defects induced by fission fragments or alpha decay. In order to decouple both phenomena, we performed two distinct experiments to study the effects of thermal annealing on the behaviour of chlorine on one hand and the effects of the irradiation with fission products on the other hand. During in reactor processes, part of the 36Cl may be displaced from its original position, due to recoil or to collisions with fission products. In order to study the behavior of the displaced chlorine, 37Cl has been implanted into sintered depleted UO2 pellets (mean grain size around 18 μm). The spatial distribution of the implanted and pristine chlorine has been analyzed by SIMS before and after treatment. Thermal annealing of 37Cl implanted UO2 pellets (implantation fluence of 1013 ions.cm−2) show that it is mobile from temperatures as low as 1273 K (Ea=4.3 eV). The irradiation with fission products (Iodine, E=63.5 MeV) performed at 300 and 510 K, shows that the diffusion of chlorine is enhanced and that a thermally activated contribution is preserved (Ea=0.1 eV). The diffusion coefficients measured at 1473 K and under fission product irradiation at 510 K are similar (D = 3.10-14 cm2.s−1). Considering in first approximation that the diffusion length L can be expressed as a function of the diffusion coefficient D and time t by : L=(Dt)1/2, the diffusion distance after 3 years is L=17 μm. It results that there is a great probability for the chlorine contained in the UO2 grains to have reached the grain boundaries after 3 years, in the core of the fuel rod as well as at its periphery. Moreover, diffusion and concentration of chlorine at grain boundaries has been evidenced using SIMS mapping. Our results indicate therefore, that, during reactor operation and after, the majority of 36Cl is likely to have moved to grain boundaries, rim and gap. This fraction might then significantly contribute to the rapid or instant release of chlorine. This could have important consequences for safety assessment.
This study aims at identifying the release mechanisms of helium in uranium dioxide. Two sets of polycrystalline UO2 sintered samples presenting different microstructures were implanted with 3He ions at concentrations in the region of 0.1 at.%. Changes in helium concentrations were monitored using two Nuclear Reaction Analysis (NRA) techniques based on the 3He(d,α)1H reaction. 3He release is measured in-situ during sample annealing at temperatures ranging between 700°C and 1000°C. Accurate helium depth profiles are generated after each annealing stage. Results that provide data for further understanding helium release mechanisms are discussed. It is found that helium diffusion appears to be enhanced above 900°C in the vicinity of grain boundaries possibly as a result of the presence of defects.
A distributed electron cyclotron resonance (DECR) plasma reactor powered by a microwave generator operating at 2.45 GHz (800 W) was used to deposit (t)a-C:H thin films at RT on <100> Si substrates RF biased within the range 25≤|V0|≤600 V.C2H2 was used as precursor. The plasma pressure was varied within the range 0.1≤P≤1.5 mtorr. The films were analysed using spectroscopic ellipsometry (SE) and Fourier transform infrared (FTIR) spectroscopy. The hydrogen content NH and the density of the films were determined from nuclear reaction analysis (NRA) using the resonance at 6.385 MeV of the reaction: 15N + 1H → 12C + 4He + γ. Positron annihilation spectroscopy was used to detect the porosity. The evolutions of NH as a function of the substrate ion current density n+ and as a function of V0 show that the hydrogen incorporation results from the competition between chemisorption and deposited energy density related effects. The increase of the hydrogen incorporation leads to a decrease in the film density and a lower deposition rate. The porosity of the films deposited at low pressure (∼0.1 mTorr) with V0= −80 V has been detected. The comparison between results of SRIM-2000 simulations and the evolution of NH as a function of V0 shows that the porosity and the hydrogen content are not correlated. The absorption of oxygen and nitrogen for the low density films has been detected from the observation of the 3250–4000 cm-1infra-red (IR) band.
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