Behaviour of implanted xenon in yttria-stabilised zirconia as inert matrix of a nuclear fuel

A zirconia-based fuel is studied for use of plutonium in light water reactors. Among the relevant properties for a nuclear fuel, efficient retention of fission products is required since the fuel matrix constitutes the first barrier against fission product release. To study the retention of xenon, its stopping power and its diffusion properties within (Er,Y,Pu,Zr)O2 potential inert matrix fuel (IMF) are investigated. Stopping and range of ions in matter (SRIM) calculations were carried out to estimate the average penetration depth of Xe ions as a function of their incident energy and of the material composition. To study its diffusion properties, Xe was implanted into yttria-stabilised zirconia (YSZ) to a depth of around 100 nm from the surface. After successive heat treatments to a maximum temperature of 1773 K, quantitative Xe depth profiles were determined by Rutherford backscattering. No profile modification by diffusion was observed. The behaviour of Xe is investigated at the subnanoscopic level and compared with the results obtained with zirconia samples implanted with Cs or I, as well as with Xe in UO2.

Inert matrix fuel for the utilisation of plutonium

Manuel Alexandre Pouchon

Utilising fuel resources responsibly, reducing waste volume and emissions as well as conflict potentials within the international community (non-proliferation, energy demand) are among the principles for the judgment of sustainable development. Utilising and burning plutonium in a light water reactor has been shown to be feasible for the disposition of the large amount of excess plutonium produced in today's power reactors and resulting from the disarmament efforts of the super powers. With regard to material technology aspects, efforts have concentrated on the evaluation of fabrication feasibility and on the determination of the physicochemical properties of a single phase zirconium/erbium/plutonium oxide material stabilised as a cubic solution by yttrium for plutonium and minor actinide incineration and transmutation. Due to the absence of uranium as origin for plutonium build-up, such a nuclear fuel is called Inert Matrix Fuel. Irradiation testing with a dedicated experiment in the material test reactor in Halden, Norway, is underway within the framework of the OECD-Halden Reactor Project.

Elsevier2001

Standardisation des outils de calcul pour les ADS et leur application à différents scénarios de transmutation des déchets

Marco Cometto

The management of radioactive wastes from the nuclear fuel cycle has become an important issue in the development of future, more sustainable nuclear energy systems. Partitioning and transmutation (P&T) of actinides and some long-lived fission products could reduce the mass and radiotoxicity of highlevel wastes and possibly ease repository licensing requirements. Influenced by political and technological developments, an increasing number of countries employing nuclear power have become interested in P&T technology which involves the development of new types of critical and/or sub-critical reactors and very efficient fuel cycle strategies. The present thesis is closely connected to two P&T related projects of the OECD Nuclear Energy Agency in Paris, a numerical benchmark exercise for an accelerator-driven minor actinides burner and a calculational system study on the role of accelerator-driven systems (ADS) and advanced fast reactors (FR) in advanced nuclear fuel cycles. The author co-coordinated the benchmark exercise and performed the comparative analysis of the different "fuel cycle schemes" investigated in the system study. The benchmark exercise contributed to a greater understanding of the physical phenomena characteristic of the transmutation of actinides in a closed fuel cycle, and allowed to test and improve the tools used for modeling ADSs and corresponding advanced fuel cycles. This work thus effectively led to the development of an efficient and more complete calculational scheme, which has permitted an in-depth and reliable analysis of different transmutation scenarios to be carried out. To quantitatively assess the advantages and drawbacks of transmutation, we considered a limited number of "base" transmutation scenarios which constitute an envelope for various possible transmutation strategies employing fast spectrum systems. We then evaluated, for an equilibrium situation, the main aspects which characterise the different transmutation strategies, such as the nuclear park composition, the mass and toxicity of the waste, the need for natural uranium, the in-pile and out-pile mass inventories and, finally, the fuel cycle requirements. Thus, this study has allowed for the reliable comparison of performances of the three main options in the nuclear waste management, viz. open cycle, recycling of plutonium alone and recycling of all the actinides, as well as an evaluation of the advantages and disadvantages of ADSs in comparison to advanced critical reactors in the management of minor actinides or transuranics. The last part of the dissertation is dedicated to a phase-out study for two schemes employing either ADSs or critical reactors. It has been shown thereby that advanced systems, optimised for an equilibrium fuel composition, can indeed be used to reduce the inventory of transuranics. A comparison of ADS and FR performances has been made in this context, and the relative benefits of transmutation have been quantified in each case taking into consideration, more realistically, the residual mass inventory after the shutdown of all nuclear installations.

EPFL2003

Fission Rates Measured Using High-Energy Gamma-Rays from Short Half-Life Fission Products in Fresh and Spent Nuclear Fuel

Hanna Kröhnert

In recent years, higher discharge burn-ups and initial fuel enrichments have led to more and more heterogeneous core configurations in light water reactors (LWRs), especially at the beginning of cycle when fresh fuel assemblies are loaded next to highly burnt ones. As this trend is expected to continue in the future, the Paul Scherrer Institute has, in collaboration with the Swiss Association of Nuclear Utilities, swissnuclear, launched the experimental programme LIFE@PROTEUS. The LIFE@PROTEUS programme aims to better characterise interfaces between burnt and fresh UO2 fuel assemblies in modern LWRs. Thereby, a novel experimental database is to be made available for enabling the validation of neutronics calculations of strongly heterogeneous LWR core configurations. During the programme, mixed fresh and highly burnt UO2 fuel lattices will be investigated in the zero-power research reactor PROTEUS. One of the main types of investigations will be to irradiate the fuel in PROTEUS and measure the resulting fission rate distributions across the interface between fresh and burnt fuel zones. The measurement of fission rates in burnt fuel re-irradiated in a zero-power reactor requires, however, the development of new experimental techniques which are able to discriminate against the high intrinsic activity of the fuel. The principal goal of the present research work has been to develop such a new measurement technique. The selected approach is based on the detection of high-energy gamma-ray lines above the intrinsic background (i.e. above 2200 keV), which are emitted by short-lived fission products freshly created in the fuel. The fission products 88Kr, 142La, 138Cs, 84Br, 89Rb, 95Y, 90mRb and 90Rb, with half-lives between 2.6 min and 2.8 h, have been identified as potential candidates. During the present research work, the gamma-ray activity of short-lived fission products has, for the first time, been measured and quantitatively evaluated for re-irradiated burnt UO2 fuel samples with burn-ups of about 36 and 46GWd/t. Based on experiments carried out with these fuel samples in a reference test lattice of the PROTEUS reactor, fresh-to-burnt-fuel fission rate ratios could be determined. The 1σ uncertainties on the derived fission rate ratios are 1.7 to 3.4% and are mainly due to the statistical uncertainties. Calculated values of the fission rate ratios, as obtained using the Monte Carlo code MCNPX, have been shown to agree with the experimental results within these uncertainties. In deriving fresh-to-burnt-fuel fission rate ratios,142La and 138Cs have emerged as the preferred fission products. Their fission yields for the main fissile isotope (235U, 239Pu and 241Pu) are similar, which makes them relatively insensitive to the exact composition of the burnt fuel. Finally, a measurement station for the future LIFE@PROTEUS experiments has been proposed and evaluated, along with a detailed formulation of recommendations for optimised irradiation and measurement strategies. The estimated accuracy for the foreseen measurements of fission rate ratios between fresh and highly burnt fuel pins is 1 to 2%. The contribution of nuclear-data related uncertainties have been pointed out as possibly representing the main constraint on the achievable accuracy in future experiments. In brief, the present research work has established a novel experimental technique for measuring and comparing fission rates in fresh and highly burnt fuels in a zero-power research reactor such as PROTEUS. Moreover, possibilities have been presented for the further optimisation needed for a future, routine application of the technique.