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Abstract:The concentrations of the long-lived nuclear reaction products 129 I and 36 Cl have been measured in samples from the MEGAPIE liquid metal spallation target. Samples from the bulk target material (lead-bismuth eutectic, LBE), from the interface of the metal free surface with the cover gas, from LBE/steel interfaces and from noble metal absorber foils installed in the cover gas system were analysed using Accelerator Mass Spectrometry at the Laboratory of Ion beam Physics at ETH Zürich. The major part of 129 I and 36 Cl was found accumulated on the interfaces, particularly at the interface of LBE and the steel walls of the target container, while bulk LBE samples contain only a minor fraction of these nuclides. Both nuclides were also detected on the absorber foils to a certain extent (≪ 1% of the total amount). The latter number is negligible concerning the radio-hazard of the irradiated target material; however it indicates a certain affinity of the absorber foils for halogens, thus proving the principle of using noble metal foils for catching these volatile radionuclides. The total amounts of 129 I and 36 Cl in the target were estimated from the analytical data by averaging within the different groups of samples and summing up these averages over the total target. This estimation could account for about half of the amount of 129 I and 36 Cl predicted to be produced using nuclear physics modelling codes for both nuclides. The significance of the results and the associated uncertainties are discussed.

Various types of proton-irradiated lead-bismuth eutectic (LBE) samples from the MEGAPIE prototype spallation target were analyzed concerning their content of (148)Gd, (173)Lu, and (146)Pm by use of α- and γ-spectrometry. A radiochemical separation procedure was developed to isolate the lanthanide fraction and to prepare thin samples for α-ray measurement. The results prove a substantial depletion of these three elements in bulk samples, whereas accumulation on the LBE/steel-interfaces was observed. The amount of material accumulated on surfaces was roughly estimated by relating the values measured on the sample surfaces to the total surface of the inner target walls. The amount of (148)Gd, (173)Lu, and (146)Pm was then quantified by summing up the contributions from every sample type. The results show a reasonable agreement with theoretical predictions. The obtained results are of utmost importance for the evaluation of the performance of high-power spallation targets, especially concerning the residual nuclide production, the physicochemical behavior of the produced radionuclides during operation, and in terms of an intermediate or final disposal.

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