Leaching behavior of prototypical corium samples: A step to understand the interactions between the fuel debris and water at the Fukushima Daiichi reactors

Abstract

On 11 March 2011, the Great East Japan Earthquake occurred and caused a severe nuclear accident at the Fukushima Daiichi Nuclear Power Station (1F). A policy for corium debris retrieval will be decided in the near future. To this end, debris management after removal from reactors must be optimized. From the viewpoint of cost and waiting for definitive solutions, interim or long-term underwater storage is one of the considered options after debris removal. Leaching data on the long term behavior of debris in water are therefore needed before debris removal. In addition, it is important to understand potential differences in leaching behaviors between debris and Spent Fuel (SF) to get comparative elements.For these reasons, simulated in-vessel and ex-vessel corium debris, fabricated in the Colima experimental facility set up in the PLINIUS platform at CEA Cadarache, were selected and leaching experiments were carried out under oxidizing conditions. In parallel, geochemical modeling was performed to better understand the experimental concentrations, pH evolutions and secondary phase’s formation.Finally, the Fractional Release Rates of the (U, Zr)O2 matrix for the two kinds of samples (in-vessel and ex-vessel) were found to be close to or one order of magnitude lower than that of SF under oxidizing conditions (from 10−6 to 10−7 per day) but the release processes are different. Indeed, the Fraction of Inventory in Aqueous Phase of Mo, Ba, Sr, Rh, La, Nd, Ce and Y tended to be higher than that of uranium and zirconium in this study whatever the element considered. The release of simulating PFs, including low volatile element like trivalent rare earths, does not appear to be fully controlled by that of the (U, Zr)O2 matrix from a macroscopic and average point of view. The FPs could be partially located outside the (U, Zr)O2 solid solution as a function of the corium history (quenching rate and thermal history, chemical interactions…). The location of inventories and their chemical forms are not very well known moreover uncertainties related to heterogeneity are important and may also impact the calculation of the global released fractions over time. For the ex-vessel sample, releases into the solution of the main concrete elements (Si, Ca, Mg) seem well correlated and dissociated from the behavior of the (U, Zr)O2 phase. Further studies are needed especially on real or prototypical corium approaching the conditions of the Fukushima accident. The study of simpler and model systems could also provide information on the reactivity of the (U, Zr)O2 matrix.