Draft paper: On the analysis of diffusive mass transfer in ex-vessel corium pools

In case of a severe accident at a nuclear power plant (NPP) involving the reactor pressure vessel (RPV) melt-through, confident solidification of ex-vessel corium is the imperative condition of its safe retention within the plant containment. The rate-determining process for solidification of ex-vessel coriums in the long-term is the chemical diffusion in the liquid phase at the solid-liquid interface. The process of chemical diffusion in the diffusive boundary layer can evolve taking on different rates, depending on the boundary conditions and the melt composition. Nonetheless, the chemical diffusion rates would entwine the self-diffusivities of corium constituents, which in turn would depend on the melt chemical composition. This work looks at some aspects of analytical and experimental determination of self-diffusivities of corium constituents. Following the corium-concrete interaction, an ex-vessel corium melt would contain several chemical components, including a fraction of silica. Accordingly, ex-vessel corium is considered in this paper as a silicate melts. In the realm of the geological and glass sciences, where silicate melts are most often discussed, the diffusive transport and viscous flow are conceived interrelated from a phenomenological point of view. Though the viscous and diffusive mass transfer mechanisms are not identical for different species even in the same melt, a combination of semi-empirical models can still provide an estimation of the diffusion thresholds in ex-vessel corium melts. Thus, the first part of this paper presents an analysis of the applicability of such empirical models for simple silicate melts based on the published data. This is followed by an estimation of diffusivities in melt compositions typical of ex-vessel coriums. Alternatively, although the general trend towards a coupled description of the viscous flow and diffusion for ex-vessel corium melts seems promising, it is limited to published data on self-diffusivities of constituents in this kind of melts. The latter can appear different in the very nature of their chemical compositions - the melt local structure, subject to the actual silica content and other factors. Whereas the chemical diffusion models presented elsewhere for silicate melts tie in the melt constituents' self-diffusion properties, their extension to ex-vessel coriums can be comparatively discussed provided reliable methods (analytical and/or experimental) for determination of self-diffusion coefficients as a function of the melt composition are verified to yield pertinent self-diffusion data. Therefore, the second part of this paper presents an experimental technique for obtaining self-diffusion coefficients of corium constituents in compositionally controlled melts. (author)