Release dynamic process identification for a cement based material in various leaching conditions. Part II. Modelling the release dynamics for different leaching conditions.

Abstract

This paper deals with process identification and model development for the case of a porous reference material leaching under certain hydrodynamic conditions. Four different dynamic leaching tests have been applied in order to take into account different types of solid/liquid contact conditions corresponding to various real leaching scenarios: monolithic and granular material with sequential eluate renewal, and granular material and continuously renewed eluate with different hydrodynamic conditions (dispersion, residence time). A coupled chemical-mass transfer model has been developed to describe the leaching behaviour under all experimental conditions. Diffusion has been considered as the mass transport mechanism inside the saturated porous material and dispersive convection as that in the leachate. Two specific phenomena have been identified and considered in the model: (i) the early surface dissolution of the material which results in high Ca concentration and (ii) the late weak dissolution of Na and K giving rise to a long-term residual release. The intrinsic material parameters such as the initial concentrations in the pore water and solid phases were determined by applying equilibrium leaching tests and geochemical modelling. Diffusion coefficients for different elements and the late solubility of alkalines have been found to reach the same values in the four tests. The estimated values of the surface dissolution kinetic constant have shown a dependence on leachate hydrodynamics when the thickness of the degraded layer is nearly the same in the four tests (intrinsic parameter of the material). The competition between the four main dynamic processes, i.e. diffusion, convection, late dissolution, and surface dissolution, has been emphasized and compared in the four leaching tests: the hydrodynamic dispersion and the residence time had no effect on the leaching behaviour of alkalines, which is controlled by diffusion, whereas the behaviour of calcium (a major element of the material) was strongly influenced. This has significant effects on eluate pH values and on the concentration of Pb (the monitored pollutant). The model was then applied to simulate a landfill scenario in the case of a stabilized/solidified incinerator residue containing heavy metals and chloride. A high rain infiltration level and the use of small blocs are favourable conditions for enhanced pollutant release.