Abstract
Equilibrium concentrations of major elements in an underground repository with a capacity of 100,000 drums have been simulated using the geochemical computer code (EQMOD). The simulation has been carried out at the conditions of pH 12 to 13.5, and Eh 520 and -520 mV. Solubilities of magnesium and calcium decrease with the increase of pH. The solubility of iron increases with pH at Eh -520 mV of reducing environment while it almost entirely exists as the precipitate of Fe(OH)$_3$(s) at Eh 520 mV of oxidizing environment. All of cobalt and nickel are predicted to be dissolved in the liquid phase regardless of pH since the solubility limit is greater than the total concentration. In the case of cesium and strontium, all forms of both ions are present in the liquid phase because they have negligible sorption capacity on cement and large solubility under disposal atmosphere. And thus the total concentration determines the equilibrium concentration. Adsorbed amount of iodide and carbonate are dependent on adsorption capacity and adsorption equilibrium constant. Especially, the calcite turns out to be a solubility-limiting phase on the carbonate system. In order to validate the model, the equilibrium concentrations measured for a number of systems which consist of iron, cement, synthetic groundwater and radionuclides are compared with those predicted by the model. The concentrations between the model and the experiment of nonadsorptive elements cesium, strontium, cobalt nickel and iron, are well agreed. It indicates that the assumptions and the thermodynamic data in this work are valid. Using the adsorption equilibrium constant as a free parameter, the experimental data of iodide and carbonate have been fitted to the model. The model is in a good agreement with the experimental data of the iodide system.
