The decontamination of concrete is a major concern in many Department of Energy (DOE) facilities. Numerous techniques (abrasive methods, manual methods, ultrasonics, concrete surface layer removal, chemical extraction methods, etc.) have been used to remove radioactive contamination from the surface of concrete. Recently, processes that are based on electrokinetic phenomena have been developed to decontaminate concrete. Electrokinetic decontamination has been shown to remove from 70 to over 90% of the surface radioactivity. To evaluate and improve the electrokinetic processes, a model has been developed to simulate the transport of ionic radionuclei constituents through the pores of concrete and into the anolyte and catholyte. The model takes into account the adsorption and desorption kinetics of the radionuclei from the pore walls, and ion transport by electro-osmosis, electromigration,and diffusion. A numerical technique, orthogonal collocation, is used to simultaneously solve the governing convective diffusion equations for a porous concrete slab and the current density equation. This paper presents the theoretical framework of the model and the results from the computation of the dynamics of ion transport during electrokinetic treatment of concrete. The simulation results are in good agreement with experimental data.