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The aim of this article was to theoretically study diffusion and migration of chloride ions during electrochemical chloride removal. The proposed model would enable optimization of its application by predicting the optimal treatment time and current combination. A mathematical model for simulating the transport behavior of chloride ions was developed by consideration of diffusion and migration of chloride ions when a constant DC current density was applied through the marine cast iron artifacts. The corresponding tests were conducted to validate the mathematical model. This model predicted the data of the extraction ratio of the chloride ion that correlated satisfactorily with the experimental values. An important issue in electrochemical chloride removal was to understand how chloride ions moved, taking account of diffusion and migration of chloride ions and the release of binding chloride ions. The effects of the treatment time, externally applied current density, chloride diffusion coefficient, and rate constant of release of binding chloride ion on chloride removal are studied. The specific quantitative details applied to one-dimensional model were discussed here. This article has proposed a mathematical model for the first time, which was showed to be a useful tool that can reveal the ionic transport mechanism and optimize the application during electrochemical chloride removal.