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With the growing need for high-quality steel, the requirement for efficient deep desulfurization technologies is growing, and lots of research have be conducted. The desulfurization in hot iron with Mg produced in situ by the aluminothermic reduction of decomposed dolomite was simulated. The magnesium generated at the molten matte-slag interface is dissolved in the molten iron and desulfurizing while spread downwards The process has been studied by experiment and computational fluid dynamics simulation. Some analysis and assumptions were made for the simulation conditions and the simulated data are in good agreement with the experimental results. The rate of desulfurization depended mainly on the reaction rate and is almost independent of the rate of diffusion of Al, S and Mg according to the results. Under the present experimental conditions, the desulfurization rate increased with the increase in temperature and the amount of reactants. However, the effect is not obvious when the temperature is higher than 1623K. The adjustment in diffusion coefficient has minimal influence on the desulfurization efficiency. The desulfurization reaction is mainly in the homogeneous phase, and the proportion of magnesium bubble desulfurization could be ignored when the temperature is between 1523 K–1723 K.