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Performance of accelerated carbonation by basic oxygen furnace slag (BOFS) in a rotating packed bed (RPB) was evaluated in this investigation. The design of experiments (DOE) was introduced to evaluate the effect of different operating parameters including reaction time , particle size of BOFS , temperature , liquid-to-solid (L/S) ratio , and rotating speed on carbonation conversion of BOFS. A quadratic response surface was established statistically to yield maximum carbonation conversion based on experimental data. In addition , both the fresh and carbonated BOFS were characterized by the thermogravimetry and differential scanning calorimetry (TG/DSC) , X-ray diffraction (XRD) , and scanning electron microscopy equipped with X-ray energy dispersive spectroscopy (SEM-XEDS) to confirm the results of accelerated carbonation of BOFS in an RPB. Furthermore , by combining the process chemistry , reaction kinetics , and mass transfer , a prediction model for carbonation of BOFS within an RPB , with an error less than 10% , was well-developed. The enhancement factors for mass transfer coefficient in case of carbonation of BOFS within an RPB were determined accordingly. In comparison with the developed model and the RSM results , a standard operation procedure (SOP) was proposed for maximizing the carbonation conversion of BOFS. It was thus concluded that the accelerated carbonation of BOFS using an RPB is a promising process for CO2 capture due to its higher carbonation conversion achieving in a short reaction time.