Kinetic Study of High-Pressure Carbonation Reaction of Calcium-Based Sorbents in the Calcium Looping Process (CLP)

In this study, the high-pressure carbonation kinetics of calcium oxide (CaO) derived from three calcium-based sorbents, namely, limestone (CaCO3), calcium hydroxide [Ca(OH)2], and precipitated calcium carbonate (PCC), used in the calcium looping process (CLP) system were studied using a magnetic suspension balance (MSB) analyzer. Different total pressures (1000–15000 torr) and concentrations of CO2 (10–30%) were tested to determine their effects on the carbonation reaction rate at a specific operating temperature of the CLP system, namely, 700 °C. The carbonation reaction rate was found to increase with increasing concentration of CO2 (10–30%) at a constant total pressure of 5000 torr and to exhibit first-order kinetics. However, the total pressure has an effect on the carbonation reaction rate only at lower total pressures. With a 20% CO2 stream, the reaction rate was observed to increase until the total pressure reached 4000 torr, beyond which a further increase in total pressure had a negative effect on the rate of the carbonation reaction of CaO derived from all three precursors. Further, the carbonation reaction had a different reaction order with respect to the partial pressure of CO2. It was found that the reaction was first-order at lower total pressures but changed to zeroth-order when the total pressure exceeded 4000 torr. The different reaction order under elevated pressures can be explained by the Langmuir mechanism. In addition, the reaction rate of carbonation conducted at high total pressure was greater than that at atmospheric pressure, under cyclic testing. The results also showed that there was no significant difference in the behavior of the carbonation reaction of CaO at elevated pressures, regardless of the different precursors used to generate the CaO.