惰性载体支撑钙铜复合吸收剂的碳酸化性能及其动力学分析

采用Pechini法分别制备了无惰性载体支撑和惰性载体(Al2O3或者ZrO2)支撑的钙铜复合吸收剂。借助热重分析仪研究了反应温度、载体种类对其氧化性能和CO2捕集性能的影响，并借助扫描电子显微镜(SEM)和氮吸附分析其微观结构。最后，利用缩核模型对惰性载体支撑和无惰性载体支撑的钙铜复合吸收剂的碳酸化反应中的动力学控制阶段开展了动力学分析。结果表明：惰性载体可以显著提升钙铜复合吸收剂的CO2捕集性能，相比于无惰性载体支撑的钙铜复合吸收剂，Al2O3和ZrO2支撑的钙铜复合吸收剂经历10次循环后，CO2捕集量分别提升了100%和71%；添加惰性载体会降低钙铜复合吸收剂的载氧量，但并不影响其循环稳定性。随着碳酸化温度的升高，钙铜复合吸收剂的碳酸化速率和最终CO2捕集量均显著增加。动力学结果表明，添加惰性载体不仅可以加快碳酸化反应动力学控制阶段的反应速率，延缓动力学控制阶段反应速率的衰减，同时还可以降低碳酸化反应活化能，进而对碳酸化反应起到显著的促进作用。

Analysis of Carbonation and Kinetic Performance of Inert Support-Stabilized CaO/CuO Composites

Unstabilized and inert support (i.e. Al2O3 or ZrO2) stabilized CaO/CuO composites were synthesized by the Pechini method, respectively. The effects of reaction temperatures and types of inert support on their oxidation and CO2 capture performance were investigated via the thermogravimetric analyzer (TGA). The morphologies and microstructures were characterized by the scanning electron microscopy (SEM) and N2 physisorption measurements. Finally, a shrinking core model was employed to describe the kinetically-controlled stage of the carbonation process for Al2O3 stabilized and unstabilized CaO/CuO composites, respectively. The results show that the incorporation of inert support significantly enhances the CO2 capture performance by 100% and 71% for Al2O3 and ZrO2 stabilized CaO/CuO composites, respectively, after 10 repeated cycles. Although the incorporation of inert support decreases O.2 carrying capacities, negligible effects have been found for the cyclic stability. Carbonation temperatures show an important role in the CO2 capture performance: with the increase in carbonation temperatures, the carbonation rate and final CO2 uptake increased simultaneously. The kinetic studies show that the incorporation of inert support enhances the reaction rate of the kinetics controlled stage slows down the decline in reaction rate, and lower the activation energies. Overall, the inert support-stabilized CaO/CuO composites exhibit better CO2 capture performance.