Mechanism of High-Temperature CO2 Sorption on Lithium Zirconate

Lithium zirconate (Li2ZrO3) is one of the most promising materials for CO2 separation from flue gas at high temperature. This material is known to be able to absorb a large amount of CO2 at around 400−700 °C. However, the mechanism of the CO2 sorption/desorption process on Li2ZrO3 is not known yet. In this study, we examined the CO2 sorption/desorption mechanism on Li2ZrO3 by analyzing the phase and microstructure change of Li2ZrO3 during the CO2 sorption/desorption process with the help of thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and X-ray diffraction (XRD) analyses. Li2ZrO3 powders were prepared from lithium carbonate (Li2CO3) and zirconium oxide (ZrO2) by the solid-state method, and the CO2 sorption/desorption property was examined by TGA. It was shown that pure Li2ZrO3 absorbs a large amount of CO2 at high temperature with a slow sorption rate. Addition of potassium carbonate (K2CO3) and Li2CO3 in the Li2ZrO3 remarkably improves the CO2 sorption rate of the Li2ZrO3 materials. DSC analysis for the CO2 sorption process indicates that doped lithium/potassium carbonate is in the liquid state during the CO2 sorption process and plays an important role in improving the CO2 uptake rate. XRD analysis for phase and structure change during the sorption/desorption process shows that the reaction between Li2ZrO3 and CO2 is reversible. Considering all data obtained in this study, we proposed a double-shell model to describe the mechanism of the CO2 sorption/desorption on both pure and modified Li2ZrO3.