Vacuum assisted desorption of sodium zirconate sorbent for enhancing cyclic stability in pre-combustion CO2 capture

•Cyclic CO2 capacity decay results from incomplete reversion from Na2CO3 to Na2ZrO3.•Vacuum desorption is beneficial to the cyclic CO2 capture by Na2ZrO3.•Vacuum desorption favors the reversion of Na2ZrO3 to the monoclinic state.•The special dislocation-stacked structure of monoclinic Na2ZrO3 is simulated by MS.•The enhanced stability shows potential in-situ CO2 capture in pre-combustion. Sodium zirconate (Na2ZrO3) is a promising material for pre-combustion CO2 capture due to its fast sorption kinetics and excellent cyclic stability at high temperatures under ideal condition (desorption in 100% N2). Still, there is a lack of study on the performance of Na2ZrO3 cyclic capture under harsh condition (desorption in high concentration CO2). In this study, Na2ZrO3 was prepared by wet-mixing and heated-drying, and the difference in the cyclic CO2 capture performance of the sample was compared between desorption under harsh condition and vacuum condition. The crystal structure of Na2ZrO3 was identified during the sorption-desorption cycles. The crystal structure was also modeled and simulated to analyze the reason for the superior capture performance from the monoclinic Na2ZrO3. It was found that the special interlocked and multilayered stacked structure of the monoclinic Na2ZrO3 allowed for high reactivity with CO2. It was found that high temperature solely had little help in the desorption of Na2ZrO3 under harsh condition, but vacuum condition promoted desorption of Na2ZrO3 in high fraction CO2, and vacuum desorption at 1000 °C-1050 °C resulted in Na2ZrO3 with both good capture performance and cycling stability. Vacuum desorption led to more complete reversion of Na2ZrO3 to the monoclinic state, benefiting for CO2 capture. This study attempted to simulate the harsh capture environments of real industrial applications and to explore the possibility of Na2ZrO3 as a carbon capture material for pre-combustion capture.