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

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Abstract

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.

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真空辅助解吸锆酸钠吸附剂以提高燃烧前二氧化碳捕获的循环稳定性
锆酸钠(Na2ZrO3)在理想条件下(100% N2 中的解吸),在高温下具有快速的吸附动力学和出色的循环稳定性,因此是一种很有前途的燃烧前二氧化碳捕集材料。但目前还缺乏对 Na2ZrO3 在苛刻条件下(高浓度 CO2 中的解吸)循环捕集性能的研究。本研究采用湿法混合和加热干燥的方法制备了 Na2ZrO3,并比较了苛刻条件下和真空条件下解吸样品循环捕集二氧化碳性能的差异。在吸附-解吸循环过程中,确定了 Na2ZrO3 的晶体结构。还对晶体结构进行了建模和模拟,以分析单斜 Na2ZrO3 具有优异捕集性能的原因。研究发现,单斜 Na2ZrO3 特殊的互锁和多层堆叠结构使其与二氧化碳的反应活性很高。研究发现,在苛刻条件下,仅靠高温对 Na2ZrO3 的解吸作用不大,但真空条件可促进 Na2ZrO3 对高浓度 CO2 的解吸,在 1000 ℃-1050 ℃ 的真空解吸条件下得到的 Na2ZrO3 具有良好的捕获性能和循环稳定性。真空解吸使 Na2ZrO3 更完全地恢复到单斜状态,有利于二氧化碳的捕获。本研究试图模拟实际工业应用中恶劣的捕集环境,并探索将 Na2ZrO3 用作燃烧前捕集的碳捕集材料的可能性。
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