Effects of the ion-exchange sequence on the CO2 uptake and CO2–over–N2 selectivity of zeolite NaKA

Wenming Hao , Yufei Shi , Latif Ullah , Ruifeng Li , Niklas Hedin
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Abstract

The CO2 and N2 adsorption on small-pore zeolite |Na12-xKx|-A was hypothesized to be affected by the ion exchange sequence used for the zeolite preparation. Zeolites were prepared by ion exchange of a commercially available zeolite |Na12|-A (4A) and a zeolite |K12|-A (3A) composition prepared from zeolite 4A. The CO2 and N2 adsorption properties were studied experimentally, and the binary CO2-over-N2 selectivity was estimated from single-component adsorption data using the apparent Henry's law coefficients. It was observed that the level of CO2 adsorption was reduced by increasing the K content for both series of zeolite NaKA. Zeolite |Na12-xKx|-A-from-4A had the highest CO2 adsorption capacity (at 1 atm and 273 K) for a given K content. At low K content, zeolite |Na12-xKx|-A-from-3A had the highest CO2-over-N2 selectivity. At an intermediate K content, the zeolites prepared from 4A had the highest selectivity. These differences show that non-equilibrium processes during the ion exchange are important for the CO2 and N2 adsorption properties of the derived zeolites. As of now, we refrain from speculating whether they relate to the detailed positioning of K+ and Na+ cations in the local structure of the zeolite or to mass-transport-related concentration gradients of the cations in the structure. Irrespectively, it was observed that the ion-exchange sequence affects the CO2 and N2 adsorption properties of the zeolites, which could be of general importance when it comes to the tuning of the properties of cation-rich zeolites.

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离子交换顺序对NaKA分子筛CO2吸收率和CO2 - over - n2选择性的影响
假设CO2和N2在小孔沸石|Na12xKx|-A上的吸附受到用于沸石制备的离子交换序列的影响。沸石是通过市售沸石|Na12|-a(4A)和由4A沸石制备的沸石|K12|-a(3A)组合物的离子交换制备的。实验研究了CO2和N2的吸附性能,并使用表观亨利定律系数从单组分吸附数据中估计了二元CO2-over-N2选择性。观察到,对于两个系列的NaKA沸石,通过增加K含量来降低CO2吸附水平。对于给定的K含量,来自4A的沸石|Na12xKx|-A具有最高的CO2吸附能力(在1atm和273K下)。在低K含量下,来自3A的沸石|Na12xKx|-A具有最高的CO2-over-N2选择性。在中等K含量下,由4A制备的沸石具有最高的选择性。这些差异表明,离子交换过程中的非平衡过程对衍生沸石的CO2和N2吸附性能很重要。到目前为止,我们不猜测它们是否与沸石局部结构中K+和Na+阳离子的详细定位有关,或者与结构中阳离子的质量传输相关浓度梯度有关。无论如何,观察到离子交换顺序影响沸石的CO2和N2吸附性能,这在调节富阳离子沸石的性能时可能具有普遍的重要性。
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