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KFI 沸石上 CO2 的吸附和分离:阳离子类型和 Si/Al 比对平衡和动力学性质的影响。

Adsorption and separation of CO2 on KFI zeolites: effect of cation type and Si/Al ratio on equilibrium and kinetic properties.

机构信息

Department of Chemical Engineering, Vrije Universiteit Brussel, Brussels, Belgium.

出版信息

Langmuir. 2013 Apr 23;29(16):4998-5012. doi: 10.1021/la400352r. Epub 2013 Apr 12.

Abstract

Selective separation of CO2 is becoming one of the key technologies in the (petro-) chemical industry. This study focuses on the adsorption and separation of CO2 from CH4 on a new low-silica (LS) type of the eight-membered ring KFI zeolite. A series of alkali (Li, Na, K) and alkaline-earth (Mg, Ca, Sr) exchanged samples of the new LS KFI were synthesized and characterized. LS Li-KFI showed the largest pore volume, whereas LS Na-KFI and LS K-KFI were inaccessible for Argon at 87 K. Adsorption of CO2 at 303 K demonstrated the dominant quadrupolar interaction on alkali-exchanged LS KFI samples. LS Li-KFI showed the largest capacities upon high pressure isotherm measurements of CO2 (4.8 mmol/g), CH4 (2.6 mmol/g), and N2 (2.2 mmol/g) up to 40 bar at 303 K. The performance of the new LS KFI was compared to a KFI sample (ZK-5) with a higher Si/Al ratio. Isotherm measurements and dynamic breakthrough experiments demonstrated that ZK-5 samples show larger working capacities for CO2/CH4 separations at low pressure. Li-ZK-5 and Na-ZK-5 show the highest capacities and high selectivities (similar to benchmark 13X).

摘要

选择性分离 CO2 正成为(石油)化工行业的关键技术之一。本研究聚焦于新型低硅(LS)八元环 KFI 沸石对 CH4 中 CO2 的吸附与分离。合成并表征了一系列碱(Li、Na、K)和碱土金属(Mg、Ca、Sr)交换的新型 LS KFI 样品。LS Li-KFI 具有最大的孔体积,而 LS Na-KFI 和 LS K-KFI 在 87 K 下无法被氩气进入。在 303 K 下吸附 CO2 表明碱金属交换的 LS KFI 样品中存在主导的偶极相互作用。在 303 K 下,LS Li-KFI 在 40 bar 以下的高压等温线测量中表现出最大的 CO2(4.8 mmol/g)、CH4(2.6 mmol/g)和 N2(2.2 mmol/g)吸附容量。新型 LS KFI 的性能与 Si/Al 比更高的 KFI 样品(ZK-5)进行了比较。等温线测量和动态穿透实验表明,ZK-5 样品在低压下对 CO2/CH4 分离具有更大的工作容量。Li-ZK-5 和 Na-ZK-5 具有最高的容量和高选择性(类似于基准 13X)。

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