Adsorption of CO2, CH4, N2 and He on MFI, CHA and DDR zeolites

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2025-03-11 DOI:10.1016/j.micromeso.2025.113599

Iliana Kyriazidou, Mojtaba Sinaei Nobandegani, Jonas Hedlund, Liang Yu

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Abstract

The adsorption equilibrium isotherms of the common components of natural gas and biogas, CO₂, CH₄, N₂, and He were experimentally measured over wide temperature ranges on all-silica MFI, CHA, and DDR zeolite crystals. First, large zeolite crystals, suitable for adsorption measurements, were synthesized and characterized by XRD and SEM. In the next step, gas adsorption data was recorded and the Toth equation was fitted to the measured adsorption data, and the adsorption capacity at saturation (C_sat), affinity constant (b), and Toth heterogeneity parameter (t) were estimated. Finally, the van't Hoff equation was used to calculate the isosteric enthalpy of adsorption and adsorption entropy for all gases on each zeolite. The results reveal that the Toth equation can accurately predict the adsorption of gases on the studied microporous zeolite crystals in the investigated temperature range. To the best of our knowledge, the saturation adsorption capacity and adsorption enthalpy for helium on CHA and DDR zeolites have been determined experimentally for the first time in the present work. The estimated adsorption parameters presented in this work are accurate, primarily due to the large crystals used for the adsorption measurements and the recording of low-temperature adsorption equilibrium isotherms over broad temperature ranges. These factors are crucial for the reliability of our results, which are invaluable for understanding adsorption and mass transfer in zeolite materials, as well as for advancing the development of zeolite materials for gas separation.

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实验测量了全硅质 MFI、CHA 和 DDR 沸石晶体在宽温度范围内对天然气和沼气中常见成分 CO2、CH4、N2 和 He 的吸附平衡等温线。首先，合成了适合吸附测量的大型沸石晶体，并通过 XRD 和 SEM 进行了表征。接下来，记录气体吸附数据，并将 Toth 方程拟合到测量的吸附数据中，从而估算出饱和吸附容量 (Csat)、亲和常数 (b) 和 Toth 异质性参数 (t)。最后，利用范特霍夫方程计算了每种沸石上所有气体的等效吸附焓和吸附熵。结果表明，在所研究的温度范围内，托斯方程可以准确预测气体在所研究的微孔沸石晶体上的吸附情况。据我们所知，CHA 和 DDR 沸石上氦的饱和吸附容量和吸附焓是在本研究中首次通过实验测定的。这项工作中提出的估计吸附参数是准确的，这主要归功于用于吸附测量的大晶体以及在宽温度范围内记录的低温吸附平衡等温线。这些因素对我们结果的可靠性至关重要，而我们的结果对了解沸石材料中的吸附和传质，以及推动气体分离用沸石材料的发展都是非常宝贵的。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.