How reliable is the Real Adsorbed Solution Theory (RAST) for estimating ternary mixture equilibrium in microporous host materials?

IF 2.8 3区工程技术 Q3 CHEMISTRY, PHYSICAL

Fluid Phase Equilibria Pub Date : 2024-10-20 DOI:10.1016/j.fluid.2024.114260

Rajamani Krishna, Jasper M. van Baten

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引用次数: 0

Abstract

Microporous crystalline adsorbents such as zeolites, and metal-organic frameworks (MOFs) have potential use in a wide variety of separations applications. In applications such as CO₂ capture, the Ideal Adsorbed Solution Theory (IAST) often fails to provide a quantitative description of mixture adsorption equilibrium especially in cation-exchanged zeolites. The failure of the IAST is ascribable to non-compliance with one or more tenets mandated by the IAST such as (a) homogeneous distribution of adsorbates within the pore landscape, (b) no preferential location of guest species, and (c) absence of molecular clustering due to say hydrogen bonding. The focus of this article is on the reliability of the Real Adsorbed Solution Theory (RAST) models for quantitative estimation of adsorption equilibrium. Configurational-Bias Monte Carlo (CBMC) simulations are undertaken to determine the adsorption equilibrium for ternary CO₂/CH₄/N₂, CO₂/CH₄/C₃H₈, CO₂/CH₄/H₂, and water/methanol/ethanol mixtures in NaX, LTA-4A, CHA, DDR, and MFI zeolites. Additionally, CBMC simulations of the constituent binary pairs are used to determine the Wilson or NRTL parameters, taking due account of the dependence of the activity coefficients on the spreading pressure. Use of the binary pair Wilson or NRTL parameters allows the estimation of ternary mixture adsorption equilibrium, that is tested against the CBMC data on component loadings. In all investigated guest/host combinations, the RAST provides a good estimation of ternary mixture adsorption equilibrium.

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真实吸附溶液理论（RAST）在估算微孔主材料中的三元混合物平衡时有多可靠？

沸石和金属有机框架（MOFs）等微孔结晶吸附剂具有广泛的分离应用潜力。在二氧化碳捕获等应用中，理想吸附溶液理论（IAST）往往无法定量描述混合物的吸附平衡，特别是在阳离子交换沸石中。IAST 的失效可归因于没有遵守 IAST 规定的一个或多个原则，例如：（a）吸附剂在孔隙中的均匀分布；（b）客体物种没有优先位置；以及（c）没有因氢键而导致的分子团聚。本文的重点是真实吸附溶液理论（RAST）模型在定量估计吸附平衡方面的可靠性。通过配置偏置蒙特卡罗（CBMC）模拟，确定了三元 CO2/CH4/N2、CO2/CH4/C3H8、CO2/CH4/H2 和水/甲醇/乙醇混合物在 NaX、LTA-4A、CHA、DDR 和 MFI 沸石中的吸附平衡。此外，对组成二元对的 CBMC 模拟用于确定 Wilson 或 NRTL 参数，同时适当考虑活性系数对扩散压力的依赖性。使用二元对 Wilson 或 NRTL 参数可以估算三元混合物的吸附平衡，并根据 CBMC 对组分负载的数据进行测试。在所有研究过的客体/主体组合中，RAST 都能很好地估计三元混合物的吸附平衡。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Fluid Phase Equilibria 工程技术-工程：化工

CiteScore

5.30

自引率

15.40%

发文量

223

审稿时长

53 days

期刊介绍： Fluid Phase Equilibria publishes high-quality papers dealing with experimental, theoretical, and applied research related to equilibrium and transport properties of fluids, solids, and interfaces. Subjects of interest include physical/phase and chemical equilibria; equilibrium and nonequilibrium thermophysical properties; fundamental thermodynamic relations; and stability. The systems central to the journal include pure substances and mixtures of organic and inorganic materials, including polymers, biochemicals, and surfactants with sufficient characterization of composition and purity for the results to be reproduced. Alloys are of interest only when thermodynamic studies are included, purely material studies will not be considered. In all cases, authors are expected to provide physical or chemical interpretations of the results. Experimental research can include measurements under all conditions of temperature, pressure, and composition, including critical and supercritical. Measurements are to be associated with systems and conditions of fundamental or applied interest, and may not be only a collection of routine data, such as physical property or solubility measurements at limited pressures and temperatures close to ambient, or surfactant studies focussed strictly on micellisation or micelle structure. Papers reporting common data must be accompanied by new physical insights and/or contemporary or new theory or techniques.