Adsorption of Aromatics in MFI-Type Zeolites: Experiments and Framework Flexibility in Monte Carlo Simulations

Caro-Ortiz, Sebastián; Zuidema, Erik; Dekker, Desmond; Rigutto, Marcello; Dubbeldam, David; Vlugt, Thijs J. H.

doi:10.1021/acs.jpcc.0c06096

Cited by 10 publications

(27 citation statements)

References 153 publications

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“…Models that capture the physics behind the flexibility of the zeolite and aromatics in confinements are needed. 80 The insights shown here are based on the thermodynamic stability of the isomers inside the zeolite pores. Thus, diffusion limitations of xylenes in the channels of the zeolite types considered should be thoroughly assessed.…”

Section: Resultsmentioning

confidence: 99%

“…It is known that framework flexibility plays a significant role in the adsorption of aromatics in zeolites. 80 For very flexible zeolite frameworks, loadings up to two times larger than in a rigid zeolite framework are obtained at a given pressure. 124 However, models for framework flexibility should not be blindly applied to zeolites.…”

Section: Methodsmentioning

confidence: 99%

“… 124 However, models for framework flexibility should not be blindly applied to zeolites. 80 The intra-framework interactions in flexible framework models induce small but important changes in the atom positions of the zeolite and hence in the adsorption isotherms. 80 The effects of using models for framework flexibility in different zeolite types are unknown.…”

Section: Methodsmentioning

confidence: 99%

“… 80 The intra-framework interactions in flexible framework models induce small but important changes in the atom positions of the zeolite and hence in the adsorption isotherms. 80 The effects of using models for framework flexibility in different zeolite types are unknown. For these reasons, the zeolite frameworks are considered rigid.…”

Section: Methodsmentioning

confidence: 99%

“…Molecular simulations are an extensively used tool to predict the thermodynamic properties of a wide diversity of systems . Molecular simulations have been extensively used to predict the adsorption properties of hydrocarbons in zeolites − and other nanoporous materials. − Commonly, Monte Carlo simulations (MCs) in the grand-canonical ensemble (GCMC) can be used to compute sorbate loadings in a zeolite for different temperatures and pressures. − Several studies where MCs are used to study adsorption of aromatics in zeolites can be found in the literature. ,− Most molecular simulation studies of adsorption of hydrocarbons in zeolites have focused on adsorption from a vapor phase . This is due to the difficult insertion and deletion of molecules at conditions close to saturation, leading to inefficient simulations .…”

Section: Introductionmentioning

confidence: 99%

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Competitive Adsorption of Xylenes at Chemical Equilibrium in Zeolites

et al. 2021

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The separation of xylenes is one of the most important processes in the petrochemical industry. In this article, the competitive adsorption from a fluid-phase mixture of xylenes in zeolites is studied. Adsorption from both vapor and liquid phases is considered. Computations of adsorption of pure xylenes and a mixture of xylenes at chemical equilibrium in several zeolite types at 250 °C are performed by Monte Carlo simulations. It is observed that shape and size selectivity entropic effects are predominant for small one-dimensional systems. Entropic effects due to the efficient arrangement of xylenes become relevant for large one-dimensional systems. For zeolites with two intersecting channels, the selectivity is determined by a competition between enthalpic and entropic effects. Such effects are related to the orientation of the methyl groups of the xylenes. m -Xylene is preferentially adsorbed if xylenes fit tightly in the intersection of the channels. If the intersection is much larger than the adsorbed molecules, p -xylene is preferentially adsorbed. This study provides insight into how the zeolite topology can influence the competitive adsorption and selectivity of xylenes at reaction conditions. Different selectivities are observed when a vapor phase is adsorbed compared to the adsorption from a liquid phase. These insight have a direct impact on the design criteria for future applications of zeolites in the industry. MRE-type and AFI-type zeolites exclusively adsorb p -xylene and o -xylene from the mixture of xylenes in the liquid phase, respectively. These zeolite types show potential to be used as high-performing molecular sieves for xylene separation and catalysis.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Competitive Adsorption of Xylenes at Chemical Equilibrium in Zeolites

et al. 2021

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Multiscale Computational Approaches toward the Understanding of Materials

Bordonhos

Galvão

Gomes

et al. 2022

Advcd Theory and Sims

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Herewith, an overview of the group's collaborative research efforts on the development and deployment of computational approaches to understand materials and tools at different length and time scales is presented. The techniques employed range from quantum mechanical approaches based on the density functional theory to classical atomistic and coarse-grained force field methods, targeting molecular systems composed of a few to several million atoms at different levels of detail. These new tools and molecular models are presented to the computational materials science community so they can be used in more realistic molecular modelling studies of the properties of materials and their dependence on subtle modifications of their structures. The review concludes by presenting a selection of recent computational case-studies oriented toward the understanding of the synthesis of materials, the interpretation of unexpected experimental results, the prediction of material properties, and the materials selection based on their characteristics for applications in areas such as gas adsorption/separation, corrosion protection, and catalysis.

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