Potential of polarizable force fields for predicting the separation performance of small hydrocarbons in M-MOF-74

Becker, Tim M.; Luna-Triguero, Azahara; Vicent-Luna, José Manuel; Lin, Li‐Chiang; Dubbeldam, David; Calero, Sofı́a; Vlugt, Thijs J. H.

doi:10.1039/c8cp05750h

Cited by 20 publications

(18 citation statements)

References 87 publications

(181 reference statements)

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“…Since this is local effect it is not possible to simply re‐parametrized the guest‐host interactions. Considering polarization explicitly can help to create force fields that overcome the shortcomings of current generic force fields …”

Section: Parameterizationmentioning

confidence: 99%

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials

Dubbeldam

Walton

Vlugt

et al. 2019

Advcd Theory and Sims

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Molecular simulations are an excellent tool to study adsorption and diffusion in nanoporous materials. Examples of nanoporous materials are zeolites, carbon nanotubes, clays, metal-organic frameworks (MOFs), covalent organic frameworks (COFs) and zeolitic imidazolate frameworks (ZIFs). The molecular confinement these materials offer has been exploited in adsorption and catalysis for almost 50 years. Molecular simulations have provided understanding of the underlying shape selectivity, and adsorption and diffusion effects. Much of the reliability of the modeling predictions depends on the accuracy and transferability of the force field. However, flexibility and the chemical and structural diversity of MOFs add significant challenges for engineering force fields that are able to reproduce experimentally observed structural and dynamic properties. Recent developments in design, parameterization, and implementation of force fields for MOFs and zeolites are reviewed.contain silicon and oxygen. They are readily available, very stable, and relatively cheap. The material should have the right combination of high adsorption selectivity, combined with adequate capacity for use in fixed-bed devices. Recently, new classes of nanoporous materials have been designed that have stability, high void volumes, and well defined tailorable cavities of uniform size. Example are metal-organic frameworks (MOFs), [1][2][3][4][5][6][7] covalent organic frameworks (COFs), [8,9] and zeolitic imidazolate frameworks (ZIFs). [10] These novel materials posses almost unlimited structural variety because of the many combinations of building blocks that can be imagined. The building blocks self-assembly during synthesis into crystalline materials that, after evacuation of the structure, can find applications in adsorption separations, air purification, gas storage, chemical sensing, and catalysis. [4,11] The judicious selection of building blocks allows the pore volume and functionality to be tailored in a rational manner. Because of the designprinciple underlying the synthesis, it is important to understand structure-properties relations, such as the mechanisms of gas separation as a function of shape and size of the pore system, in order to create "blueprints to MOF-design." Computer simulation is cost-effective, fast, and allows for rapid identification of important structural parameters affecting adsorption.Most of the published works on molecular simulation studying zeolites have used the Kiselev model. [12] In this model, zeolite atoms are fixed and interactions of guest atoms with silicon atoms is accounted for by an effective interaction only with the surrounding oxygen atoms. Interactions between sorbate molecules and the host are modeled by placing Lennard-Jones sites and partial charges on all framework atoms and sorbate molecules. The Kiselev model is attractive because of its simplicity and computational efficiency. This model has shown significant success, both in using the molecular dynamics method to compute, for example, the diffu...

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Section: Parameterizationmentioning

confidence: 99%

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials

Dubbeldam

Walton

Vlugt

et al. 2019

Advcd Theory and Sims

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“…Recently, more sophisticated polarizable models have also been used to model guest-framework interactions. [49][50][51][52][53][54] Among different guest molecules, modeling water in MOFs presents particular challenges due to the complex nature of the water-water interactions, which is responsible for the anomalous behavior of water as a function of temperature and pressure. [55][56][57] In this study, we integrate experimental and computational IR spectroscopy with MD simulations to investigate the properties of water in ZIF-90.…”

Section: Introductionmentioning

confidence: 99%

“…These FFs have been extensively used to simulate adsorption isotherms as well as structural, thermodynamic, and dynamical properties of various molecules (e.g., methane and small hydrocarbons, carbon dioxide, and water) adsorbed in the MOF pores. Recently, more sophisticated polarizable models have also been used to model guest–framework interactions. − Among different guest molecules, modeling water in MOFs presents particular challenges due to the complex nature of the water–water interactions, which is responsible for the anomalous behavior of water as a function of temperature and pressure. − …”

Section: Introductionmentioning

confidence: 99%

Simulation Meets Experiment: Unraveling the Properties of Water in Metal–Organic Frameworks through Vibrational Spectroscopy

et al. 2021

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In nanoporous materials, guest-host interactions affect the properties and function of both adsorbent and adsorbate molecules. Due to their structural and chemical diversity, metal-organic frameworks (MOFs), a common class of nanoporous materials, have been shown to be able to efficiently and, often, selectively adsorb various types of guest molecules. In this study, we characterize the structure and dynamics of water confined in ZIF-90. Through the integration of experimental and computational infrared (IR) spectroscopy, we probe the structure of heavy water (D 2 O) adsorbed in the pores, disentangling the fundamental framework-water and water-water interactions. The experimental IR spectrum of D 2 O in ZIF-90 displays a blue-shifted OD-stretch band compared to liquid D 2 O. The analysis of the IR spectra simulated at both classical and quantum levels indicates that the D 2 O molecules preferentially interact with the carbonyl groups of the framework and highlights the importance of including nuclear quantum effects and taking into account Fermi resonances for a correct interpretation of the OD-stretch band in terms of the underlying hydrogen-bonding motifs. Through a systematic comparison with the experimental spectra, we demonstrate that computational spectroscopy can be used to gain quantitative, molecular-level insights into framework-water interactions that determine the water adsorption capacity of MOFs as well as the spatial arrangements of the water molecules inside the MOF pores which, in turn, are key to the design of MOF-based materials for water harvesting.File list (2) download file view on ChemRxiv water_in_zif90.pdf (4.99 MiB) download file view on ChemRxiv supporting_information.pdf (4.44 MiB)

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“…The removal and enrichment of acetylene (C 2 H 2 ) from light hydrocarbon mixtures in the petrochemical industry is an indispensable and challenging task and is routinely implemented by the means of low-temperature multieffect distillation technology and accompanied by extremely high energy consumption and capital input, − whereas a high-purity single light hydrocarbon derived from oil cracking in the petrochemical industry is still difficult to achieve because of the extremely similar physical properties of hydrocarbons in terms of melting–boiling points and molecular dynamic sizes. − For instance, ethylene (C 2 H 4 ), originating from the fractionation of petroleum, usually tends to coexist with 1% C 2 H 2 , which could poison the catalyst in the process of Ziegler–Natta catalytic polymerization and even cause the compression operation to explode. − Thus, it is very imperative to generate highly pure single light hydrocarbon gas by exploring a competency separation method.…”

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confidence: 99%

Robust Heterometallic Co^IILa^III₂–Organic Framework for the Highly Efficient Separation of Acetylene from Light Hydrocarbon Mixtures

et al. 2021

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A highly robust heterometallic CoIILaIII 2–organic framework (NUC-19) is synthesized and features 1D rectangle-like channels with a window size of 3.4 × 6.3 Å2 and a carboxyl-group-modified inner surface. NUC-19 exhibits significantly differential uptake for C2H2, C2H4, and CH4, and the ideal adsorbed solution theory selectivities of C2H2/C2H4 (1:99, v/v) and C2H2/CH4 (50:50, v/v) at room temperature can reach up to 4.0 and 79.7, respectively. Fixed-bed dynamic breakthrough experiments under simulated industrial conditions indicate that NUC-19 could efficiently trap C2H2 from mixed gases of C2H2/CH4 and C2H2/C2H4.

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Potential of polarizable force fields for predicting the separation performance of small hydrocarbons in M-MOF-74

Abstract: Including explicit polarization significantly improves the description of the adsorption in comparison to non-polarizable generic force fields.

Cited by 20 publications

References 87 publications

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials

Simulation Meets Experiment: Unraveling the Properties of Water in Metal–Organic Frameworks through Vibrational Spectroscopy

Robust Heterometallic Co^IILa^III₂–Organic Framework for the Highly Efficient Separation of Acetylene from Light Hydrocarbon Mixtures

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Potential of polarizable force fields for predicting the separation performance of small hydrocarbons in M-MOF-74

Abstract: Including explicit polarization significantly improves the description of the adsorption in comparison to non-polarizable generic force fields.

Cited by 20 publications

References 87 publications

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials

Design, Parameterization, and Implementation of Atomic Force Fields for Adsorption in Nanoporous Materials

Simulation Meets Experiment: Unraveling the Properties of Water in Metal–Organic Frameworks through Vibrational Spectroscopy

Robust Heterometallic CoIILaIII2–Organic Framework for the Highly Efficient Separation of Acetylene from Light Hydrocarbon Mixtures

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Robust Heterometallic Co^IILa^III₂–Organic Framework for the Highly Efficient Separation of Acetylene from Light Hydrocarbon Mixtures