Predicting Multicomponent Adsorption Isotherms in Open‐Metal Site Materials Using Force Field Calculations Based on Energy Decomposed Density Functional Theory

Heinen, Jurn; Burtch, Nicholas C.; Walton, Krista S.; Guerra, Célia Fonseca; Dubbeldam, David

doi:10.1002/chem.201603895

Cited by 11 publications

(15 citation statements)

References 47 publications

(104 reference statements)

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“…Ideal Adsorption Solution Theory (IAST) fails, but Heinen et al. have shown that accurate results can be obtained by explicit binary‐mixture simulations using a force field that captures the relevant orbital interactions using an additional charge‐induced‐dipole‐like term . Recently, Durholt et al.…”

Section: Zeolite and Mof Force Fieldsmentioning

confidence: 99%

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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: Zeolite and Mof Force Fieldsmentioning

confidence: 99%

“…Unfortunately, conventional force fields do not capture the olefin‐metal interactions. Ideal adsorbed solution theory (IAST) breaks down for olefin adsorption in open‐metal site materials due to non‐ideal donor–acceptor interactions …”

Section: Introductionmentioning

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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“…A pragmatic approach is the derivation of improved parameter sets from density-functional theory (DFT) calculations of adsorption energies at the CUS [41][42][43][44][47][48][49]. This strategy has yielded good results for alkanes, alkenes and alkynes in CUS-containing MOFs [19,43,44,[50][51][52][53][54].…”

Section: Introductionmentioning

confidence: 99%

A computational study of the interaction of C2 hydrocarbons with CuBTC

Afonso

Toda

Gomes

et al. 2020

Computational Materials Science

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The adsorptions of ethane, ethene, and ethyne over the coordinatively unsaturated sites (CUS) of copper (II) benzene-1,3,5-tricarboxylate (CuBTC) were studied by means of density functional theory (DFT), using both cluster or periodic models. Exchange-correlation functionals from different rungs of the Jacobs ladder of the DFT were used and energies were corrected for the basis superposition error either through extrapolation to the complete basis set limit or upon the consideration of the Counterpoise method. From the calculated data, it was found that the adsorbate to CUS distances decrease in the order ethane > ethene ≈ ethyne and that the strength of adsorption increase in the order ethane to ethyne to ethene. The energies of interactions of ethene and ethyne with the CUS of CuBTC are approximately the double of that calculated for ethane. The calculated adsorption energies and geometries are in very satisfactory agreement with the available experimental results. The results of topological analyses confirm that the unsaturated bonds of ethene and ethyne form open shell like bonds with the CUS while interaction with ethane have predominant closed shell character.

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“…For example, for ethane the adsorption sites in the small pockets, but for ethene the adsorption site is at the copper-site. In a mixture, the molecules are adsorbing at different sites (segregation) which differ strongly in interaction energy and Ideal Adsorption Solution Theory (IAST) therefore fails in this case [77]. Figure 15 shows an aqueous solution of ionic liquids (cationanion-water system).…”

Section: Examining Adsorption Sitesmentioning

confidence: 99%

iRASPA: GPU-accelerated visualization software for materials scientists

Dubbeldam

Calero

Vlugt

2018

Molecular Simulation

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142

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A new macOS software package, iRASPA, for visualisation and editing of materials is presented. iRASPA is a document-based app that manages multiple documents with each document containing a unique set of data that is stored in a file located either in the application sandbox or in iCloud drive. The latter allows collaboration on a shared document (on High Sierra). A document contains a gallery of projects that show off the main features, a CloudKit-based access to the CoRE MOF database (approximately 8000 structures), and local projects of the user. Each project contains a scene of one or more structures that can initially be read from CIF, PDB or XYZ-files, or made from scratch. Main features of iRASPA are: structure creation and editing, pictures and movies, ambient occlusion and high-dynamic range rendering, collage of structures, (transparent) adsorption surfaces, cell replicas and supercells, symmetry operations like space group and primitive cell detection, screening of structures using user-defined predicates, and GPU-computation of helium void fraction and surface areas in a matter of seconds. Leveraging the latest graphics technologies like Metal, iRASPA can render hundreds of thousands of atoms (including ambient occlusion) with stunning performance. The software is freely available from the Mac App Store. ARTICLE HISTORY

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Predicting Multicomponent Adsorption Isotherms in Open‐Metal Site Materials Using Force Field Calculations Based on Energy Decomposed Density Functional Theory

Cited by 11 publications

References 47 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

A computational study of the interaction of C2 hydrocarbons with CuBTC

iRASPA: GPU-accelerated visualization software for materials scientists

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