Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field

Verploegh, Ross J.; Kulkarni, Ambarish; Boulfelfel, Salah Eddine; Haydak, Jonathan; Tang, Dai; Sholl, David S.

doi:10.1021/acs.jpcc.9b00733

Cited by 46 publications

(54 citation statements)

References 120 publications

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“…Self-diffusion coefficients of alkanes were mildly dependent on loading, and transport diffusivities increased by more than an order of magnitude with loading for C 3 and C 4 hydrocarbons [231]. A recent article by Verploegh et al has extended these correlations to additional ZIFs and found a similar relationship between diffusivity and molecular diameter that also depends on the average window size [232]. These calculated diffusivities exhibited good agreement with the measurements by Chmelik for C 3 alkanes [233].…”

Section: Flexible Microporous Metal-organic Frameworksupporting

confidence: 70%

Connecting theory and simulation with experiment for the study of diffusion in nanoporous solids

et al. 2021

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Nanoporous solids are ubiquitous in chemical, energy, and environmental processes, where controlled transport of molecules through the pores plays a crucial role. They are used as sorbents, chromatographic or membrane materials for separations, and as catalysts and catalyst supports. Defined as materials where confinement effects lead to substantial deviations from bulk diffusion, nanoporous materials include crystalline microporous zeotypes and metal–organic frameworks (MOFs), and a number of semi-crystalline and amorphous mesoporous solids, as well as hierarchically structured materials, containing both nanopores and wider meso- or macropores to facilitate transport over macroscopic distances. The ranges of pore sizes, shapes, and topologies spanned by these materials represent a considerable challenge for predicting molecular diffusivities, but fundamental understanding also provides an opportunity to guide the design of new nanoporous materials to increase the performance of transport limited processes. Remarkable progress in synthesis increasingly allows these designs to be put into practice. Molecular simulation techniques have been used in conjunction with experimental measurements to examine in detail the fundamental diffusion processes within nanoporous solids, to provide insight into the free energy landscape navigated by adsorbates, and to better understand nano-confinement effects. Pore network models, discrete particle models and synthesis-mimicking atomistic models allow to tackle diffusion in mesoporous and hierarchically structured porous materials, where multiscale approaches benefit from ever cheaper parallel computing and higher resolution imaging. Here, we discuss synergistic combinations of simulation and experiment to showcase theoretical progress and computational techniques that have been successful in predicting guest diffusion and providing insights. We also outline where new fundamental developments and experimental techniques are needed to enable more accurate predictions for complex systems.

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Section: Flexible Microporous Metal-organic Frameworksupporting

confidence: 70%

Connecting theory and simulation with experiment for the study of diffusion in nanoporous solids

et al. 2021

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“…Also, generic force fields like DREIDING were used to model ZIF-8. [455] Recently, more general and transferable intra-molecular ZIF force fields were developed by Verploegh et al [456] , ZIF-FF by Weng et al [457] and MOF-FF for ZIFs by Durholt et al [458] Several other general approaches and force field for MOFs have been developed. MOF-FF, a third generation force field of Schmid and coworkers is based on the building block methodology.…”

Section: Mof Force Fieldsmentioning

confidence: 99%

“…Also, generic force fields like DREIDING were used to model ZIF‐8 . Recently, more general and transferable intra‐molecular ZIF force fields were developed by Verploegh et al ,. ZIF‐FF by Weng et al .…”

Section: Zeolite and Mof Force Fieldsmentioning

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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“…Adsorbate molecules are often described by empirical force fields fit to match the vapor/liquid coexistence properties of the molecule; [321] however, when these schemes prove to be inadequate, first principle-derived force fields [322,323] or corrections to account for quantum effects may be deployed. [324,325] Notably, Verploegh et al [326] have derived an enhanced force field for assessing the diffusion of small molecules in MOFs (the specific study was on ZIF structures). The force field was fit to DFT data and gives similar quality of forces to those extracted from periodic ab initio MD studies.…”

Section: Methodsmentioning

confidence: 99%

High Throughput Methods in the Synthesis, Characterization, and Optimization of Porous Materials

et al. 2020

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Notwithstanding these impediments, in many fields of materials science, solutions are being designed to mitigate hindrances to the efficient sampling of chemical space and improving the robustness of computational screening models through a combination of high throughput synthesis (HTS), characterization, and machine learning. In this review, we highlight key developments in high throughput approaches pertinent to porous materials. Specifically, we focus on developments in the field of zeolitic materials, metal-organic frameworks (MOFs), and touch upon covalent organic frameworks (COFs). Although superficially these classes of materials have little in common, there are structural links such as topology which allow for the consideration of how high throughput methods contrast with one another. By contrasting developments in different fields, we identify some underutilized approaches which could be leveraged in the future. We target structurally ordered materials because the exploration of chemical and topological space is more straightforward to enumerate, though similar approaches could be applied to disordered materials. The scale of the problem faced in materials science of targeted structure and function [1] is by no means unique; in drug discovery, HTS and chemoinformatic approaches have been used for more than 40 years in an attempt to accelerate the discovery of druggable molecules. [2,3] Unlike the drug discovery process, where Lipinski's "rule of 5" [4] provides a reliable top level sift for viable targets, identifying the most promising material for a target application requires very particular properties that may be intertwined in complex and contradictory ways. For example, thermoelectrics require high electrical conductivity and low thermal conductivity and yet these properties are typically correlated unless they can be separated. [5] Given the large scope of potential applications, the advent of the Materials Genome Initiative (MGI) [6,7] in the United States has undoubtedly helped to promote ways to solve the aforementioned obstacles and numerous others. Similarly there are major initiatives within the EU (e.g., NOMAD [8] and BIGmax [9]) and Switzerland (MARVEL [10]). In the MGI, nanoporous materials, including zeolites and MOFs, have been specifically targeted [11] and in this review, we seek to highlight particular challenges in the field of porous materials and how researchers have sought to overcome these challenges. We focus primarily on the methods used in HTS and rapid throughput/screening computational approaches. Aspects of high throughput computation applied to porous materials have been reviewed before, [12-14] as has high throughput experimentation (HTE) [15,16] but here we focus on their combination within an integrated workflow. Porous materials are widely employed in a large range of applications, in particular, for storage, separation, and catalysis of fine chemicals. Synthesis, characterization, and pre-and post-synthetic computer simulations are mostly carried out in a piecemeal a...

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Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field

Cited by 46 publications

References 120 publications

Connecting theory and simulation with experiment for the study of diffusion in nanoporous solids

Connecting theory and simulation with experiment for the study of diffusion in nanoporous solids

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

High Throughput Methods in the Synthesis, Characterization, and Optimization of Porous Materials

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