Ab initio parametrized MM3 force field for the metal‐organic framework MOF‐5

Tafipolsky, Maxim; Amirjalayer, Saeed; Schmid, Rochus

doi:10.1002/jcc.20648

Cited by 125 publications

(185 citation statements)

References 66 publications

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“…This model successfully predicts the IRMOF-1 structure and yields vibrational frequencies in reasonable agreement with the predictions of density functional theory (DFT). 33 It is also encouraging that the benzene self-diffusion constant obtained from MD calculations is within ~30% of the value measured by NMR. 24 More recently, another fully bonded, but flexible force field for IRMOF-1 was used to calculate the phonon thermal conductivity and vibrational power spectra of this MOF using molecular dynamics.…”

Section: Introductionmentioning

confidence: 60%

“…Recently published experimental spectra of IRMOF-1 54-56 and analogous inorganic complexes provide a basis for comparison 57,58 In addition, there are two recently published spectra obtained from force field simulations. 33,34 Unlike our nonbonded approach, however, these force fields include bonded terms between all atoms, including Zn, O cent , and O carb .…”

Section: Energetic Validationmentioning

confidence: 99%

“…In some cases allowing the empty framework to relax results in unreasonably short bond distances, 32 while in others diffusion constants are significantly overpredicted. 24 One approach to these problems is the "flexible," but still fully bonded, force field developed by Schmid and coworkers, 24,33 who parameterized the MM3 force field to account for interactions with the Zn 4 O clusters in IRMOF-1. This model successfully predicts the IRMOF-1 structure and yields vibrational frequencies in reasonable agreement with the predictions of density functional theory (DFT).…”

Section: Introductionmentioning

confidence: 99%

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Stress-Induced Chemical Detection Using Flexible Metal−Organic Frameworks

et al. 2008

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In this work we demonstrate the concept of stress-induced chemical detection using metalorganic frameworks (MOFs) by integrating a thin film of the MOF HKUST-1 with a microcantilever surface. The results show that the energy of molecular adsorption, which causes slight distortions in the MOF crystal structure, can be efficiently converted to mechanical energy to create a highly responsive, reversible, and selective sensor. This sensor responds to water, methanol, and ethanol vapors, but yields no response to either N 2 or O 2 . The magnitude of the signal, which is measured by a built-in piezoresistor, is correlated with the concentration and can be fitted to a Langmuir isotherm. Furthermore, we show that the hydration state of the MOF layer can be used to impart selectivity to CO 2 . We also report the first use of surface-enhanced Raman spectroscopy to characterize the structure of a MOF film. We conclude that the synthetic versatility of these nanoporous materials holds great promise for creating recognition chemistries to enable selective detection of a wide range of analytes. A force field model is described that successfully predicts changes in MOF properties and the uptake of gases. This model is used to predict adsorption isotherms for a number of representative compounds, including explosives, nerve agents, volatile organic compounds, and polyaromatic hydrocarbons. The results show that, as a result of relatively large heats of adsorption (> 20 kcal mol -1 ) in most cases, we expect an onset of adsorption by MOF as low as 10 -6 kPa, suggesting the potential to detect compounds such as RDX at levels as low as 10 ppb at atmospheric pressure.

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Section: Introductionmentioning

confidence: 60%

Section: Energetic Validationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Stress-Induced Chemical Detection Using Flexible Metal−Organic Frameworks

et al. 2008

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“…[13][14][15] A number of force fields have been developed to accurately describe individual important MOFs. One of the first such was the extended MM3 16 force field for MOF-5 17 and for later Copper paddlewheel -based MOFs, 18 both from Schmid and coworkers. Recently, Smit and coworkers derived a force field from entirely periodic calculations to predict the CO 2 and H 2 O adsorption isotherms in Mg-MOF-2 and ZIF-11 22 Many MOFs possess significant structural flexibility, and in these cases, this flexibility largely dictates the behaviour of the MOF w.r.t gas adsorption, thermal expansion and response to pressure.…”

Section: Introductionmentioning

confidence: 99%

“…al published a program, QuickFF, 29 that automates the process of force field generation beginning from quantum mechanical calculations. In the case of MOFs, by employing DFT calculations on both connector-and linker-centred clusters, QuickFF was validated against previously derived force fields for MIL-53(Al) 24 and MOF-5 17 Rather than directly deriving force fields from ab initio data, a different approach toward a force field that may be applied universally to MOFs is to build upon the Universal Force Field of Rappé. 30 UFF has been applied broadly to systems as far ranging as organic molecules, metal complexes and even MOFs.…”

Section: Introductionmentioning

confidence: 99%

Extension of the Universal Force Field for Metal–Organic Frameworks

Coupry

Addicoat

Heine

2016

J. Chem. Theory Comput.

171

174

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We have extended the Universal Force Field for to cover all moieties present in the most extensive framework library to date, i.e. the Computation-Ready Experimental (CoRE) database (Chem. Mater. 26, 6185 (2014)).Thus, we have extended the parameters to include the fourth and fifth row transition metals, lanthanides and an additional atom type for Sulphur, while the parameters of original UFF and of UFF4MOF are not modified. Employing the new parameters significantly enlarges the number of structures that may be subjected to a UFF calculation, i.e. more than doubling accessible MOFs of the CoRE structures and thus reaching over 99% of CoRE structure coverage. In turn, 95% of optimized cell parameters are within 10% of their experimental values. We contend these parameters will be most useful for the generation and rapid prototyping of hypothetical MOF structures from SBU databases.

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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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Ab initio parametrized MM3 force field for the metal‐organic framework MOF‐5

Cited by 125 publications

References 66 publications

Stress-Induced Chemical Detection Using Flexible Metal−Organic Frameworks

Stress-Induced Chemical Detection Using Flexible Metal−Organic Frameworks

Extension of the Universal Force Field for Metal–Organic Frameworks

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

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