Polarizable Force Fields for CO<sub>2</sub>and CH<sub>4</sub>Adsorption in M-MOF-74

Becker, Tim M.; Heinen, Jurn; Dubbeldam, David; Lin, Li‐Chiang; Vlugt, Thijs J. H.

doi:10.1021/acs.jpcc.6b12052

Cited by 102 publications

(84 citation statements)

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“…Considering polarization explicitly can help to create force fields that overcome the shortcomings of current generic force fields. [313,[317][318][319][320] Lachet et al explored polarization in MC simulations using solely polarization between the framework and adsorbate molecules and neglecting polarization caused by induced dipoles, so-called back-polarization. [219] Thereby, an iterative scheme is avoided and the computational costs of the method are drastically reduced.…”

Section: Polarizable and Qm-derived Force Fields For Open-metal Sitesmentioning

confidence: 99%

“…Becker et al therefore removed the contribution of implicitly considered polarization to the interaction potential, by applying a global scaling parameter to all Lennard-Jones energy parameters developed without explicit polarization. [313] In Figure 7b, we compare the polarization energy of a CO 2 molecule Figure 8. Comparison between the experimental results of Herm et al [321] (open), Queen et al [322] (yellow), Yu et al [323] (orange), and Dietzel et al [324] (brown) and simulation results using the polarizable force field of Becker et al [313] (black), the UFF force field (blue) and the DFT-derived non-polarizable force field of Mercado et al [325] (green) for CO 2 in Mg-MOF-74.…”

Section: Polarizable and Qm-derived Force Fields For Open-metal Sitesmentioning

confidence: 99%

“…[313] In Figure 7b, we compare the polarization energy of a CO 2 molecule Figure 8. Comparison between the experimental results of Herm et al [321] (open), Queen et al [322] (yellow), Yu et al [323] (orange), and Dietzel et al [324] (brown) and simulation results using the polarizable force field of Becker et al [313] (black), the UFF force field (blue) and the DFT-derived non-polarizable force field of Mercado et al [325] (green) for CO 2 in Mg-MOF-74. a) adsorption isotherm at 298 K (Herm et al [321] 313K) (b) heat of adsorption as a function of uptake.…”

Section: Polarizable and Qm-derived Force Fields For Open-metal Sitesmentioning

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: Polarizable and Qm-derived Force Fields For Open-metal Sitesmentioning

confidence: 99%

Section: Polarizable and Qm-derived Force Fields For Open-metal Sitesmentioning

confidence: 99%

Section: Polarizable and Qm-derived Force Fields For Open-metal Sitesmentioning

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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“…Over time the pure A crystal either grows or shrinks, which changes the ratio of A to B particles in the liquid phase. When equilibrium has been reached, the temperature is the melting temperature of that particular liquid composition [35]. Figure 1(b) shows the fraction of B particles where the abscissa is the melting temperature at the pressure identified in Fig.…”

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confidence: 99%

Phase Diagram of Kob-Andersen-Type Binary Lennard-Jones Mixtures

2018

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The binary Kob-Andersen (KA) Lennard-Jones mixture is the standard model for computational studies of viscous liquids and the glass transition. For very long simulations, the viscous KA system crystallizes, however, by phase separating into a pure A particle phase forming a fcc crystal. We present the thermodynamic phase diagram for KA-type mixtures consisting of up to 50% small (B) particles showing, in particular, that the melting temperature of the standard KA system at liquid density 1.2 is 1.028(3) in A particle Lennard-Jones units. At large B particle concentrations, the system crystallizes into the CsCl crystal structure. The eutectic corresponding to the fcc and CsCl structures is cutoff in a narrow interval of B particle concentrations around 26% at which the bipyramidal orthorhombic PuBr_{3} structure is the thermodynamically stable phase. The melting temperature's variation with B particle concentration at two constant pressures, as well as at the constant density 1.2, is estimated from simulations at pressure 10.19 using isomorph theory. Our data demonstrate approximate identity between the melting temperature and the onset temperature below which viscous dynamics appears. Finally, the nature of the solid-liquid interface is briefly discussed.

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“…100,[116][117][118] To capture the charge interactions between a gas particle and a materials' charge density, partial charges are typically assigned to each atom in the gas and framework. This effectively treats the complex electron density and nuclei of each atom as a single point charge positioned at its centre, which is then used to compute energy interactions with coulombs' law.…”

Section: H1 Charge Generationmentioning

confidence: 99%

Computational development of the nanoporous materials genome

2017

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H1 Abstract.There is currently a large push towards big data and data mining in materials research to accelerate discovery. Zeolites, metal-organic frameworks (MOFs) and other related crystalline porous materials are not immune to this recent phenomenon, as evidenced by the proliferation of porous structure databases and computational gas adsorption screening studies over the past decade. The strive to identify the best materials for a variety of gas separation and storage applications has not only led to collections of thousands of synthesised structures, but the development of hypothetical material building algorithms.The materials databases assembled with these algorithms expand greatly on the range of complex pore structures that have been synthesised, with the rationale that we have discovered only a small fraction of realisable structures and expanding upon these will accelerate rational design. In this review, we highlight some of the methods developed to build these databases, and some of the important outcomes resulting from large-scale computational screening efforts. SummaryIn the field of nanoporous materials discovery, we are witnessing the emergence of big data analytics combined with traditional computational thermodynamics calculations. This review turns a critical eye on the current state of the art, with a focus on computational database generation and results from large-scale screening for gas separations. H1 Introduction.The discovery, in the late 19 th century, that zeolites could trap interesting and valuable particles in their pores opened up an entire field of research 1,2 . This seemingly simple phenomenon was an enormous boon to the oil and gas industry, seeing as how cheap, but effective porous materials could serve as a catalyst for hydrocarbon cracking. From their humble beginnings (being carved out of rock faces), zeolites, and their ability to selectively trap guests in their pores, have become integral in not only the oil and gas industry, but in detergents (as ion exchangers) and natural gas purification to name a few 1 .Zeolites have since enjoyed an almost exclusive dominance in porous materials research until the late 20 th century, when we began to observe the creation of more diverse materials in terms of chemistry, network connectivity, and physical properties.At present, there are a little over 200 known zeolite structures, which is only a small fraction of the total number of structures that have been predicted 3 . In addition, if we were also able to expand the chemical diversity of these materials beyond the conventional Si 4+ , O 2-, and Al 3+ ions found in zeolites, one could envision designing materials for virtually any gas separation application. Thus when the first articles arose in the 1990's characterising Metal-Organic Frameworks (MOFs) [4][5][6][7][8] , and later Covalent Organic Frameworks (COFs) 9,10 , Zeolitic Imidazolate Frameworks (ZIFs) 11 , and Porous Polymer Networks (PPNs) 12 the excitement was palpable. It was recognised early-on by Yaghi, O'Keeffe, ...

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Polarizable Force Fields for CO₂and CH₄Adsorption in M-MOF-74

Cited by 102 publications

References 152 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

Phase Diagram of Kob-Andersen-Type Binary Lennard-Jones Mixtures

Computational development of the nanoporous materials genome

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Polarizable Force Fields for CO2and CH4Adsorption in M-MOF-74

Cited by 102 publications

References 152 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

Phase Diagram of Kob-Andersen-Type Binary Lennard-Jones Mixtures

Computational development of the nanoporous materials genome

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Polarizable Force Fields for CO₂and CH₄Adsorption in M-MOF-74