Studies of Capillary Phase Transitions of Methane in Metal−Organic Frameworks by Gauge Cell Monte Carlo Simulation

Ma, Qintian; Yang, Qingyuan; Zhong, Chongli; Mi, Jianguo; Liu, Dahuan

doi:10.1021/la903643f

Cited by 10 publications

(8 citation statements)

References 50 publications

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“…Of great interest for new materials development, however, is that the ever‐increasing use of general force field parameters for MOF atoms is allowing the use of molecular simulation as a screening tool, as summarized in Table 1 . The majority of these studies involve energy‐related gases such as methane,50 carbon dioxide,54–57 hydrogen,58–60 or some combination of these,48, 51–53 but applications to more complex analytes also have been reported 49, 61, 62. Although many modeling investigations focus on high‐pressure conditions typical of industrial applications, comparison of adsorption energies at infinite dilution is relevant to chemical sensing, as seen in Figure for a range of organic analytes and MOFs.…”

Section: Computational Modelingmentioning

confidence: 99%

Metal‐Organic Frameworks: A Rapidly Growing Class of Versatile Nanoporous Materials

2010

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Metal-organic frameworks (MOFs) represent a new class of hybrid organic-inorganic supramolecular materials comprised of ordered networks formed from organic electron donor linkers and metal cations. They can exhibit extremely high surface areas, as well as tunable pore size and functionality, and can act as hosts for a variety of guest molecules. Since their discovery, MOFs have enjoyed extensive exploration, with applications ranging from gas storage to drug delivery to sensing. This review covers advances in the MOF field from the past three years, focusing on applications, including gas separation, catalysis, drug delivery, optical and electronic applications, and sensing. We also summarize recent work on methods for MOF synthesis and computational modeling.

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Section: Computational Modelingmentioning

confidence: 99%

Metal‐Organic Frameworks: A Rapidly Growing Class of Versatile Nanoporous Materials

2010

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“…[38][39][40][41][42][43] However, in none of the latter studies the coexisting phases have been characterized. Moreover, evidence has been given for only one condensation transition and the applied simulation techniques did not allow to systematically explore the critical behavior and to study inhomogeneous systems where the coexisting phases are separated from each other by an interface.…”

Section: Introductionmentioning

confidence: 99%

“…Several computer simulation studies using grand canonical Monte Carlo (GCMC) simulations of gases such as CO 2 and CH 4 in various IRMOFs have determined adsorption isotherms at low temperatures and found evidence for the emergence of a line of first-order phase transition ending in a critical point. − However, in none of the latter studies the coexisting phases have been characterized. Moreover, evidence has been given for only one condensation transition, and the applied simulation techniques did not allow to systematically explore the critical behavior and to study inhomogeneous systems where the coexisting phases are separated from each other by an interface.…”

Section: Introductionmentioning

confidence: 99%

Condensation of Methane in the Metal–Organic Framework IRMOF-1: Evidence for Two Critical Points

Höft

Horbach

2015

J. Am. Chem. Soc.

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Extensive grand canonical Monte Carlo simulations in combination with successive umbrella sampling are used to investigate the condensation of methane in the nanoporous crystalline material IRMOF-1. Two different types of novel condensation transitions are found, each of them ending in a critical point: (i) a fluid-fluid transition at higher densities (the analog of the liquid-gas transition in the bulk) and (ii) a phase transition at low densities on the surface of the IRMOF-1 structure. The nature of these transitions is different from the usual capillary condensation in thin films and cylindrical pores where the coexisting phases are confined in one or two of the three spatial dimensions. In contrast to that, in IRMOF-1 the different phases can be described as bulk phases that are inhomogeneous due to the presence of the metal-organic framework. As a consequence, the condensation transitions in IRMOF-1 belong to the three-dimensional (3D) Ising universality class.

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“…However, by using a general force field approach such as the Universal or DREIDING force fields, a large set of NFMs may be initially ranked according to some simulated property for more detailed computational or experimental analysis. A number of computational screening studies have been published relating to the storage or separation of industrially relevant small gases − and also chemical detection of larger organics. , …”

Section: Introductionmentioning

confidence: 99%

Grand Canonical Monte Carlo Simulation of Low-Pressure Methane Adsorption in Nanoporous Framework Materials for Sensing Applications

2012

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Although the properties of nanoporous framework materials (NFMs) for high-pressure gas storage are well-known, low-level gas detection (<5 mbar) is also possible. Here, we describe a systematic investigation of NFM structure to identify advantageous features for methane sensing. Using grand canonical Monte Carlo simulations, we show that trends at low pressures relevant to sensing do not fully mirror those at high pressures. NFMs with pore diameters similar in size to methane show the highest uptake, and amine functionalization of the M 2 (dhtp) series provides modest enhancement. Unexpectedly, the presence of coordinated solvent can yield enhancements up to 250%. Our results enable prediction of NFM film thicknesses required to achieve a given methane sensitivity by three adsorption-based sensor types. Finally, the results of CH 4 /N 2 and CH 4 /H 2 O mixture simulations for promising candidate materials provide additional insight into the utility of these materials in multiple environments. Only small changes in uptake were observed when N 2 or H 2 O was introduced as a background gas, justifying the use of pure methane simulations for largescale screening of NFMs. One notable exception is Zn 2 (dhtp), which could serve well in an inert N 2 environment, but not in a humid one. Overall, these results provide general guidance for identifying effective NFMs for chemical detection, as well as for the specific case of methane, and for designing effective sensors for that purpose.

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Studies of Capillary Phase Transitions of Methane in Metal−Organic Frameworks by Gauge Cell Monte Carlo Simulation

Cited by 10 publications

References 50 publications

Metal‐Organic Frameworks: A Rapidly Growing Class of Versatile Nanoporous Materials

Metal‐Organic Frameworks: A Rapidly Growing Class of Versatile Nanoporous Materials

Condensation of Methane in the Metal–Organic Framework IRMOF-1: Evidence for Two Critical Points

Grand Canonical Monte Carlo Simulation of Low-Pressure Methane Adsorption in Nanoporous Framework Materials for Sensing Applications

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