Plasticization behavior in polymers of intrinsic microporosity (PIM-1): A simulation study from combined Monte Carlo and molecular dynamics

Kupgan, Grit; Demidov, Alexander G.; Colina, Coray M.

doi:10.1016/j.memsci.2018.08.004

Cited by 67 publications

(78 citation statements)

References 97 publications

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“…Fang et al [62,63] applied the Widom test particle insertion method [50] to predict CO 2 solubility in PIM-1 and their results were in close agreement with the experimental ones. Recently, Kupgan et al [64] predicted CO 2 sorption in PIM-1 up to 50 bar, employing a scheme combining Grand Canonical Monte Carlo (GCMC) and Molecular Dynamics simulations devised by Hölck et al [65], while Frentrup et al [66] performed Nonequilibium Molecular Dynamics simulations for the direct simulation of He and CO 2 permeability through a thin membrane of PIM-1, which was in good qualitative agreement with experimental data.…”

Section: Introductionmentioning

confidence: 83%

Modelling Mixed-Gas Sorption in Glassy Polymers for CO2 Removal: A Sensitivity Analysis of the Dual Mode Sorption Model

Ricci

Angelis

2019

Membranes

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In an effort to reduce the experimental tests required to characterize the mixed-gas solubility and solubility-selectivity of materials for membrane separation processes, there is a need for reliable models which involve a minimum number of adjustable parameters. In this work, the ability of the Dual Mode Sorption (DMS) model to represent the sorption of CO2/CH4 mixtures in three high free volume glassy polymers, poly(trimethylsilyl propyne) (PTMSP), the first reported polymer of intrinsic microporosity (PIM-1) and tetrazole-modified PIM-1 (TZ-PIM), was tested. The sorption of gas mixtures in these materials suitable for CO2 separation has been characterized experimentally in previous works, which showed that these systems exhibit rather marked deviations from the ideal pure-gas behavior, especially due to competitive effects. The accuracy of the DMS model in representing the non-idealities that arise during mixed-gas sorption was assessed in a wide range of temperatures, pressures and compositions, by comparing with the experimental results available. Using the parameters obtained from the best fit of pure-gas sorption isotherms, the agreement between the mixed-gas calculations and the experimental data varied greatly in the different cases inspected, especially in the case of CH4 absorbed in mixed-gas conditions. A sensitivity analysis revealed that pure-gas data can be represented with the same accuracy by several different parameter sets, which, however, yield markedly different mixed-gas predictions, that, in some cases, agree with the experimental data only qualitatively. However, the multicomponent calculations with the DMS model yield more reliable results than the use of pure-gas data in the estimation of the solubility-selectivity of the material.

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Section: Introductionmentioning

confidence: 83%

Modelling Mixed-Gas Sorption in Glassy Polymers for CO2 Removal: A Sensitivity Analysis of the Dual Mode Sorption Model

Ricci

Angelis

2019

Membranes

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“…Sorption and penetrant-induced plasticization and swelling phenomena have been investigated by molecular simulation of bulk polymeric systems [38,183,184,185,186,187,188,189] using either CGMC or implementing iterative multi-stage methods to determine the correct pressure at given penetrant concentration [46,47,190]. Van der Vegt et al [46,186] have studied sorption of CO 2 in a polyethylene-like membrane and have identified below T g a hole filling mechanism in combination with a finite positive partial molar volume of CO 2 being responsible for the gas sorption thermodynamics in the glassy polymer.…”

Section: Mechanistic Aspects Of Sorption and Transportmentioning

confidence: 99%

“…Performance and plasticization resistance of an emerging class of polymeric membrane materials called ‘thermally rearranged polymers’ [194,195,196,197,198,199,200,201,202,203,204] that are generated by thermally modifying aromatic polyimide chains, has also been investigated computationally [205,206,207,208,209,210,211] in recent years. These phenomena have been also simulated for high free volume polymers of intrinsic microporosity (PIM) [56,189,212,213].…”

Section: Mechanistic Aspects Of Sorption and Transportmentioning

confidence: 99%

Molecular Modeling Investigations of Sorption and Diffusion of Small Molecules in Glassy Polymers

Vergadou

Theodorou

2019

Membranes

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With a wide range of applications, from energy and environmental engineering, such as in gas separations and water purification, to biomedical engineering and packaging, glassy polymeric materials remain in the core of novel membrane and state-of the art barrier technologies. This review focuses on molecular simulation methodologies implemented for the study of sorption and diffusion of small molecules in dense glassy polymeric systems. Basic concepts are introduced and systematic methods for the generation of realistic polymer configurations are briefly presented. Challenges related to the long length and time scale phenomena that govern the permeation process in the glassy polymer matrix are described and molecular simulation approaches developed to address the multiscale problem at hand are discussed.

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“…38 Allowing polymer relaxation during sorption produces isotherms that are more consistent with experiment. 38,96 This polymer relaxation in the presence of CO 2 is associated with shifting the FVE distribution to larger sizes. 38 It is unclear if the shift in FVE distribution is the same polymer MD investigations of gas transport through glassy polymers shows that when gas molecules occupy a void site, they explore the full surface area of the void, and the rate-limiting step for their forward motion is polymer chain fluctuation creating a channel between voids then closing off space behind the molecule.…”

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confidence: 98%

Permeation of CO₂ and N₂ through glassy poly(dimethyl phenylene) oxide under steady‐ and presteady‐state conditions

Soniat

Tesfaye

Mafi

et al. 2020

Journal of Polymer Science

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Glassy polymers are often used for gas separations because of their high selectivity. Although the dual‐mode permeation model correctly fits their sorption and permeation isotherms, its physical interpretation is disputed, and it does not describe permeation far from steady state, a condition expected when separations involve intermittent renewable energy sources. To develop a more comprehensive permeation model, we combine experiment, molecular dynamics, and multiscale reaction–diffusion modeling to characterize the time‐dependent permeation of N2 and CO2 through a glassy poly(dimethyl phenylene oxide) membrane, a model system. Simulations of experimental time‐dependent permeation data for both gases in the presteady‐state and steady‐state regimes show that both single‐ and dual‐mode reaction–diffusion models reproduce the experimental observations, and that sorbed gas concentrations lag the external pressure rise. The results point to environment‐sensitive diffusion coefficients as a vital characteristic of transport in glassy polymers.

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Plasticization behavior in polymers of intrinsic microporosity (PIM-1): A simulation study from combined Monte Carlo and molecular dynamics

Cited by 67 publications

References 97 publications

Modelling Mixed-Gas Sorption in Glassy Polymers for CO2 Removal: A Sensitivity Analysis of the Dual Mode Sorption Model

Modelling Mixed-Gas Sorption in Glassy Polymers for CO2 Removal: A Sensitivity Analysis of the Dual Mode Sorption Model

Molecular Modeling Investigations of Sorption and Diffusion of Small Molecules in Glassy Polymers

Permeation of CO₂ and N₂ through glassy poly(dimethyl phenylene) oxide under steady‐ and presteady‐state conditions

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Plasticization behavior in polymers of intrinsic microporosity (PIM-1): A simulation study from combined Monte Carlo and molecular dynamics

Cited by 67 publications

References 97 publications

Modelling Mixed-Gas Sorption in Glassy Polymers for CO2 Removal: A Sensitivity Analysis of the Dual Mode Sorption Model

Modelling Mixed-Gas Sorption in Glassy Polymers for CO2 Removal: A Sensitivity Analysis of the Dual Mode Sorption Model

Molecular Modeling Investigations of Sorption and Diffusion of Small Molecules in Glassy Polymers

Permeation of CO2 and N2 through glassy poly(dimethyl phenylene) oxide under steady‐ and presteady‐state conditions

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Permeation of CO₂ and N₂ through glassy poly(dimethyl phenylene) oxide under steady‐ and presteady‐state conditions