Toward Effective CO<sub>2</sub>/CH<sub>4</sub> Separations by Sulfur-Containing PIMs via Predictive Molecular Simulations

Hart, Kyle E.; Abbott, Lauren J.; McKeown, Neil B.; Colina, Coray M.

doi:10.1021/ma400334b

Cited by 57 publications

(63 citation statements)

References 88 publications

(137 reference statements)

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“…Molecular simulations of PIM-1, using the same force field model used here, have been shown to resemble the physical polymer in properties, such as BET surface area, adsorption isotherms, enthalpies of adsorption, gas selectivities and wide angle X-ray scattering experimental data, in previous works of the authors [ 18 , 26 , 35 , 37 , 46 ]. Moreover, the results of the structural characterization of the PIM-1 (2D) model is in excellent agreement with the average values of the previous 3D periodic PIM-1 simulated samples (“PIM-1 (sims.…”

Section: Molecular Modelingmentioning

confidence: 80%

“…In order to construct an atomistic sample of a slice of an amorphous polymer, the predictive virtual synthesis software, Polymatic [ 34 , 35 ], in conjunction with the LAMMPS simulation package [ 36 ], was used. Polymatic has recently been used to simulate a wide variety of polymeric materials, including porous [ 18 , 37 , 38 , 39 ] and nonporous glassy [ 35 ], linear [ 40 ], networked [ 41 , 42 , 43 ] and composite polymer structures [ 44 ]. One of the benefits of using this procedure is the versatility in designing an environment in which the sample is polymerized.…”

Section: Molecular Modelingmentioning

confidence: 99%

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In Silico Determination of Gas Permeabilities by Non-Equilibrium Molecular Dynamics: CO2 and He through PIM-1

et al. 2015

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We study the permeation dynamics of helium and carbon dioxide through an atomistically detailed model of a polymer of intrinsic microporosity, PIM-1, via non-equilibrium molecular dynamics (NEMD) simulations. This work presents the first explicit molecular modeling of gas permeation through a high free-volume polymer sample, and it demonstrates how permeability and solubility can be obtained coherently from a single simulation. Solubilities in particular can be obtained to a very high degree of confidence and within experimental inaccuracies. Furthermore, the simulations make it possible to obtain very specific information on the diffusion dynamics of penetrant molecules and yield detailed maps of gas occupancy, which are akin to a digital tomographic scan of the polymer network. In addition to determining permeability and solubility directly from NEMD simulations, the results shed light on the permeation mechanism of the penetrant gases, suggesting that the relative openness of the microporous topology promotes the anomalous diffusion of penetrant gases, which entails a deviation from the pore hopping mechanism usually observed in gas diffusion in polymers.

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Section: Molecular Modelingmentioning

confidence: 80%

Section: Molecular Modelingmentioning

confidence: 99%

In Silico Determination of Gas Permeabilities by Non-Equilibrium Molecular Dynamics: CO2 and He through PIM-1

et al. 2015

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“…The above observations demonstrate that the thermal regeneration energy does not correlate strongly with the common used single structural properties. In our previous work (Wu et al, 2012a), a concept of "adsorbility" (AD) was proposed to build the structure-property relationships for MOFs and then successfully by others applied to porous polymeric systems (Hart et al, 2013 "solubility parameter" in solution theory that can be used as an estimate of the compatibility (mutual solubility) of two components in solution. The adsorbility of an adsorbate in a nanoporous material is defined as AD ¼ E ad ¼ Q 0 st =φ, where Q 0 st is the isosteric heat of adsorption at infinite dilution in units of kJ/mol for an adsorbate, and φ is the material's free volume in units of cm 3 /cm 3 , which is also known as the porosity.…”

Section: Structure-separation Performance Relationshipsmentioning

confidence: 99%

Computational exploration of metal–organic frameworks for CO2/CH4 separation via temperature swing adsorption

Xiao

Yang

et al. 2014

Chemical Engineering Science

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“…Pressure swing adsorption (PSA) has been previously proposed as a technology suitable for CH 4 /CO 2 separation typically using a zeolite (e.g., 13X, 4A, or silicalite), metal‐organic framework (MOF), zeolitic imidazolate framework, activated carbon, sepiolite, or polymer as the sorbent. For zeolites and MOFs, for which there exist databases containing thousands of possible candidates, an efficient computational screening procedure is required.…”

Section: Introductionmentioning

confidence: 99%

Discovery of novel zeolites for natural gas purification through combined material screening and process optimization

2014

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in Wiley Online Library (wileyonlinelibrary.com) An efficient computational screening approach is proposed to select the most cost-effective materials and adsorption process conditions for CH 4 /CO 2 separation. The method identifies eight novel zeolites for removing CO 2 from natural gas, coalbed methane, shale gas, enhanced oil recovery gas, biogas, and landfill gas sources. The separation cost is minimized through hierarchical material screening combined with rigorous process modeling and optimization. Minimum purity and recovery constraints of 97 and 95%, respectively, are introduced to meet natural gas pipeline specifications and minimize losses. The top zeolite, WEI, can recover methane as economically as $0.15/MMBTU from natural gas with 5% CO 2 to $1.44/MMBTU from natural gas with 50% CO 2 , showing the potential for developing natural gas reservoirs with higher CO 2 content. The necessity of a combined material selection and process optimization approach is demonstrated by the lack of clear correlation between cost and material-centric metrics such as adsorption selectivity. V C 2014 American Institute of Chemical Engineers AIChE J, 60: 1767-1785, 2014 Keywords: zeolites, adsorption/gas, process synthesis, optimization, computational screening IntroductionThere are vast reserves of natural gas worldwide that are uneconomical to develop due to high CO 2 content, which can be as high as 70% by volume.1 About 10% of natural gas in the United States contains significant quantities of CO 2 that must be removed prior to pipeline transportation to meet the typical specification on CO 2 of 3%.2,3 Typical specifications on composition for U.S. pipelines are provided in Table 1. Even for natural gas sources with low to moderate CO 2 content that is separated before pipeline transport, the CO 2 is often vented into the atmosphere, which contributes to global climate change. In fact, natural gas production is the second-largest source of CO 2 emissions in the United States (after fossil fuel consumption). 5 Even more of an environmental concern is methane, which is the most potent greenhouse gas (GHG) with about 21 times the GHG warming potential than CO 2 . It is, therefore, important to minimize methane losses during natural gas purification for both economic and environmental reasons.Major methane sources in the United States that may require CO 2 separation are illustrated in Figure 1. Shale gas sources typically contain 0-10% CO 2 , but the CO 2 content can increase during the life of a well to up to 30%. 6 Coalbed methane is a type of natural gas found in unmineable coal areas, which is typically extracted through the addition of CO 2 that is selectively adsorbed in the coal bed. As a result, coalbed methane typically contains 30-50% CO 2 . 7 The gases resulting from enhanced oil recovery may contain 20-80% CO 2 in addition to CH 4 . 8 Biogas is the result of anaerobic decomposition of organic waste, such as animal products (e.g., manure), agricultural residues, municipal solid waste, and municipal wastewat...

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Toward Effective CO₂/CH₄ Separations by Sulfur-Containing PIMs via Predictive Molecular Simulations

Cited by 57 publications

References 88 publications

In Silico Determination of Gas Permeabilities by Non-Equilibrium Molecular Dynamics: CO2 and He through PIM-1

In Silico Determination of Gas Permeabilities by Non-Equilibrium Molecular Dynamics: CO2 and He through PIM-1

Computational exploration of metal–organic frameworks for CO2/CH4 separation via temperature swing adsorption

Discovery of novel zeolites for natural gas purification through combined material screening and process optimization

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Toward Effective CO2/CH4 Separations by Sulfur-Containing PIMs via Predictive Molecular Simulations

Cited by 57 publications

References 88 publications

In Silico Determination of Gas Permeabilities by Non-Equilibrium Molecular Dynamics: CO2 and He through PIM-1

In Silico Determination of Gas Permeabilities by Non-Equilibrium Molecular Dynamics: CO2 and He through PIM-1

Computational exploration of metal–organic frameworks for CO2/CH4 separation via temperature swing adsorption

Discovery of novel zeolites for natural gas purification through combined material screening and process optimization

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Toward Effective CO₂/CH₄ Separations by Sulfur-Containing PIMs via Predictive Molecular Simulations