Thermodynamics and Kinetics of Gas Storage in Porous Liquids

Fei Zhang; Fengchang Yang; Jingsong Huang; Bobby G. Sumpter; Rui Qiao

doi:10.1021/acs.jpcb.6b04784

Thermodynamics and Kinetics of Gas Storage in Porous Liquids

Fei Zhang, Fengchang Yang, Jingsong Huang, Bobby G. Sumpter, Rui Qiao

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68 Scopus citations

Abstract

The recent synthesis of organic molecular liquids with permanent porosity opens up exciting new avenues for gas capture, storage, and separation. Using molecular simulations, we study the thermodynamics and kinetics for the storage of CH₄, CO₂, and N₂ molecules in porous liquids consisting of crown-ether-substituted cage molecules in a 15-crown-5 solvent. It is found that the intrinsic gas storage capacity per cage molecule follows the order CH₄ > CO₂ > N₂, which does not correlate simply with the size of gas molecules. Different gas molecules are stored inside the cage differently; e.g., CO₂ molecules prefer the cage's core whereas CH₄ molecules favor both the core and the branch regions. All gas molecules considered can enter the cage essentially without energy barriers and leave the cage on a nanosecond time scale by overcoming a modest energy penalty. The molecular mechanisms of these observations are clarified.

Original language	English
Pages (from-to)	7195-7200
Number of pages	6
Journal	Journal of Physical Chemistry B
Volume	120
Issue number	29
DOIs	https://doi.org/10.1021/acs.jpcb.6b04784
State	Published - Jul 28 2016

Funding

We thank the ARC at Virginia Tech for generous allocations of computer time on the NewRiver cluster. R.Q. was partially supported by an appointment to the HERE program for faculty at the Oak Ridge National Laboratory administered by ORISE. J.H. acknowledges work performed at the Center for Nanophase Materials Sciences, a US DOE Office of Science User Facility. B.G.S. acknowledges support from the Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences.

Funders	Funder number
ARC at Virginia Tech
Center for Nanophase Materials Sciences
Center for Understanding and Control of Acid
HERE
U.S. Department of Energy
Office of Science
Basic Energy Sciences

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title = "Thermodynamics and Kinetics of Gas Storage in Porous Liquids",

abstract = "The recent synthesis of organic molecular liquids with permanent porosity opens up exciting new avenues for gas capture, storage, and separation. Using molecular simulations, we study the thermodynamics and kinetics for the storage of CH4, CO2, and N2 molecules in porous liquids consisting of crown-ether-substituted cage molecules in a 15-crown-5 solvent. It is found that the intrinsic gas storage capacity per cage molecule follows the order CH4 > CO2 > N2, which does not correlate simply with the size of gas molecules. Different gas molecules are stored inside the cage differently; e.g., CO2 molecules prefer the cage's core whereas CH4 molecules favor both the core and the branch regions. All gas molecules considered can enter the cage essentially without energy barriers and leave the cage on a nanosecond time scale by overcoming a modest energy penalty. The molecular mechanisms of these observations are clarified.",

author = "Fei Zhang and Fengchang Yang and Jingsong Huang and Sumpter, {Bobby G.} and Rui Qiao",

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AU - Zhang, Fei

AU - Yang, Fengchang

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AU - Qiao, Rui

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AB - The recent synthesis of organic molecular liquids with permanent porosity opens up exciting new avenues for gas capture, storage, and separation. Using molecular simulations, we study the thermodynamics and kinetics for the storage of CH4, CO2, and N2 molecules in porous liquids consisting of crown-ether-substituted cage molecules in a 15-crown-5 solvent. It is found that the intrinsic gas storage capacity per cage molecule follows the order CH4 > CO2 > N2, which does not correlate simply with the size of gas molecules. Different gas molecules are stored inside the cage differently; e.g., CO2 molecules prefer the cage's core whereas CH4 molecules favor both the core and the branch regions. All gas molecules considered can enter the cage essentially without energy barriers and leave the cage on a nanosecond time scale by overcoming a modest energy penalty. The molecular mechanisms of these observations are clarified.

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Thermodynamics and Kinetics of Gas Storage in Porous Liquids

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