Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane-CO2 Mixture in Mesoporous CPG Silica

Sumant Patankar; Siddharth Gautam; Gernot Rother; Andrey Podlesnyak; Georg Ehlers; Tingting Liu; David R. Cole; David L. Tomasko

doi:10.1021/acs.jpcc.5b09984

Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane-CO₂ Mixture in Mesoporous CPG Silica

Sumant Patankar, Siddharth Gautam, Gernot Rother, Andrey Podlesnyak, Georg Ehlers, Tingting Liu, David R. Cole, David L. Tomasko

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Abstract

Ethane is found confined to mineral and organic pores in certain shale formations. Effects of confinement on structural and dynamic properties of ethane in mesoporous controlled pore glass (CPG) were studied by gravimetric adsorption and quasi-elastic neutron scattering (QENS) measurements. The obtained isotherms and scattering data complement each other by quantifying the relative strength of the solid-fluid interactions and the transport properties of the fluid under confinement, respectively. A magnetic suspension balance was used to measure the adsorption isotherms at two temperatures and over a range of pressures corresponding to a bulk density range of 0.01-0.35 g/cm³. Key confinement effects were highlighted through differences between isotherms for the two pore sizes. A comparison was made with previously published isotherms for CO₂ on the same CPG materials. Behavior of ethane in the smaller pore size was probed further using quasi-elastic neutron scattering. By extracting the self-diffusivity and residence time, we were able to study the effect of pressure and transition from gaseous to supercritical densities on the dynamics of confined ethane. A temperature variation QENS study was also completed with pure ethane and a CO₂-ethane mixture. Activation energies extracted from the Arrhenius plots show the effects of CO₂ addition on ethane mobility.

Original language	English
Pages (from-to)	4843-4853
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	120
Issue number	9
DOIs	https://doi.org/10.1021/acs.jpcc.5b09984
State	Published - Mar 10 2016

Funding

S.P., S.G., and T.L. are grateful for the support from the U.S. Department of Energy, Office of Basic Energy Sciences, Geoscience Program under Contract DE-SC0006878. D.R.C. acknowledges support from the A. P. Sloan Foundation Deep Carbon Observatory. The research of G.R. was sponsored by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. SEM images were acquired by Julie Sheets at the Subsurface Energy Materials Characterization and Analysis Laboratory (SEMCAL), School of Earth Sciences, The Ohio State University. Research at Oak Ridge National Laboratory''s Spallation Neutron Source was supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy.

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title = "Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane-CO2 Mixture in Mesoporous CPG Silica",

abstract = "Ethane is found confined to mineral and organic pores in certain shale formations. Effects of confinement on structural and dynamic properties of ethane in mesoporous controlled pore glass (CPG) were studied by gravimetric adsorption and quasi-elastic neutron scattering (QENS) measurements. The obtained isotherms and scattering data complement each other by quantifying the relative strength of the solid-fluid interactions and the transport properties of the fluid under confinement, respectively. A magnetic suspension balance was used to measure the adsorption isotherms at two temperatures and over a range of pressures corresponding to a bulk density range of 0.01-0.35 g/cm3. Key confinement effects were highlighted through differences between isotherms for the two pore sizes. A comparison was made with previously published isotherms for CO2 on the same CPG materials. Behavior of ethane in the smaller pore size was probed further using quasi-elastic neutron scattering. By extracting the self-diffusivity and residence time, we were able to study the effect of pressure and transition from gaseous to supercritical densities on the dynamics of confined ethane. A temperature variation QENS study was also completed with pure ethane and a CO2-ethane mixture. Activation energies extracted from the Arrhenius plots show the effects of CO2 addition on ethane mobility.",

author = "Sumant Patankar and Siddharth Gautam and Gernot Rother and Andrey Podlesnyak and Georg Ehlers and Tingting Liu and Cole, {David R.} and Tomasko, {David L.}",

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AU - Podlesnyak, Andrey

AU - Ehlers, Georg

AU - Liu, Tingting

AU - Cole, David R.

AU - Tomasko, David L.

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Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane-CO₂ Mixture in Mesoporous CPG Silica

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