Effects of water on the stochastic motions of propane confined in MCM-41-S pores
Abstract
Hydrocarbons confined in porous media find applications in a wide variety of industries and therefore their diffusive behavior is widely studied. Most of the porous media found in natural environments are laden with water, which might affect the confined hydrocarbons. To quantify the effect of hydration, we report here a combined quasielastic neutron scattering (QENS) and molecular dynamics (MD) simulation study on the dynamics of propane confined in the 1.5 nm-wide micropores of MCM-41-S in the presence of water at 230 and 250 K. To eliminate the strong incoherent signal from water and emphasize the propane signal we have used heavy water (D2O). QENS data show two dynamically different populations of propane in MCM-41-S and suggest that the presence of water hinders the diffusion of propane. Weak elastic contributions to the QENS spectra suggest that only long-range translational motion of propane molecules contributes to the quasielastic broadening. MD simulations carried out using a model cylindrical silica pore of 1.6 nm diameter filled with water and propane agree with the experimental finding of water hindering the diffusion of propane. Further, the simulation results suggest that the slowing down of propane motions is a function of the water content within the poremore »
- Authors:
-
- The Ohio State Univ., Columbus, OH (United States)
- Univ. College London (UCL), Surrey (United Kingdom)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Nuclear Science Directorate
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1606829
- Alternate Identifier(s):
- OSTI ID: 1573265
- Grant/Contract Number:
- AC05-00OR22725; SC0006878
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP (Print)
- Additional Journal Information:
- Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 21; Journal Issue: 45; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Gautam, Siddharth, Le, Tran Thi Bao, Rother, Gernot, Jalarvo, Niina, Liu, Tingting, Mamontov, Eugene, Dai, Sheng, Qiao, Zhen-An, Striolo, Alberto, and Cole, David. Effects of water on the stochastic motions of propane confined in MCM-41-S pores. United States: N. p., 2019.
Web. doi:10.1039/C9CP04741G.
Gautam, Siddharth, Le, Tran Thi Bao, Rother, Gernot, Jalarvo, Niina, Liu, Tingting, Mamontov, Eugene, Dai, Sheng, Qiao, Zhen-An, Striolo, Alberto, & Cole, David. Effects of water on the stochastic motions of propane confined in MCM-41-S pores. United States. https://doi.org/10.1039/C9CP04741G
Gautam, Siddharth, Le, Tran Thi Bao, Rother, Gernot, Jalarvo, Niina, Liu, Tingting, Mamontov, Eugene, Dai, Sheng, Qiao, Zhen-An, Striolo, Alberto, and Cole, David. Tue .
"Effects of water on the stochastic motions of propane confined in MCM-41-S pores". United States. https://doi.org/10.1039/C9CP04741G. https://www.osti.gov/servlets/purl/1606829.
@article{osti_1606829,
title = {Effects of water on the stochastic motions of propane confined in MCM-41-S pores},
author = {Gautam, Siddharth and Le, Tran Thi Bao and Rother, Gernot and Jalarvo, Niina and Liu, Tingting and Mamontov, Eugene and Dai, Sheng and Qiao, Zhen-An and Striolo, Alberto and Cole, David},
abstractNote = {Hydrocarbons confined in porous media find applications in a wide variety of industries and therefore their diffusive behavior is widely studied. Most of the porous media found in natural environments are laden with water, which might affect the confined hydrocarbons. To quantify the effect of hydration, we report here a combined quasielastic neutron scattering (QENS) and molecular dynamics (MD) simulation study on the dynamics of propane confined in the 1.5 nm-wide micropores of MCM-41-S in the presence of water at 230 and 250 K. To eliminate the strong incoherent signal from water and emphasize the propane signal we have used heavy water (D2O). QENS data show two dynamically different populations of propane in MCM-41-S and suggest that the presence of water hinders the diffusion of propane. Weak elastic contributions to the QENS spectra suggest that only long-range translational motion of propane molecules contributes to the quasielastic broadening. MD simulations carried out using a model cylindrical silica pore of 1.6 nm diameter filled with water and propane agree with the experimental finding of water hindering the diffusion of propane. Further, the simulation results suggest that the slowing down of propane motions is a function of the water content within the pore and is stronger at higher water contents. At high water content, the structure and the dynamics, both translational and rotational, of propane are severely impacted. Simulation data suggest that the rotational motion of the propane molecule occurs on time scales much faster than those accessible with the QENS instrument used, and thus explain the weak elastic contribution to the QENS spectra measured in the experiments. This study shows the effects of hydration on the structure and dynamics of volatiles in porous media, which are of interest for fundamental understanding and applied studies of confined fluids.},
doi = {10.1039/C9CP04741G},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 45,
volume = 21,
place = {United States},
year = {Tue Oct 29 00:00:00 EDT 2019},
month = {Tue Oct 29 00:00:00 EDT 2019}
}
Web of Science
Works referenced in this record:
Location dependent orientational structure and dynamics of ethane in ZSM5
journal, March 2016
- Gautam, Siddharth; Liu, Tingting; Patankar, Sumant
- Chemical Physics Letters, Vol. 648
Rotational dynamics of propane in Na-Y zeolite: A molecular dynamics and quasielastic neutron-scattering study
journal, December 2002
- Mukhopadhyay, R.; Sayeed, Ahmed; Mitra, S.
- Physical Review E, Vol. 66, Issue 6
Molecular Models of Hydroxide, Oxyhydroxide, and Clay Phases and the Development of a General Force Field
journal, January 2004
- Cygan, Randall T.; Liang, Jian-Jie; Kalinichev, Andrey G.
- The Journal of Physical Chemistry B, Vol. 108, Issue 4
Structure and Dynamics of Confined C-O-H Fluids Relevant to the Subsurface: Application of Magnetic Resonance, Neutron Scattering, and Molecular Dynamics Simulations
journal, June 2017
- Gautam, Siddharth S.; Ok, Salim; Cole, David R.
- Frontiers in Earth Science, Vol. 5
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009
- Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming
- Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6
A potential model for the study of ices and amorphous water: TIP4P/Ice
journal, June 2005
- Abascal, J. L. F.; Sanz, E.; García Fernández, R.
- The Journal of Chemical Physics, Vol. 122, Issue 23
Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane–CO 2 Mixture in Mesoporous CPG Silica
journal, February 2016
- Patankar, Sumant; Gautam, Siddharth; Rother, Gernot
- The Journal of Physical Chemistry C, Vol. 120, Issue 9
Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study
journal, January 2019
- Dhiman, I.; Shrestha, U. R.; Bhowmik, D.
- Chemical Physics, Vol. 516
Self‐diffusion in the compressed fluid lower alkanes: Methane, ethane, and propane
journal, April 1991
- Greiner‐Schmid, A.; Wappmann, S.; Has, M.
- The Journal of Chemical Physics, Vol. 94, Issue 8
Confined Water: Structure, Dynamics, and Thermodynamics
journal, August 2017
- Chakraborty, Sudip; Kumar, Hemant; Dasgupta, Chandan
- Accounts of Chemical Research, Vol. 50, Issue 9
Rotational dynamics of propylene in ZSM-5 zeolitic frameworks
journal, January 2011
- Gautam, Siddharth; Sharma, V. K.; Mitra, S.
- Chemical Physics Letters, Vol. 501, Issue 4-6
Molecular dynamics simulations of propane in slit shaped silica nano-pores: direct comparison with quasielastic neutron scattering experiments
journal, January 2017
- Gautam, Siddharth; Le, Thu; Striolo, Alberto
- Physical Chemistry Chemical Physics, Vol. 19, Issue 48
Single-File Diffusion Observation
journal, April 1996
- Hahn, K.; Kärger, J.; Kukla, V.
- Physical Review Letters, Vol. 76, Issue 15
Effect of molecular shape on rotation under severe confinement
journal, April 2018
- Dhiman, I.; Bhowmik, D.; Shrestha, Utsab R.
- Chemical Engineering Science, Vol. 180
Morse Stretch Potential Charge Equilibrium Force Field for Ceramics: Application to the Quartz-Stishovite Phase Transition and to Silica Glass
journal, February 1999
- Demiralp, Ersan; Çağin, Tahir; Goddard, William A.
- Physical Review Letters, Vol. 82, Issue 8
Molecular dynamics simulation study of meso-confined propane in TiO2
journal, September 2015
- Gautam, Siddharth; Cole, David
- Chemical Physics, Vol. 458
Transport Mechanism of Guest Methane in Water-Filled Nanopores
journal, May 2017
- Bui, Tai; Phan, Anh; Cole, David R.
- The Journal of Physical Chemistry C, Vol. 121, Issue 29
Diffusive Motions in Water and Cold Neutron Scattering
journal, August 1960
- Singwi, K. S.; Sjölander, Alf
- Physical Review, Vol. 119, Issue 3
Dynamics of 1,3-butadiene adsorbed in Na-Y zeolite: A molecular dynamics simulation study
journal, June 2008
- Gautam, Siddharth; Mitra, S.; Chaplot, S. L.
- Physical Review E, Vol. 77, Issue 6
N-octane diffusivity enhancement via carbon dioxide in silica slit-shaped nanopores – a molecular dynamics simulation
journal, October 2015
- Le, Thu; Ogbe, Stephanie; Striolo, Alberto
- Molecular Simulation, Vol. 42, Issue 9
Comparison of the dynamics of n-hexane in ZSM-5 and 5A zeolite structures
journal, September 2003
- Stepanov, A. G.; Shegai, T. O.; Luzgin, M. V.
- The European Physical Journal E, Vol. 12, Issue 1
Why is the melting point of propane the lowest among n-alkanes?
journal, January 2000
- Thalladi, Venkat R.; Boese, Roland
- New Journal of Chemistry, Vol. 24, Issue 8
Dependence of the self-diffusion coefficient on the sorbate concentration: A two-dimensional lattice gas model with and without confinement
journal, July 1999
- Bhide, Shreyas Y.; Yashonath, S.
- The Journal of Chemical Physics, Vol. 111, Issue 4
Diffusion of 1,3-butadiene adsorbed in Na–Y zeolite: Neutron scattering study
journal, July 2007
- Gautam, S.; Mitra, S.; Sayeed, A.
- Chemical Physics Letters, Vol. 442, Issue 4-6
Effects of Confinement and Pressure on the Vibrational Behavior of Nano-Confined Propane
journal, July 2018
- Gautam, Siddharth; Kolesnikov, Alexander I.; Rother, Gernot
- The Journal of Physical Chemistry A, Vol. 122, Issue 33
Transferable Potentials for Phase Equilibria. 1. United-Atom Description of n-Alkanes
March 1998
- Martin, Marcus G.; Siepmann, J. Ilja
Water and methane in shale rocks: Flow pattern effects on fluid transport and pore structure
journal, August 2015
- Ho, Tuan A.; Striolo, Alberto
- AIChE Journal, Vol. 61, Issue 9
Confined Water Determines Transport Properties of Guest Molecules in Narrow Pores
journal, July 2016
- Phan, Anh; Cole, David R.; Weiß, R. Gregor
- ACS Nano, Vol. 10, Issue 8
Diffusion of Binary CO 2 /CH 4 Mixtures in the MIL-47(V) and MIL-53(Cr) Metal–Organic Framework Type Solids: A Combination of Neutron Scattering Measurements and Molecular Dynamics Simulations
journal, May 2013
- Salles, Fabrice; Jobic, Hervé; Devic, Thomas
- The Journal of Physical Chemistry C, Vol. 117, Issue 21
Effect of carbon dioxide and nitrogen on the diffusivity of methane confined in nano-porous carbon aerogel
journal, January 2012
- Chathoth, S. M.; He, L.; Mamontov, E.
- Microporous and Mesoporous Materials, Vol. 148, Issue 1
Types of Dependence of Self-Diffusivity on Sorbate Concentration in Parameter Space: A Two-Dimensional Lattice Gas Study †
journal, March 2000
- Bhide, Shreyas Y.; Yashonath, S.
- The Journal of Physical Chemistry B, Vol. 104, Issue 12
Dynamics of Propane in Nanoporous Silica Aerogel: A Quasielastic Neutron Scattering Study
journal, July 2015
- Gautam, Siddharth; Liu, Tingting; Rother, Gernot
- The Journal of Physical Chemistry C, Vol. 119, Issue 32
A smooth particle mesh Ewald method
journal, November 1995
- Essmann, Ulrich; Perera, Lalith; Berkowitz, Max L.
- The Journal of Chemical Physics, Vol. 103, Issue 19
Confined Water as Model of Supercooled Water
journal, March 2016
- Cerveny, Silvina; Mallamace, Francesco; Swenson, Jan
- Chemical Reviews, Vol. 116, Issue 13
Structure and Dynamics of Zeolites Investigated by Molecular Dynamics
journal, December 1997
- Demontis, Pierfranco; Suffritti, Giuseppe B.
- Chemical Reviews, Vol. 97, Issue 8
Dynamics of Adsorbed Hydrocarbon in Nanoporous Zeolite Framework
journal, June 2009
- Sharma, V. K.; Gautam, S.; Mitra, S.
- The Journal of Physical Chemistry B, Vol. 113, Issue 23
CO 2 –C 4 H 10 Mixtures Simulated in Silica Slit Pores: Relation between Structure and Dynamics
journal, June 2015
- Le, Thu; Striolo, Alberto; Cole, David R.
- The Journal of Physical Chemistry C, Vol. 119, Issue 27
Propane simulated in silica pores: Adsorption isotherms, molecular structure, and mobility
journal, January 2015
- Le, Thu; Striolo, Alberto; Cole, David R.
- Chemical Engineering Science, Vol. 121
Propane–Water Mixtures Confined within Cylindrical Silica Nanopores: Structural and Dynamical Properties Probed by Molecular Dynamics
journal, September 2017
- Le, Tran Thi Bao; Striolo, Alberto; Gautam, Siddharth S.
- Langmuir, Vol. 33, Issue 42
Diffusion of acetylene inside zeolite: Molecular dynamics simulation studies
journal, October 2006
- Gautam, Siddharth; Mitra, S.; Mukhopadhyay, R.
- Physical Review E, Vol. 74, Issue 4
A time-of-flight backscattering spectrometer at the Spallation Neutron Source, BASIS
journal, August 2011
- Mamontov, E.; Herwig, K. W.
- Review of Scientific Instruments, Vol. 82, Issue 8
Diffusion and adsorption of methane confined in nano-porous carbon aerogel: A combined quasi-elastic and small-angle neutron scattering study
journal, July 2010
- Chathoth, Suresh M.; Mamontov, Eugene; Melnichenko, Yuri B.
- Microporous and Mesoporous Materials, Vol. 132, Issue 1-2