Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study

Dhiman, Indu; Shrestha, Utsab R.; Bhowmik, Debsindhu; Cole, David; Gautam, Siddharth

doi:10.1016/j.chemphys.2018.08.033

Title: Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study

Abstract

In this study, we have investigated the effect of molecular shape and charge asymmetry on the translation dynamics of confined hydrocarbon molecules having different shapes but similar kinetic diameters, inside ZSM-5 pores using molecular dynamics simulations. The mean square displacement of propane, acetonitrile, acetaldehyde, and acetone in ZSM-5 exhibit two different regimes – ballistic and diffusive/sub-diffusive. All the molecules except propane exhibit sub-diffusive motion at time scales greater than 1 ps. The intermediate scattering functions reveal that there is a considerable rotational-translational coupling in the motion of all the molecules, due to the strong geometrical restriction imposed by ZSM-5. Overall the difference in shape and asymmetry in charge imposes severe restriction inside the ZSM-5 channels for all the molecules to different extents. Additionally, the behavior of molecules confined in ZSM-5 in the present study, quantified wherever possible, is compared to their behavior in bulk or in other porous media reported in literature.

Authors:

^[1];

^[2];

^[3]; Cole, David ^[4]; Gautam, Siddharth ^[4]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics, Biosciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computational Science and Engineering Division
The Ohio State Univ., Columbus, OH (United States). School of Earth Sciences

Publication Date:: Fri Aug 24 00:00:00 EDT 2018

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

OSTI Identifier:: 1474635

Alternate Identifier(s):: OSTI ID: 1701971

Grant/Contract Number:: AC05-00OR22725; SC0006878

Resource Type:: Accepted Manuscript

Journal Name:: Chemical Physics

Additional Journal Information:: Journal Volume: 516; Journal Issue: C; Journal ID: ISSN 0301-0104

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Dhiman, Indu, Shrestha, Utsab R., Bhowmik, Debsindhu, Cole, David, and Gautam, Siddharth. Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study.  United States: N. p., 2018. 
Web.  doi:10.1016/j.chemphys.2018.08.033.

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                    Dhiman, Indu, Shrestha, Utsab R., Bhowmik, Debsindhu, Cole, David, & Gautam, Siddharth. Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study.  United States.  https://doi.org/10.1016/j.chemphys.2018.08.033

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                    Dhiman, Indu, Shrestha, Utsab R., Bhowmik, Debsindhu, Cole, David, and Gautam, Siddharth. Fri .  
"Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study".  United States.  https://doi.org/10.1016/j.chemphys.2018.08.033.  https://www.osti.gov/servlets/purl/1474635.

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@article{osti_1474635,

  title        = {Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study},

  author       = {Dhiman, Indu and Shrestha, Utsab R. and Bhowmik, Debsindhu and Cole, David and Gautam, Siddharth},

  abstractNote = {In this study, we have investigated the effect of molecular shape and charge asymmetry on the translation dynamics of confined hydrocarbon molecules having different shapes but similar kinetic diameters, inside ZSM-5 pores using molecular dynamics simulations. The mean square displacement of propane, acetonitrile, acetaldehyde, and acetone in ZSM-5 exhibit two different regimes – ballistic and diffusive/sub-diffusive. All the molecules except propane exhibit sub-diffusive motion at time scales greater than 1 ps. The intermediate scattering functions reveal that there is a considerable rotational-translational coupling in the motion of all the molecules, due to the strong geometrical restriction imposed by ZSM-5. Overall the difference in shape and asymmetry in charge imposes severe restriction inside the ZSM-5 channels for all the molecules to different extents. Additionally, the behavior of molecules confined in ZSM-5 in the present study, quantified wherever possible, is compared to their behavior in bulk or in other porous media reported in literature.},

  doi          = {10.1016/j.chemphys.2018.08.033},

  journal      = {Chemical Physics},

  number       = C,

  volume       = 516,

  place        = {United States},

  year         = {Fri Aug 24 00:00:00 EDT 2018},

  month        = {Fri Aug 24 00:00:00 EDT 2018}

}

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Works referencing / citing this record:

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journal, January 2019

Gautam, Siddharth; Le, Tran Thi Bao; Rother, Gernot
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Title: Influence of molecular shape on self-diffusion under severe confinement: A molecular dynamics study

Abstract

Citation Formats

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Unidirectional and Single-File Diffusion of Molecules in One-Dimensional Channel Systems. A Quasi-Elastic Neutron Scattering Study journal, July 1997

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Diffusion of Propane in Zeolite NaY: A Molecular Dynamics and Quasi-Elastic Neutron Scattering Study journal, January 2003

Diffusion of acetylene inside Na − Y zeolite: Molecular dynamics simulation studies journal, October 2006

Rotational dynamics of propane in Na-Y zeolite: A molecular dynamics and quasielastic neutron-scattering study journal, December 2002

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Dynamics of 1,3-butadiene adsorbed in Na-Y zeolite: A molecular dynamics simulation study journal, June 2008

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QENS and FTIR studies on binding states of benzene molecules adsorbed in zeolite HZSM-5 at room temperature journal, January 2001

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Acetylene diffusion in Na-Y zeolite journal, August 2004

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Molecular dynamics studies on zeolites. 4. Diffusion of methane in silicalite journal, May 1990

Molecular Dynamics Simulations of Alkanes in the Zeolite Silicalite: Evidence for Resonant Diffusion Effects journal, August 1997

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Location dependent orientational structure and dynamics of ethane in ZSM5 journal, March 2016

Molecular dynamics simulation of ethene diffusion in MFI and H[Al]ZSM-5 journal, November 1999

Investigation of a Nanocomposite of 75 wt % Poly(methyl methacrylate) Nanoparticles with 25 wt % Poly(ethylene oxide) Linear Chains: A Quasielatic Neutron Scattering, Calorimetric, and WAXS Study journal, April 2014

Single Chain Dynamic Structure Factor of Linear Polymers in an All-Polymer Nano-Composite journal, March 2016

Effects of pressure on the dynamics of an oligomeric protein from deep-sea hyperthermophile journal, October 2015

Enhanced Dynamics of Hydrated tRNA on Nanodiamond Surfaces: A Combined Neutron Scattering and MD Simulation Study journal, September 2016

Molecular dynamics simulations of propane in slit shaped silica nano-pores: direct comparison with quasielastic neutron scattering experiments journal, January 2017

Rotation driven translational diffusion of polyatomic ions in water: A novel mechanism for breakdown of Stokes-Einstein relation journal, April 2017

Effect of molecular shape on rotation under severe confinement journal, April 2018

Dynamics of Propane in Nanoporous Silica Aerogel: A Quasielastic Neutron Scattering Study journal, July 2015

Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane–CO 2 Mixture in Mesoporous CPG Silica journal, February 2016

Self‐diffusion in the compressed fluid lower alkanes: Methane, ethane, and propane journal, April 1991

Self-diffusion in liquid acetonitrile under pressure journal, January 1982

Self-diffusion and viscosity of some liquids as a function of temperature journal, November 1973

Estimation of Diffusion Coefficients in Acetone−Cellulose Acetate Solutions journal, September 1999

Properties of liquid acetone in silica pores: Molecular dynamics simulation journal, April 1996

Effects of water on the stochastic motions of propane confined in MCM-41-S pores journal, January 2019

Sorption, Structure and Dynamics of CO2 and Ethane in Silicalite at High Pressure: A Combined Monte Carlo and Molecular Dynamics Simulation Study journal, December 2018

Mass transfer in mesoporous materials: the benefit of microscopic diffusion measurement
journal, January 2013

Structural and dynamical properties of guest molecules confined in mesoporous silica materials revealed by NMR
journal, January 2007

Hydrogen Storage in Single-Walled Carbon Nanotubes at Room Temperature
journal, November 1999

DNA-assisted dispersion and separation of carbon nanotubes
journal, April 2003

Nanopores and nucleic acids: prospects for ultrarapid sequencing
journal, April 2000

Single Carbon Nanotube Membranes: A Well-Defined Model for Studying Mass Transport through Nanoporous Materials
journal, December 2000

Capillarity-induced filling of carbon nanotubes
journal, January 1993

Carbon nanotubes as removable templates for metal oxide nanocomposites and nanostructures
journal, June 1995

Rotational dynamics of propylene in ZSM-5 zeolitic frameworks
journal, January 2011

Towards a molecular understanding of shape selectivity
journal, February 2008

Nanogeochemistry: Geochemical reactions and mass transfers in nanopores
journal, January 2003

Thickness trends and sequence stratigraphy of the Middle Devonian Marcellus Formation, Appalachian Basin: Implications for Acadian foreland basin evolution
journal, January 2011

Unidirectional and Single-File Diffusion of Molecules in One-Dimensional Channel Systems. A Quasi-Elastic Neutron Scattering Study
journal, July 1997

Single-file diffusion and reaction in zeolites
journal, August 1992

Diffusion of Propane in Zeolite NaY: A Molecular Dynamics and Quasi-Elastic Neutron Scattering Study
journal, January 2003

Diffusion of acetylene inside $Na − Y$ zeolite: Molecular dynamics simulation studies
journal, October 2006

Rotational dynamics of propane in Na-Y zeolite: A molecular dynamics and quasielastic neutron-scattering study
journal, December 2002

Diffusion of acetylene embedded in Na–Y zeolite: QENS and MD simulation studies
journal, November 2006

Dynamics of 1,3-butadiene adsorbed in Na-Y zeolite: A molecular dynamics simulation study
journal, June 2008

Effect of pore characteristics on the dynamics of cyclohexane molecules confined in ZSM-5 and MCM-41 molecular sieves: FTIR and QENS study
journal, January 2003

QENS and FTIR studies on binding states of benzene molecules adsorbed in zeolite HZSM-5 at room temperature
journal, January 2001

Molecular motions of benzene adsorbed in ZSM-5 zeolite: quasielastic neutron scattering study
journal, December 2002

Acetylene diffusion in Na-Y zeolite
journal, August 2004

Mobility of adsorbed species in zeolites: a molecular dynamics simulation of xenon in silicalite
journal, February 1990

Molecular dynamics studies on zeolites. 4. Diffusion of methane in silicalite
journal, May 1990

Molecular Dynamics Simulations of Alkanes in the Zeolite Silicalite: Evidence for Resonant Diffusion Effects
journal, August 1997

Diffusion of propylene adsorbed in Na-Y and Na-ZSM5 zeolites: Neutron scattering and FTIR studies
journal, November 2008

Shape Selectivity in Hydrocarbon Conversion
journal, February 2001

Nanofiltration as a treatment method for the removal of pesticides from ground waters
journal, September 1998

Influence of molecular size, polarity and charge on the retention of organic molecules by nanofiltration
journal, April 1999

Study of tetrabutylammonium bromide in aqueous solution by neutron scattering
journal, November 2012

Effect of solute geometry and orientation on the rejection of uncharged compounds by nanofiltration
journal, June 2006

Why is the melting point of propane the lowest among n-alkanes?
journal, January 2000

Transferable Potentials for Phase Equilibria. 1. United-Atom Description of n-Alkanes
March 1998

DL_POLY_3: new dimensions in molecular dynamics simulations via massive parallelism
journal, January 2006

On the location and disorder of the tetrapropylammonium (TPA) ion in zeolite ZSM-5 with improved framework accuracy
journal, April 1987

Does lattice vibration drive diffusion in zeolites?
journal, February 2001

Molecular dynamics studies on zeolites. 6. Temperature dependence of diffusion of methane in silicalite
journal, February 1992

Study of Translational and Rotational Mobility and Orientational Preference of Ethane in One-Dimensional Channels
journal, August 2002

Location dependent orientational structure and dynamics of ethane in ZSM5
journal, March 2016

Molecular dynamics simulation of ethene diffusion in MFI and H[Al]ZSM-5
journal, November 1999

Investigation of a Nanocomposite of 75 wt % Poly(methyl methacrylate) Nanoparticles with 25 wt % Poly(ethylene oxide) Linear Chains: A Quasielatic Neutron Scattering, Calorimetric, and WAXS Study
journal, April 2014

Single Chain Dynamic Structure Factor of Linear Polymers in an All-Polymer Nano-Composite
journal, March 2016

Effects of pressure on the dynamics of an oligomeric protein from deep-sea hyperthermophile
journal, October 2015

Enhanced Dynamics of Hydrated tRNA on Nanodiamond Surfaces: A Combined Neutron Scattering and MD Simulation Study
journal, September 2016

Molecular dynamics simulations of propane in slit shaped silica nano-pores: direct comparison with quasielastic neutron scattering experiments
journal, January 2017

Rotation driven translational diffusion of polyatomic ions in water: A novel mechanism for breakdown of Stokes-Einstein relation
journal, April 2017

Effect of molecular shape on rotation under severe confinement
journal, April 2018

Dynamics of Propane in Nanoporous Silica Aerogel: A Quasielastic Neutron Scattering Study
journal, July 2015

Role of Confinement on Adsorption and Dynamics of Ethane and an Ethane–CO ₂ Mixture in Mesoporous CPG Silica
journal, February 2016

Self‐diffusion in the compressed fluid lower alkanes: Methane, ethane, and propane
journal, April 1991

Self-diffusion in liquid acetonitrile under pressure
journal, January 1982

Self-diffusion and viscosity of some liquids as a function of temperature
journal, November 1973

Estimation of Diffusion Coefficients in Acetone−Cellulose Acetate Solutions
journal, September 1999

Properties of liquid acetone in silica pores: Molecular dynamics simulation
journal, April 1996

Effects of water on the stochastic motions of propane confined in MCM-41-S pores
journal, January 2019

Sorption, Structure and Dynamics of CO2 and Ethane in Silicalite at High Pressure: A Combined Monte Carlo and Molecular Dynamics Simulation Study
journal, December 2018