Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Effect of pore density on gas permeation through nanoporous graphene membranes

Abstract

Pore density is an important factor dictating gas separations through one-atom-thin nanoporous membranes, but how it influences the gas permeation is not fully understood. We use molecular dynamics (MD) simulations to investigate gas permeation through nanoporous graphene membranes with the same pore size (3.0 Å × 3.8 Å in dimensions) but varying pore densities (from 0.01 to 1.28 nm-2). We find that higher pore density leads to higher permeation per unit area of membrane for both CO2 and He, but the rate of the increase decreases greatly for CO2 at high pore densities. As a result, the per-pore permeance decreases for CO2 but remains relatively constant for He with the pore density, leading to a dramatic change in CO2/He selectivity. By separating the total flux into direct flux and surface flux, we find that He permeation is dominated by direct flux and hence the per-pore permeation rate is roughly constant with the pore density. In contrast, CO2 permeation is dominated by surface flux and the overall decreasing trend of the per-pore permeation rate of CO2 with the pore density can be explained by the decreasing per-pore coverage of CO2 on the feed side with the pore density. Finally, our workmore » now provides a complete picture of the pore-density dependence of gas permeation through one-atom-thin nanoporous membranes.« less

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  2. Chinese Academy of Sciences (CAS), Ningbo (China). Ningbo Inst. of Materials Technology and Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of California, Riverside, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1479714
Alternate Identifier(s):
OSTI ID: 1461213
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 10; Journal Issue: 30; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wang, Song, Tian, Ziqi, Dai, Sheng, and Jiang, De-en. Effect of pore density on gas permeation through nanoporous graphene membranes. United States: N. p., 2018. Web. doi:10.1039/C8NR02625D.
Copy to clipboard
Wang, Song, Tian, Ziqi, Dai, Sheng, & Jiang, De-en. Effect of pore density on gas permeation through nanoporous graphene membranes. United States. https://doi.org/10.1039/C8NR02625D
Copy to clipboard
Wang, Song, Tian, Ziqi, Dai, Sheng, and Jiang, De-en. Wed . "Effect of pore density on gas permeation through nanoporous graphene membranes". United States. https://doi.org/10.1039/C8NR02625D. https://www.osti.gov/servlets/purl/1479714.
Copy to clipboard
@article{osti_1479714,
title = {Effect of pore density on gas permeation through nanoporous graphene membranes},
author = {Wang, Song and Tian, Ziqi and Dai, Sheng and Jiang, De-en},
abstractNote = {Pore density is an important factor dictating gas separations through one-atom-thin nanoporous membranes, but how it influences the gas permeation is not fully understood. We use molecular dynamics (MD) simulations to investigate gas permeation through nanoporous graphene membranes with the same pore size (3.0 Å × 3.8 Å in dimensions) but varying pore densities (from 0.01 to 1.28 nm-2). We find that higher pore density leads to higher permeation per unit area of membrane for both CO2 and He, but the rate of the increase decreases greatly for CO2 at high pore densities. As a result, the per-pore permeance decreases for CO2 but remains relatively constant for He with the pore density, leading to a dramatic change in CO2/He selectivity. By separating the total flux into direct flux and surface flux, we find that He permeation is dominated by direct flux and hence the per-pore permeation rate is roughly constant with the pore density. In contrast, CO2 permeation is dominated by surface flux and the overall decreasing trend of the per-pore permeation rate of CO2 with the pore density can be explained by the decreasing per-pore coverage of CO2 on the feed side with the pore density. Finally, our work now provides a complete picture of the pore-density dependence of gas permeation through one-atom-thin nanoporous membranes.},
doi = {10.1039/C8NR02625D},
journal = {Nanoscale},
number = 30,
volume = 10,
place = {United States},
year = {Wed Jul 18 00:00:00 EDT 2018},
month = {Wed Jul 18 00:00:00 EDT 2018}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/C8NR02625D
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 28 works
Citation information provided by
Web of Science

Figures / Tables:

Fig.1 Fig.1: The 10×10 nm2 porous-graphene membrane with different numbers of the same pore (3.0 Å ×3.8 Å in size): (a) 1; (b) 2; (c) 4; (d) 8; (e) 16; (f) 32; (g) 64; (h) 128. They correspond to pore densities from 0.01 (a) nm-2 to 1.28 nm-2 (h). Side viewmore » of the bi-chamber setup (i) for simulating gas permeation through the membrane in the middle; the upper chamber (the feed side) is pressurized at 20 atm while the lower chamber (the permeate side) is vacuum initially.« less
All figures and tables (9 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Ab Initio Calculations for Helium: A Standard for Transport Property Measurements
journal, February 1995

Water Transport through Ultrathin Graphene
journal, April 2010

  • Suk, Myung E.; Aluru, N. R.
  • The Journal of Physical Chemistry Letters, Vol. 1, Issue 10, p. 1590-1594
  • DOI: 10.1021/jz100240r

Graphene Oxide Membranes for Ionic and Molecular Sieving
journal, February 2014

Fast Mass Transport Through Sub-2-Nanometer Carbon Nanotubes
journal, May 2006

Permeance of H2 through porous graphene from molecular dynamics
journal, December 2013

Ultrathin, Molecular-Sieving Graphene Oxide Membranes for Selective Hydrogen Separation
journal, October 2013

Mechanisms of Gas Permeation through Single Layer Graphene Membranes
journal, November 2012

  • Drahushuk, Lee W.; Strano, Michael S.
  • Langmuir, Vol. 28, Issue 48
  • DOI: 10.1021/la303468r

Insights into CO2/N2 separation through nanoporous graphene from molecular dynamics
journal, January 2013

  • Liu, Hongjun; Dai, Sheng; Jiang, De-en
  • Nanoscale, Vol. 5, Issue 20
  • DOI: 10.1039/c3nr02852f

Two-Dimensional-Material Membranes: A New Family of High-Performance Separation Membranes
journal, July 2016

  • Liu, Gongping; Jin, Wanqin; Xu, Nanping
  • Angewandte Chemie International Edition, Vol. 55, Issue 43, p. 13384-13397
  • DOI: 10.1002/anie.201600438

Water desalination using nanoporous single-layer graphene
journal, March 2015

  • Surwade, Sumedh P.; Smirnov, Sergei N.; Vlassiouk, Ivan V.
  • Nature Nanotechnology, Vol. 10, Issue 5
  • DOI: 10.1038/nnano.2015.37

Carbon Dioxide Separation with a Two-Dimensional Polymer Membrane
journal, June 2012

  • Schrier, Joshua
  • ACS Applied Materials & Interfaces, Vol. 4, Issue 7
  • DOI: 10.1021/am300867d

Expanded Porphyrins as Two-Dimensional Porous Membranes for CO 2 Separation
journal, March 2015

  • Tian, Ziqi; Dai, Sheng; Jiang, De-en
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 23
  • DOI: 10.1021/acsami.5b03275

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Plasticization-Enhanced Hydrogen Purification Using Polymeric Membranes
journal, February 2006

Ewald summation for systems with slab geometry
journal, August 1999

  • Yeh, In-Chul; Berkowitz, Max L.
  • The Journal of Chemical Physics, Vol. 111, Issue 7
  • DOI: 10.1063/1.479595

Molecular Dynamics Simulations of Helium Permeation in Polyimides with a Bulky Dianhydride and a Fluorinated Diamine
journal, July 2007

Ion transport through a graphene nanopore
journal, September 2012

Activated carbon for gas separation and storage
journal, January 1996

Simulations of non-neutral slab systems with long-range electrostatic interactions in two-dimensional periodic boundary conditions
journal, January 2009

  • Ballenegger, V.; Arnold, A.; Cerdà, J. J.
  • The Journal of Chemical Physics, Vol. 131, Issue 9
  • DOI: 10.1063/1.3216473

Graphene-based materials: Synthesis and gas sorption, storage and separation
journal, April 2015

Canonical dynamics: Equilibrium phase-space distributions
journal, March 1985

Graphene-based membranes
journal, January 2015

  • Liu, Gongping; Jin, Wanqin; Xu, Nanping
  • Chemical Society Reviews, Vol. 44, Issue 15
  • DOI: 10.1039/C4CS00423J

Selectivity trend of gas separation through nanoporous graphene
journal, April 2015

Helium Tunneling through Nitrogen-Functionalized Graphene Pores: Pressure- and Temperature-Driven Approaches to Isotope Separation
journal, May 2012

  • Hauser, Andreas W.; Schrier, Joshua; Schwerdtfeger, Peter
  • The Journal of Physical Chemistry C, Vol. 116, Issue 19
  • DOI: 10.1021/jp302498d

Selective Gas Transport Through Few-Layered Graphene and Graphene Oxide Membranes
journal, October 2013

Two-dimensional graphene-like C 2 N: an experimentally available porous membrane for hydrogen purification
journal, January 2015

  • Xu, B.; Xiang, H.; Wei, Q.
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 23
  • DOI: 10.1039/C5CP01789K

Bottom-up synthesis of multifunctional nanoporous graphene
journal, April 2018

Mechanism and Prediction of Gas Permeation through Sub-Nanometer Graphene Pores: Comparison of Theory and Simulation
journal, July 2017

Water Desalination across Nanoporous Graphene
journal, June 2012

  • Cohen-Tanugi, David; Grossman, Jeffrey C.
  • Nano Letters, Vol. 12, Issue 7, p. 3602-3608
  • DOI: 10.1021/nl3012853

Porous Graphene as the Ultimate Membrane for Gas Separation
journal, December 2009

  • Jiang, De-en; Cooper, Valentino R.; Dai, Sheng
  • Nano Letters, Vol. 9, Issue 12, p. 4019-4024
  • DOI: 10.1021/nl9021946

Synthetic Two-Dimensional Materials: A New Paradigm of Membranes for Ultimate Separation
journal, May 2016

  • Zheng, Zhikun; Grünker, Ronny; Feng, Xinliang
  • Advanced Materials, Vol. 28, Issue 31
  • DOI: 10.1002/adma.201506237

A review on the latest development of carbon membranes for gas separation
journal, October 2001

Asymmetrically Decorated, Doped Porous Graphene As an Effective Membrane for Hydrogen Isotope Separation
journal, March 2012

  • Hankel, Marlies; Jiao, Yan; Du, Aijun
  • The Journal of Physical Chemistry C, Vol. 116, Issue 11
  • DOI: 10.1021/jp211930a

A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984

  • Nosé, Shuichi
  • The Journal of Chemical Physics, Vol. 81, Issue 1
  • DOI: 10.1063/1.447334

Nanoporous Graphene Membranes for Efficient 3 He/ 4 He Separation
journal, January 2012

  • Hauser, Andreas W.; Schwerdtfeger, Peter
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 2
  • DOI: 10.1021/jz201504k

Mechanisms of Molecular Permeation through Nanoporous Graphene Membranes
journal, January 2014

  • Sun, Chengzhen; Boutilier, Michael S. H.; Au, Harold
  • Langmuir, Vol. 30, Issue 2
  • DOI: 10.1021/la403969g

Selective molecular sieving through porous graphene
journal, October 2012

  • Koenig, Steven P.; Wang, Luda; Pellegrino, John
  • Nature Nanotechnology, Vol. 7, Issue 11
  • DOI: 10.1038/nnano.2012.162

Selective Ion Passage through Functionalized Graphene Nanopores
journal, December 2008

  • Sint, Kyaw; Wang, Boyang; Král, Petr
  • Journal of the American Chemical Society, Vol. 130, Issue 49, p. 16448-16449
  • DOI: 10.1021/ja804409f

MXene molecular sieving membranes for highly efficient gas separation
journal, January 2018

Designing the Next Generation of Chemical Separation Membranes
journal, May 2011

Transport of Water and Ions through a Graphene Nanopore in an Electric Field
journal, February 2017

Amorphization-induced surface electronic states modulation of cobaltous oxide nanosheets for lithium-sulfur batteries
journal, May 2021

MXene molecular sieving membranes for highly efficient gas separation
other, January 2018

  • Ding, Li; Wei, Yanying; Li, Libo
  • London : Nature Publishing Group
  • DOI: 10.15488/3192

Selective Ion Passage through Functionalized Graphene Nanopores
journal, July 2009

  • Sint, Kyaw; Wang, Boyang; Král, Petr
  • Journal of the American Chemical Society, Vol. 131, Issue 27
  • DOI: 10.1021/ja903655u

Computer Simulation Using Particles
book, January 1988

Computer Simulation Using Particles
book, January 1988

Selective Molecular Sieving through Porous Graphene
text, January 2012

Ion transport through a graphene nanopore
text, January 2013

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Adsorption-assisted transport of water vapour in super-hydrophobic membranes filled with multilayer graphene platelets
    journal, January 2019

    • Gontarek, E.; Macedonio, F.; Militano, F.
    • Nanoscale, Vol. 11, Issue 24
    • DOI: 10.1039/c9nr02581b
      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Fig.1 (p. 4)figure
      Fig. 2 (p. 5)figure
      Fig. 3 (p. 6)figure
      Fig. 4 (p. 7)figure
      Fig. 5 (p. 8)figure
      Fig. 6 (p. 8)figure
      Fig. 7 (p. 9)figure
      Fig. 8 (p. 10)figure
      Fig. 9 (p. 11)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: