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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 CO 2 and He, but the rate of the increase decreases greatly for CO 2 at high pore densities. As a result, the per-pore permeance decreases for CO 2 but remains relatively constant for He with the pore density, leading to a dramatic change in CO 2/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, CO 2 permeation is dominated by surface flux and the overall decreasing trend of the per-pore permeation rate of CO 2 with the pore density can be explained by the decreasing per-pore coverage of CO 2 on the feedmore » 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.« less

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [1]
  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 Lab. (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:
Journal Article: 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.
Wang, Song, Tian, Ziqi, Dai, Sheng, & Jiang, De-en. Effect of pore density on gas permeation through nanoporous graphene membranes. United States. doi:10.1039/C8NR02625D.
Wang, Song, Tian, Ziqi, Dai, Sheng, and Jiang, De-en. Wed . "Effect of pore density on gas permeation through nanoporous graphene membranes". United States. doi:10.1039/C8NR02625D. https://www.osti.gov/servlets/purl/1479714.
@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},
issn = {2040-3364},
number = 30,
volume = 10,
place = {United States},
year = {2018},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 2 works
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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

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.