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Monte Carlo Simulations of Framework Defects in Layered Two-Dimensional Nanomaterial Desalination Membranes: Implications for Permeability and Selectivity
Abstract
Two-dimensional nanomaterial (2-D NM) frameworks, especially those comprising graphene oxide, have received extensive research interest for membrane-based separation processes and desalination. However, the impact of horizontal defects in 2-D NM frameworks, which stem from nonuniform deposition of 2-D NM flakes during layer build-up, has been almost entirely overlooked. In this work, we apply Monte Carlo simulations, under idealized conditions wherein the vertical interlayer spacing allows for water permeation while perfectly excluding salt, on both the formation of the laminate structure and molecular transport through the laminate. Our simulations show that 2-D NM frameworks are extremely tortuous (tortuosity ≈103), with water permeability decreasing from 20 to <1 L m-2 h-1 bar-1 as thickness increased from 8 to 167 nm. Additionally, we find that framework defects allow salt to percolate through the framework, hindering water–salt selectivity. 2-D NM frameworks with a packing density of 75%, representative of most 2-D NM membranes, are projected to achieve <92% NaCl rejection at a water permeability of <1 L m-2 h-1 bar-1, even with ideal interlayer spacing. A high packing density of 90%, which to our knowledge has yet to be achieved, could yield comparable performance to current desalination membranes. Maximizing packing density is therefore amore »
- Authors:
-
[1];
[1];
[1];
[1]
- Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). The Center for Enhanced Nanofluidic Transport (CENT); Yale Univ., New Haven, CT (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1515120
- Alternate Identifier(s):
- OSTI ID: 1524336
- Grant/Contract Number:
- SC0019112
- Resource Type:
- Journal Article: Published Article
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Name: Environmental Science and Technology Journal Volume: 53 Journal Issue: 11; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 36 MATERIALS SCIENCE
Citation Formats
Ritt, Cody L., Werber, Jay R., Deshmukh, Akshay, and Elimelech, Menachem. Monte Carlo Simulations of Framework Defects in Layered Two-Dimensional Nanomaterial Desalination Membranes: Implications for Permeability and Selectivity. United States: N. p., 2019.
Web. doi:10.1021/acs.est.8b06880.
Ritt, Cody L., Werber, Jay R., Deshmukh, Akshay, & Elimelech, Menachem. Monte Carlo Simulations of Framework Defects in Layered Two-Dimensional Nanomaterial Desalination Membranes: Implications for Permeability and Selectivity. United States. https://doi.org/10.1021/acs.est.8b06880
Ritt, Cody L., Werber, Jay R., Deshmukh, Akshay, and Elimelech, Menachem. 2019.
"Monte Carlo Simulations of Framework Defects in Layered Two-Dimensional Nanomaterial Desalination Membranes: Implications for Permeability and Selectivity". United States. https://doi.org/10.1021/acs.est.8b06880.
@article{osti_1515120,
title = {Monte Carlo Simulations of Framework Defects in Layered Two-Dimensional Nanomaterial Desalination Membranes: Implications for Permeability and Selectivity},
author = {Ritt, Cody L. and Werber, Jay R. and Deshmukh, Akshay and Elimelech, Menachem},
abstractNote = {Two-dimensional nanomaterial (2-D NM) frameworks, especially those comprising graphene oxide, have received extensive research interest for membrane-based separation processes and desalination. However, the impact of horizontal defects in 2-D NM frameworks, which stem from nonuniform deposition of 2-D NM flakes during layer build-up, has been almost entirely overlooked. In this work, we apply Monte Carlo simulations, under idealized conditions wherein the vertical interlayer spacing allows for water permeation while perfectly excluding salt, on both the formation of the laminate structure and molecular transport through the laminate. Our simulations show that 2-D NM frameworks are extremely tortuous (tortuosity ≈103), with water permeability decreasing from 20 to <1 L m-2 h-1 bar-1 as thickness increased from 8 to 167 nm. Additionally, we find that framework defects allow salt to percolate through the framework, hindering water–salt selectivity. 2-D NM frameworks with a packing density of 75%, representative of most 2-D NM membranes, are projected to achieve <92% NaCl rejection at a water permeability of <1 L m-2 h-1 bar-1, even with ideal interlayer spacing. A high packing density of 90%, which to our knowledge has yet to be achieved, could yield comparable performance to current desalination membranes. Maximizing packing density is therefore a critical technical challenge, in addition to the already daunting challenge of optimizing interlayer spacing, for the development of 2-D NM membranes.},
doi = {10.1021/acs.est.8b06880},
url = {https://www.osti.gov/biblio/1515120},
journal = {Environmental Science and Technology},
issn = {0013-936X},
number = 11,
volume = 53,
place = {United States},
year = {Wed May 08 00:00:00 EDT 2019},
month = {Wed May 08 00:00:00 EDT 2019}
}
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Figures / Tables:
Figure 1: Construction of in silico 2-D nanomaterial frameworks. Randomized deposition of squares is repeated in a layer-by-layer fashion. Salt (as hydrated sodium ions) and water molecules are probed as hard spheres against the framework. Interlayer free spacings were set to 0.5 nm, which is assumed to allow for watermore »
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