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Title: Understanding Cation Selectivity in Carbon Nanopores with Hybrid First-Principles/Continuum Simulations: Implications for Water Desalination and Separation Technologies

Abstract

Understanding ion adsorption in porous carbons is crucial for a range of technologies, including water desalination and energy storage. In this work, we combined density functional theory with a continuum solvation model to investigate thermodynamics and kinetics of the adsorption process of alkali metal ions from aqueous solutions into carbon nanopores with different sizes and geometries. We found that cations with a larger ionic radius are more favorable to enter the nanopores because of a lower energy penalty of dehydration. In addition, the pore size and geometry were found to have a significant impact on the ion–pore interaction under confinement and cation selectivity. Our study highlights a complex interplay among nanopore geometry, ion size, and hydration on the cation adsorption selectivity, suggesting that tuning the porosity could represent a general strategy for improving ion separations.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1769127
Report Number(s):
LLNL-JRNL-814495
Journal ID: ISSN 2574-0970; 1022783
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Nano Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 10; Journal ID: ISSN 2574-0970
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; density functional theory; continuum solvation model; cation selectivity; nanopore separation

Citation Formats

Zhan, Cheng, Aydin, Fikret, Schwegler, Eric, Noy, Aleksandr, and Pham, Tuan Anh. Understanding Cation Selectivity in Carbon Nanopores with Hybrid First-Principles/Continuum Simulations: Implications for Water Desalination and Separation Technologies. United States: N. p., 2020. Web. doi:10.1021/acsanm.0c01842.
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Zhan, Cheng, Aydin, Fikret, Schwegler, Eric, Noy, Aleksandr, & Pham, Tuan Anh. Understanding Cation Selectivity in Carbon Nanopores with Hybrid First-Principles/Continuum Simulations: Implications for Water Desalination and Separation Technologies. United States. https://doi.org/10.1021/acsanm.0c01842
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Zhan, Cheng, Aydin, Fikret, Schwegler, Eric, Noy, Aleksandr, and Pham, Tuan Anh. Tue . "Understanding Cation Selectivity in Carbon Nanopores with Hybrid First-Principles/Continuum Simulations: Implications for Water Desalination and Separation Technologies". United States. https://doi.org/10.1021/acsanm.0c01842. https://www.osti.gov/servlets/purl/1769127.
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@article{osti_1769127,
title = {Understanding Cation Selectivity in Carbon Nanopores with Hybrid First-Principles/Continuum Simulations: Implications for Water Desalination and Separation Technologies},
author = {Zhan, Cheng and Aydin, Fikret and Schwegler, Eric and Noy, Aleksandr and Pham, Tuan Anh},
abstractNote = {Understanding ion adsorption in porous carbons is crucial for a range of technologies, including water desalination and energy storage. In this work, we combined density functional theory with a continuum solvation model to investigate thermodynamics and kinetics of the adsorption process of alkali metal ions from aqueous solutions into carbon nanopores with different sizes and geometries. We found that cations with a larger ionic radius are more favorable to enter the nanopores because of a lower energy penalty of dehydration. In addition, the pore size and geometry were found to have a significant impact on the ion–pore interaction under confinement and cation selectivity. Our study highlights a complex interplay among nanopore geometry, ion size, and hydration on the cation adsorption selectivity, suggesting that tuning the porosity could represent a general strategy for improving ion separations.},
doi = {10.1021/acsanm.0c01842},
journal = {ACS Applied Nano Materials},
number = 10,
volume = 3,
place = {United States},
year = {Tue Sep 08 00:00:00 EDT 2020},
month = {Tue Sep 08 00:00:00 EDT 2020}
}
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https://doi.org/10.1021/acsanm.0c01842
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