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Title: Intrapore energy barriers govern ion transport and selectivity of desalination membranes

Abstract

State-of-the-art desalination membranes exhibit high water-salt selectivity, but their ability to discriminate between ions is limited. Elucidating the fundamental mechanisms underlying ion transport and selectivity in subnanometer pores is therefore imperative for the development of ion-selective membranes. Here, we compare the overall energy barrier for salt transport and energy barriers for individual ion transport, showing that cations and anions traverse the membrane pore in an independent manner. Supported by density functional theory simulations, we demonstrate that electrostatic interactions between permeating counterion and fixed charges on the membrane substantially hinder intrapore diffusion. Furthermore, using quartz crystal microbalance, we break down the contributions of partitioning at the pore mouth and intrapore diffusion to the overall energy barrier for salt transport. Overall, our results indicate that intrapore diffusion governs salt transport through subnanometer pores due to ion-pore wall interactions, providing the scientific base for the design of membranes with high ion-ion selectivity.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [1];  [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Department of Chemical and Environmental Engineering, Yale University, New Haven, CT 06511, USA.
  2. Faculty of Civil and Environmental Engineering, Technion—Israel Institute of Technology, Technion City, Haifa 32000, Israel.
  3. Lawrence Livermore National Laboratory, Livermore, CA 94551, USA.
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Enhanced Nanofluidic Transport (CENT)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1724272
Alternate Identifier(s):
OSTI ID: 1781762
Report Number(s):
LLNL-JRNL-814370
Journal ID: ISSN 2375-2548; eabd9045
Grant/Contract Number:  
SC0019112; AC52-07NA27344
Resource Type:
Published Article
Journal Name:
Science Advances
Additional Journal Information:
Journal Name: Science Advances Journal Volume: 6 Journal Issue: 48; Journal ID: ISSN 2375-2548
Publisher:
American Association for the Advancement of Science (AAAS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhou, Xuechen, Wang, Zhangxin, Epsztein, Razi, Zhan, Cheng, Li, Wenlu, Fortner, John D., Pham, Tuan Anh, Kim, Jae-Hong, and Elimelech, Menachem. Intrapore energy barriers govern ion transport and selectivity of desalination membranes. United States: N. p., 2020. Web. https://doi.org/10.1126/sciadv.abd9045.
Zhou, Xuechen, Wang, Zhangxin, Epsztein, Razi, Zhan, Cheng, Li, Wenlu, Fortner, John D., Pham, Tuan Anh, Kim, Jae-Hong, & Elimelech, Menachem. Intrapore energy barriers govern ion transport and selectivity of desalination membranes. United States. https://doi.org/10.1126/sciadv.abd9045
Zhou, Xuechen, Wang, Zhangxin, Epsztein, Razi, Zhan, Cheng, Li, Wenlu, Fortner, John D., Pham, Tuan Anh, Kim, Jae-Hong, and Elimelech, Menachem. Fri . "Intrapore energy barriers govern ion transport and selectivity of desalination membranes". United States. https://doi.org/10.1126/sciadv.abd9045.
@article{osti_1724272,
title = {Intrapore energy barriers govern ion transport and selectivity of desalination membranes},
author = {Zhou, Xuechen and Wang, Zhangxin and Epsztein, Razi and Zhan, Cheng and Li, Wenlu and Fortner, John D. and Pham, Tuan Anh and Kim, Jae-Hong and Elimelech, Menachem},
abstractNote = {State-of-the-art desalination membranes exhibit high water-salt selectivity, but their ability to discriminate between ions is limited. Elucidating the fundamental mechanisms underlying ion transport and selectivity in subnanometer pores is therefore imperative for the development of ion-selective membranes. Here, we compare the overall energy barrier for salt transport and energy barriers for individual ion transport, showing that cations and anions traverse the membrane pore in an independent manner. Supported by density functional theory simulations, we demonstrate that electrostatic interactions between permeating counterion and fixed charges on the membrane substantially hinder intrapore diffusion. Furthermore, using quartz crystal microbalance, we break down the contributions of partitioning at the pore mouth and intrapore diffusion to the overall energy barrier for salt transport. Overall, our results indicate that intrapore diffusion governs salt transport through subnanometer pores due to ion-pore wall interactions, providing the scientific base for the design of membranes with high ion-ion selectivity.},
doi = {10.1126/sciadv.abd9045},
journal = {Science Advances},
number = 48,
volume = 6,
place = {United States},
year = {2020},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1126/sciadv.abd9045

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