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Title: Fast and selective fluoride ion conduction in sub-1-nanometer metal-organic framework channels

Abstract

Biological fluoride ion channels are sub-1-nanometer protein pores with ultrahigh F- conductivity and selectivity over other halogen ions. Developing synthetic F- channels with biological-level selectivity is highly desirable for ion separations such as water defluoridation, but it remains a great challenge. Here we report synthetic F- channels fabricated from zirconium-based metal-organic frameworks (MOFs), UiO-66-X ( x = H, NH2, and N+(CH3)3). These MOFs are comprised of nanometer-sized cavities connected by sub-1-nanometer-sized windows and have specific F- binding sites along the channels, sharing some features of biological F- channels. UiO-66-X channels consistently show ultrahigh F- conductivity up to ~10 S m-1, and ultrahigh F-/Cl- selectivity, from ~13 to ~240. Molecular dynamics simulations reveal that the ultrahigh F- conductivity and selectivity can be ascribed mainly to the high F- concentration in the UiO-66 channels, arising from specific interactions between F- ions and F- binding sites in the MOF channels.

Authors:
 [1]; ORCiD logo [1];  [2]; ORCiD logo [1];  [1];  [3];  [1];  [4];  [3]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [3];  [1];  [1]
  1. Monash Univ., Clayton, VIC (Australia)
  2. Univ. of Melbourne, Parkville, VIC (Australia)
  3. Commonwealth Scientific and Industrial Research Organisation (CSIRO), Clayton, VIC (Australia)
  4. Monash Univ., Clayton, VIC (Australia); Commonwealth Scientific and Industrial Research Organisation (CSIRO), Clayton, VIC (Australia)
  5. Univ. of Texas, Austin, TX (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Materials for Water and Energy Systems (M-WET); Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Australian Research Council; Australia-China Science and Research Fund
OSTI Identifier:
1613158
Grant/Contract Number:  
SC0019272; DP150100765; DP180100298; DE170100006; ACSRF48154
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Li, Xingya, Zhang, Huacheng, Wang, Peiyao, Hou, Jue, Lu, Jun, Easton, Christopher D., Zhang, Xiwang, Hill, Matthew R., Thornton, Aaron W., Liu, Jefferson Zhe, Freeman, Benny D., Hill, Anita J., Jiang, Lei, and Wang, Huanting. Fast and selective fluoride ion conduction in sub-1-nanometer metal-organic framework channels. United States: N. p., 2019. Web. doi:10.1038/s41467-019-10420-9.
Li, Xingya, Zhang, Huacheng, Wang, Peiyao, Hou, Jue, Lu, Jun, Easton, Christopher D., Zhang, Xiwang, Hill, Matthew R., Thornton, Aaron W., Liu, Jefferson Zhe, Freeman, Benny D., Hill, Anita J., Jiang, Lei, & Wang, Huanting. Fast and selective fluoride ion conduction in sub-1-nanometer metal-organic framework channels. United States. https://doi.org/10.1038/s41467-019-10420-9
Li, Xingya, Zhang, Huacheng, Wang, Peiyao, Hou, Jue, Lu, Jun, Easton, Christopher D., Zhang, Xiwang, Hill, Matthew R., Thornton, Aaron W., Liu, Jefferson Zhe, Freeman, Benny D., Hill, Anita J., Jiang, Lei, and Wang, Huanting. Tue . "Fast and selective fluoride ion conduction in sub-1-nanometer metal-organic framework channels". United States. https://doi.org/10.1038/s41467-019-10420-9. https://www.osti.gov/servlets/purl/1613158.
@article{osti_1613158,
title = {Fast and selective fluoride ion conduction in sub-1-nanometer metal-organic framework channels},
author = {Li, Xingya and Zhang, Huacheng and Wang, Peiyao and Hou, Jue and Lu, Jun and Easton, Christopher D. and Zhang, Xiwang and Hill, Matthew R. and Thornton, Aaron W. and Liu, Jefferson Zhe and Freeman, Benny D. and Hill, Anita J. and Jiang, Lei and Wang, Huanting},
abstractNote = {Biological fluoride ion channels are sub-1-nanometer protein pores with ultrahigh F- conductivity and selectivity over other halogen ions. Developing synthetic F- channels with biological-level selectivity is highly desirable for ion separations such as water defluoridation, but it remains a great challenge. Here we report synthetic F- channels fabricated from zirconium-based metal-organic frameworks (MOFs), UiO-66-X ( x = H, NH2, and N+(CH3)3). These MOFs are comprised of nanometer-sized cavities connected by sub-1-nanometer-sized windows and have specific F- binding sites along the channels, sharing some features of biological F- channels. UiO-66-X channels consistently show ultrahigh F- conductivity up to ~10 S m-1, and ultrahigh F-/Cl- selectivity, from ~13 to ~240. Molecular dynamics simulations reveal that the ultrahigh F- conductivity and selectivity can be ascribed mainly to the high F- concentration in the UiO-66 channels, arising from specific interactions between F- ions and F- binding sites in the MOF channels.},
doi = {10.1038/s41467-019-10420-9},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Tue Jun 11 00:00:00 EDT 2019},
month = {Tue Jun 11 00:00:00 EDT 2019}
}

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Superior removal of arsenic from water with zirconium metal-organic framework UiO-66
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Zeolitic imidazolate framework-8 as a reverse osmosis membrane for water desalination: Insight from molecular simulation
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  • The Journal of Chemical Physics, Vol. 134, Issue 13
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Molecular dynamics simulation of ionic mobility. I. Alkali metal cations in water at 25 °C
journal, October 1994

  • Lee, Song Hi; Rasaiah, Jayendran C.
  • The Journal of Chemical Physics, Vol. 101, Issue 8
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Bacterial fluoride resistance, Fluc channels, and the weak acid accumulation effect
journal, August 2014

  • Ji, Chunhui; Stockbridge, Randy B.; Miller, Christopher
  • The Journal of General Physiology, Vol. 144, Issue 3
  • DOI: 10.1085/jgp.201411243

Effect of nanopore geometry on ion current rectification
journal, March 2011


Ultrafast selective transport of alkali metal ions in metal organic frameworks with subnanometer pores
journal, February 2018


Widespread Genetic Switches and Toxicity Resistance Proteins for Fluoride
journal, December 2011


Ion transport through a graphene nanopore
text, January 2013


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