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

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

doi:10.1038/s41467-019-10420-9

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

Journal Article · 11 June 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-10420-9 · OSTI ID:1613158

Li, Xingya ^[1];

^[1]; Wang, Peiyao ^[2];

^[1]; Lu, Jun ^[1]; Easton, Christopher D. ^[3]; Zhang, Xiwang ^[1]; Hill, Matthew R. ^[4]; Thornton, Aaron W. ^[3];

^[2];

^[5];

^[3]; Jiang, Lei ^[1]; Wang, Huanting ^[1]

Monash Univ., Clayton, VIC (Australia)
Univ. of Melbourne, Parkville, VIC (Australia)
Commonwealth Scientific and Industrial Research Organisation (CSIRO), Clayton, VIC (Australia)
Monash Univ., Clayton, VIC (Australia); Commonwealth Scientific and Industrial Research Organisation (CSIRO), Clayton, VIC (Australia)
Univ. of Texas, Austin, TX (United States)

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.

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Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Australian Research Council; Australia-China Science and Research Fund

Grant/Contract Number:: SC0019272; DP150100765; DP180100298; DE170100006; ACSRF48154

OSTI ID:: 1613158

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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In Situ Probes of Capture and Decomposition of Chemical Warfare Agent Simulants by Zr-Based Metal Organic Frameworks Plonka, Anna M.; Wang, Qi; Gordon, Wesley O. Journal of the American Chemical Society, Vol. 139, Issue 2 https://doi.org/10.1021/jacs.6b11373	journal	January 2017
Understanding the Thermodynamic and Kinetic Behavior of the CO ₂ /CH ₄ Gas Mixture within the Porous Zirconium Terephthalate UiO-66(Zr): A Joint Experimental and Modeling Approach Yang, Qingyuan; Wiersum, Andrew D.; Jobic, Hervé The Journal of Physical Chemistry C, Vol. 115, Issue 28 https://doi.org/10.1021/jp202633t	journal	June 2011
Molecular Dynamics Simulation of Ion Mobility. 2. Alkali Metal and Halide Ions Using the SPC/E Model for Water at 25 °C ^† Lee, Song Hi; Rasaiah, Jayendran C. The Journal of Physical Chemistry, Vol. 100, Issue 4 https://doi.org/10.1021/jp953050c	journal	January 1996
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Separation of Fluoride from Other Monovalent Anions Using Multilayer Polyelectrolyte Nanofiltration Membranes Hong, Seong Uk; Malaisamy, Ramamoorthy; Bruening, Merlin L. Langmuir, Vol. 23, Issue 4 https://doi.org/10.1021/la061701y	journal	February 2007
Covalent Modification of a Glassy Carbon Surface by 4-Aminobenzoic Acid and Its Application in Fabrication of a Polyoxometalates-Consisting Monolayer and Multilayer Films Liu, Jianyun; Cheng, Long; Liu, Baifeng Langmuir, Vol. 16, Issue 19 https://doi.org/10.1021/la9913506	journal	September 2000
Chemical, thermal and mechanical stabilities of metal–organic frameworks Howarth, Ashlee J.; Liu, Yangyang; Li, Peng Nature Reviews Materials, Vol. 1, Issue 3 https://doi.org/10.1038/natrevmats.2015.18	journal	February 2016
Metal–organic frameworks for membrane-based separations Denny, Michael S.; Moreton, Jessica C.; Benz, Lauren Nature Reviews Materials, Vol. 1, Issue 12 https://doi.org/10.1038/natrevmats.2016.78	journal	November 2016
Proof of dual-topology architecture of Fluc F− channels with monobody blockers Stockbridge, Randy B.; Koide, Akiko; Miller, Christopher Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6120	journal	October 2014
Microporous metal–organic framework with dual functionalities for highly efficient removal of acetylene from ethylene/acetylene mixtures Hu, Tong-Liang; Wang, Hailong; Li, Bin Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8328	journal	June 2015
Superior removal of arsenic from water with zirconium metal-organic framework UiO-66 Wang, Chenghong; Liu, Xinlei; Chen, J. Paul Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep16613	journal	November 2015
Canonical Monte Carlo simulations of the fluctuating-charge molecular water between charged surfaces Yang, Kun-Lin; Yiacoumi, Sotira; Tsouris, Costas The Journal of Chemical Physics, Vol. 117, Issue 1 https://doi.org/10.1063/1.1480858	journal	July 2002
Zeolitic imidazolate framework-8 as a reverse osmosis membrane for water desalination: Insight from molecular simulation Hu, Zhongqiao; Chen, Yifei; Jiang, Jianwen The Journal of Chemical Physics, Vol. 134, Issue 13 https://doi.org/10.1063/1.3573902	journal	April 2011
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