Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
Abstract
The main challenge for gas storage and separation in nanoporous materials is that many molecules of interest adsorb too weakly to be effectively retained. Instead of synthetically modifying the internal surface structure of the entire bulk—as is typically done to enhance adsorption—here we show that post exposure of a prototypical porous metal-organic framework to ethylenediamine can effectively retain a variety of weakly adsorbing molecules (for example, CO, CO2, SO2, C2H4, NO) inside the materials by forming a monolayer-thick cap at the external surface of microcrystals. Furthermore, this capping mechanism, based on hydrogen bonding as explained by ab initio modelling, opens the door for potential selectivity. For example, water molecules are shown to disrupt the hydrogen-bonded amine network and diffuse through the cap without hindrance and fully displace/release the retained small molecules out of the metal-organic framework at room temperature. Lastly, these findings may provide alternative strategies for gas storage, delivery and separation.
- Authors:
-
- Univ. of Texas-Dallas, Richardson, TX (United States). Dept. of Materials Science & Engineering
- Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Physics
- Rutgers Univ., Piscataway, NJ (United States). Dept. of Chemistry and Chemical Biology
- Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Univ. of Texas at Dallas, Richardson, TX (United States); UT-Battelle LLC/ORNL, Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1361675
- Grant/Contract Number:
- FG02-08ER46491; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Metal–organic frameworks; Structural materials
Citation Formats
Tan, Kui, Zuluaga, Sebastian, Fuentes, Erika, Mattson, Eric C., Veyan, Jean-François, Wang, Hao, Li, Jing, Thonhauser, Timo, and Chabal, Yves J. Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer. United States: N. p., 2016.
Web. doi:10.1038/ncomms13871.
Tan, Kui, Zuluaga, Sebastian, Fuentes, Erika, Mattson, Eric C., Veyan, Jean-François, Wang, Hao, Li, Jing, Thonhauser, Timo, & Chabal, Yves J. Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer. United States. https://doi.org/10.1038/ncomms13871
Tan, Kui, Zuluaga, Sebastian, Fuentes, Erika, Mattson, Eric C., Veyan, Jean-François, Wang, Hao, Li, Jing, Thonhauser, Timo, and Chabal, Yves J. Tue .
"Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer". United States. https://doi.org/10.1038/ncomms13871. https://www.osti.gov/servlets/purl/1361675.
@article{osti_1361675,
title = {Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer},
author = {Tan, Kui and Zuluaga, Sebastian and Fuentes, Erika and Mattson, Eric C. and Veyan, Jean-François and Wang, Hao and Li, Jing and Thonhauser, Timo and Chabal, Yves J.},
abstractNote = {The main challenge for gas storage and separation in nanoporous materials is that many molecules of interest adsorb too weakly to be effectively retained. Instead of synthetically modifying the internal surface structure of the entire bulk—as is typically done to enhance adsorption—here we show that post exposure of a prototypical porous metal-organic framework to ethylenediamine can effectively retain a variety of weakly adsorbing molecules (for example, CO, CO2, SO2, C2H4, NO) inside the materials by forming a monolayer-thick cap at the external surface of microcrystals. Furthermore, this capping mechanism, based on hydrogen bonding as explained by ab initio modelling, opens the door for potential selectivity. For example, water molecules are shown to disrupt the hydrogen-bonded amine network and diffuse through the cap without hindrance and fully displace/release the retained small molecules out of the metal-organic framework at room temperature. Lastly, these findings may provide alternative strategies for gas storage, delivery and separation.},
doi = {10.1038/ncomms13871},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Tue Dec 13 00:00:00 EST 2016},
month = {Tue Dec 13 00:00:00 EST 2016}
}
Web of Science
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