Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer

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...

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Main Authors: Tan, Kui, Zuluaga, Sebastian, Fuentes, Erika, Veyan, Jean-François, Li, Jing, Chabal, Yves J., Mattson, Eric Michael, Wang, Hao, Thonhauser, Timo
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:en_US
Published: Nature Publishing Group 2017
Online Access:http://hdl.handle.net/1721.1/107630
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author Tan, Kui
Zuluaga, Sebastian
Fuentes, Erika
Veyan, Jean-François
Li, Jing
Chabal, Yves J.
Mattson, Eric Michael
Wang, Hao
Thonhauser, Timo
author2 Massachusetts Institute of Technology. Department of Chemistry
author_facet Massachusetts Institute of Technology. Department of Chemistry
Tan, Kui
Zuluaga, Sebastian
Fuentes, Erika
Veyan, Jean-François
Li, Jing
Chabal, Yves J.
Mattson, Eric Michael
Wang, Hao
Thonhauser, Timo
author_sort Tan, Kui
collection MIT
description 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, C₂H₂, 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. These findings may provide alternative strategies for gas storage, delivery and separation.
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spelling mit-1721.1/1076302022-09-30T19:24:11Z Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer Tan, Kui Zuluaga, Sebastian Fuentes, Erika Veyan, Jean-François Li, Jing Chabal, Yves J. Mattson, Eric Michael Wang, Hao Thonhauser, Timo Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Department of Civil and Environmental Engineering Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science Mattson, Eric Michael Wang, Hao Thonhauser, Timo 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, C₂H₂, 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. These findings may provide alternative strategies for gas storage, delivery and separation. 2017-03-22T13:53:47Z 2017-03-22T13:53:47Z 2016-12 2016-08 Article http://purl.org/eprint/type/JournalArticle 2041-1723 http://hdl.handle.net/1721.1/107630 Tan, Kui, Sebastian Zuluaga, Erika Fuentes, Eric C. Mattson, Jean-François Veyan, Hao Wang, Jing Li, Timo Thonhauser, and Yves J. Chabal. “Trapping Gases in Metal-Organic Frameworks with a Selective Surface Molecular Barrier Layer.” Nature Communications 7 (December 13, 2016): 13871. en_US http://dx.doi.org/10.1038/ncomms13871 Nature Communications Creative Commons Attribution 4.0 International License http://creativecommons.org/licenses/by/4.0/ application/pdf Nature Publishing Group Nature
spellingShingle Tan, Kui
Zuluaga, Sebastian
Fuentes, Erika
Veyan, Jean-François
Li, Jing
Chabal, Yves J.
Mattson, Eric Michael
Wang, Hao
Thonhauser, Timo
Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
title Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
title_full Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
title_fullStr Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
title_full_unstemmed Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
title_short Trapping gases in metal-organic frameworks with a selective surface molecular barrier layer
title_sort trapping gases in metal organic frameworks with a selective surface molecular barrier layer
url http://hdl.handle.net/1721.1/107630
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