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

Tan, Kui; Zuluaga, Sebastian; Fuentes, Erika; Mattson, Eric C.; Veyan, Jean-François; Wang, Hao; Li, Jing; Thonhauser, Timo; Chabal, Yves J.

doi:10.1038/ncomms13871

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

Journal Article · Tue Dec 13 00:00:00 EST 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms13871· OSTI ID:1361675

Tan, Kui ^[1]; Zuluaga, Sebastian ^[2]; Fuentes, Erika ^[1]; Mattson, Eric C. ^[1]; Veyan, Jean-François ^[1]; Wang, Hao ^[3]; Li, Jing ^[3]; Thonhauser, Timo ^[4]; Chabal, Yves J. ^[1]

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

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.

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Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-08ER46491; AC05-00OR22725

OSTI ID:: 1361675

Journal Information:: Nature Communications, Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 56 works

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

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