Supramolecular binding and separation of hydrocarbons within a functionalized porous metal–organic framework
Abstract
Supramolecular interactions are fundamental to host-guest binding in many chemical and biological processes. Direct visualization of such supramolecular interactions within host-guest systems is extremely challenging, but crucial to understanding their function. We report a comprehensive study that combines neutron scattering, synchrotron X-ray and neutron diffraction, and computational modelling to define the detailed binding at a molecular level of acetylene, ethylene and ethane within the porous host NOTT-300. This study reveals simultaneous and cooperative hydrogen-bonding, pi center dot center dot center dot pi stacking interactions and intermolecular dipole interactions in the binding of acetylene and ethylene to give up to 12 individual weak supramolecular interactions aligned within the host to form an optimal geometry for the selective binding of hydrocarbons. We also report the cooperative binding of a mixture of acetylene and ethylene within the porous host, together with the corresponding breakthrough experiments and analysis of adsorption isotherms of gas mixtures.
- Authors:
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1286811
- Alternate Identifier(s):
- OSTI ID: 1352748
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Chemistry
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 1755-4330
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Metal–organic frameworks
Citation Formats
Yang, Sihai, Ramirez-Cuesta, Anibal J., Newby, Ruth, Garcia-Sakai, Victoria, Manuel, Pascal, Callear, Samantha K., Campbell, Stuart I., Tang, Chiu C., and Schröder, Martin. Supramolecular binding and separation of hydrocarbons within a functionalized porous metal–organic framework. United States: N. p., 2014.
Web. doi:10.1038/nchem.2114.
Yang, Sihai, Ramirez-Cuesta, Anibal J., Newby, Ruth, Garcia-Sakai, Victoria, Manuel, Pascal, Callear, Samantha K., Campbell, Stuart I., Tang, Chiu C., & Schröder, Martin. Supramolecular binding and separation of hydrocarbons within a functionalized porous metal–organic framework. United States. https://doi.org/10.1038/nchem.2114
Yang, Sihai, Ramirez-Cuesta, Anibal J., Newby, Ruth, Garcia-Sakai, Victoria, Manuel, Pascal, Callear, Samantha K., Campbell, Stuart I., Tang, Chiu C., and Schröder, Martin. Mon .
"Supramolecular binding and separation of hydrocarbons within a functionalized porous metal–organic framework". United States. https://doi.org/10.1038/nchem.2114. https://www.osti.gov/servlets/purl/1286811.
@article{osti_1286811,
title = {Supramolecular binding and separation of hydrocarbons within a functionalized porous metal–organic framework},
author = {Yang, Sihai and Ramirez-Cuesta, Anibal J. and Newby, Ruth and Garcia-Sakai, Victoria and Manuel, Pascal and Callear, Samantha K. and Campbell, Stuart I. and Tang, Chiu C. and Schröder, Martin},
abstractNote = {Supramolecular interactions are fundamental to host-guest binding in many chemical and biological processes. Direct visualization of such supramolecular interactions within host-guest systems is extremely challenging, but crucial to understanding their function. We report a comprehensive study that combines neutron scattering, synchrotron X-ray and neutron diffraction, and computational modelling to define the detailed binding at a molecular level of acetylene, ethylene and ethane within the porous host NOTT-300. This study reveals simultaneous and cooperative hydrogen-bonding, pi center dot center dot center dot pi stacking interactions and intermolecular dipole interactions in the binding of acetylene and ethylene to give up to 12 individual weak supramolecular interactions aligned within the host to form an optimal geometry for the selective binding of hydrocarbons. We also report the cooperative binding of a mixture of acetylene and ethylene within the porous host, together with the corresponding breakthrough experiments and analysis of adsorption isotherms of gas mixtures.},
doi = {10.1038/nchem.2114},
journal = {Nature Chemistry},
number = 2,
volume = 7,
place = {United States},
year = {Mon Dec 01 00:00:00 EST 2014},
month = {Mon Dec 01 00:00:00 EST 2014}
}
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