Temperature-regulated guest admission and release in microporous materials
Abstract
While it has long been known that some highly adsorbing microporous materials suddenly become inaccessible to guest molecules below certain temperatures, previous attempts to explain this phenomenon have failed. Here we show that this anomalous sorption behaviour is a temperature-regulated guest admission process, where the pore-keeping group’s thermal fluctuations are influenced by interactions with guest molecules. A physical model is presented to explain the atomic-level chemistry and structure of these thermally regulated micropores, which is crucial to systematic engineering of new functional materials such as tunable molecular sieves, gated membranes and controlled-release nanocontainers. The model was validated experimentally with H2, N2, Ar and CH4 on three classes of microporous materials: trapdoor zeolites, supramolecular host calixarenes and metal-organic frameworks. We also demonstrate how temperature can be exploited to achieve appreciable hydrogen and methane storage in such materials without sustained pressure. Our findings also open new avenues for gas sensing and isotope separation.
- Authors:
-
[6];
[1]
- Univ. of Western Australia, Crawley, WA (Australia). Centre for Energy
- City Univ. of Hong Kong (China). School of Energy and Environmental Catalysis; Univ. of Melbourne (Australia). Dept. of Chemical and Biomolecular Engineering
- Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, VIC (Australia). Australian Synchrotron
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
- Univ. of Melbourne (Australia). Dept. of Chemical and Biomolecular Engineering
- Monash Univ., Melbourne, VIC (Australia). Dept. of Mechanical and Aerospace Engineering
- Publication Date:
- Research Org.:
- Georgia Institute of Technology, Atlanta, GA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1374884
- Grant/Contract Number:
- SC0012577; DE140101824; DP130103708; IC150100019
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 8; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; chemical engineering; hydrogen storage materials; metal-organic frameworks; porous materials
Citation Formats
Li, Gang, Shang, Jin, Gu, Qinfen, Awati, Rohan V., Jensen, Nathan, Grant, Andrew, Zhang, Xueying, Sholl, David S., Liu, Jefferson Z., Webley, Paul A., and May, Eric F. Temperature-regulated guest admission and release in microporous materials. United States: N. p., 2017.
Web. doi:10.1038/ncomms15777.
Li, Gang, Shang, Jin, Gu, Qinfen, Awati, Rohan V., Jensen, Nathan, Grant, Andrew, Zhang, Xueying, Sholl, David S., Liu, Jefferson Z., Webley, Paul A., & May, Eric F. Temperature-regulated guest admission and release in microporous materials. United States. https://doi.org/10.1038/ncomms15777
Li, Gang, Shang, Jin, Gu, Qinfen, Awati, Rohan V., Jensen, Nathan, Grant, Andrew, Zhang, Xueying, Sholl, David S., Liu, Jefferson Z., Webley, Paul A., and May, Eric F. Fri .
"Temperature-regulated guest admission and release in microporous materials". United States. https://doi.org/10.1038/ncomms15777. https://www.osti.gov/servlets/purl/1374884.
@article{osti_1374884,
title = {Temperature-regulated guest admission and release in microporous materials},
author = {Li, Gang and Shang, Jin and Gu, Qinfen and Awati, Rohan V. and Jensen, Nathan and Grant, Andrew and Zhang, Xueying and Sholl, David S. and Liu, Jefferson Z. and Webley, Paul A. and May, Eric F.},
abstractNote = {While it has long been known that some highly adsorbing microporous materials suddenly become inaccessible to guest molecules below certain temperatures, previous attempts to explain this phenomenon have failed. Here we show that this anomalous sorption behaviour is a temperature-regulated guest admission process, where the pore-keeping group’s thermal fluctuations are influenced by interactions with guest molecules. A physical model is presented to explain the atomic-level chemistry and structure of these thermally regulated micropores, which is crucial to systematic engineering of new functional materials such as tunable molecular sieves, gated membranes and controlled-release nanocontainers. The model was validated experimentally with H2, N2, Ar and CH4 on three classes of microporous materials: trapdoor zeolites, supramolecular host calixarenes and metal-organic frameworks. We also demonstrate how temperature can be exploited to achieve appreciable hydrogen and methane storage in such materials without sustained pressure. Our findings also open new avenues for gas sensing and isotope separation.},
doi = {10.1038/ncomms15777},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Fri Jun 09 00:00:00 EDT 2017},
month = {Fri Jun 09 00:00:00 EDT 2017}
}
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Figure 1: | Paradox of non-polar gas molecule admission through the apparently blocked pores of a potassium chabazite. (a) Illustration of the structure of an ideal potassium chabazite crystal, highlighting the eight-membered oxygen ring (8MR) which sets the nominal pore aperture diameter to be 3.8Å (distance between opposing oxygen atoms).more »
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Works referencing / citing this record:
An optimal trapdoor zeolite for exclusive admission of CO 2 at industrial carbon capture operating temperatures
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- Du, Tao; Fang, Xin; Liu, Liying
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Data from: Temperature-regulated guest admission and release in microporous materials
dataset, June 2017
- Li, Gang Kevin; Shang, Jin; Gu, Qinfen
- Dryad Digital Repository-Supplementary information for journal article at DOI: 10.1038/ncomms15777, 3 CIF files
Data from: Temperature-regulated guest admission and release in microporous materials
dataset, June 2017
- Li, Gang Kevin; Shang, Jin; Gu, Qinfen
- Dryad Digital Repository-Supplementary information for journal article at DOI: 10.1038/ncomms15777, 3 CIF files
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Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.