Temperature-regulated guest admission and release in microporous materials

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.

doi:10.1038/ncomms15777

Title: Temperature-regulated guest admission and release in microporous materials

Journal Article · Fri Jun 09 04:00:00 UTC 2017 · Nature Communications

DOI: https://doi.org/10.1038/ncomms15777 · OSTI ID:1374884

Li, Gang ^[1]; Shang, Jin ^[2]; Gu, Qinfen ^[3]; Awati, Rohan V. ^[4]; Jensen, Nathan ^[5]; Grant, Andrew ^[5]; Zhang, Xueying ^[6]; Sholl, David S. ^[4];

^[7]; Webley, Paul A. ^[6];

^[5]

Univ. of Western Australia, Crawley, WA (Australia). Centre for Energy; The University of Western Australia
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 Western Australia, Crawley, WA (Australia). Centre for Energy
Univ. of Melbourne (Australia). Dept. of Chemical and Biomolecular Engineering
Monash Univ., Melbourne, VIC (Australia). Dept. of Mechanical and Aerospace Engineering

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.

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Research Organization:: Georgia Tech Research Corporation, 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012577

OSTI ID:: 1374884

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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