Temperature-regulated guest admission and release in microporous materials
| Autor: | Jin Shang, Rohan Awati, Nathan K. Jensen, Paul A. Webley, Eric F. May, Andrew Grant, Xueying Zhang, David S. Sholl, Gang Kevin Li, Jefferson Zhe Liu, Qinfen Gu |
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| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
Multidisciplinary
Materials science Science Supramolecular chemistry General Physics and Astronomy Thermal fluctuations Sorption Nanotechnology 02 engineering and technology General Chemistry Microporous material 010402 general chemistry 021001 nanoscience & nanotechnology Molecular sieve 01 natural sciences General Biochemistry Genetics and Molecular Biology Article 0104 chemical sciences Membrane Chemical engineering Molecule Metal-organic framework 0210 nano-technology |
| Zdroj: | Nature Communications Nature Communications, Vol 8, Iss 1, Pp 1-9 (2017) |
| ISSN: | 2041-1723 |
| Popis: | 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 demonstrate how temperature can be exploited to achieve appreciable hydrogen and methane storage in such materials without sustained pressure. These findings also open new avenues for gas sensing and isotope separation. Regulating guest access and release in porous materials remains an important goal. Here, May and colleagues elucidate the mechanism by which guest admission can be temperature-regulated in typical microporous materials, and experimentally exploit this process to achieve appreciable and reversible hydrogen storage. |
| Databáze: | OpenAIRE |
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