Journal article

Temperature-regulated guest admission and release in microporous materials

Gang Kevin Li, Jin Shang, Qinfen Gu, Rohan V Awati, Nathan Jensen, Andrew Grant, Xueying Zhang, David S Sholl, Jefferson Z Liu, Paul A Webley, Eric F May

NATURE COMMUNICATIONS | NATURE PUBLISHING GROUP | Published : 2017

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 nanocontaine..

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Grants

Awarded by Australian Research Council


Awarded by Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences


Funding Acknowledgements

G.L. is the recipient of an Australian Research Council Discovery Early Career Researcher Award (DE140101824). This research was undertaken on the powder X-ray diffraction beamline at the Australian Synchrotron, Victoria, Australia. J.S., P.A.W. and J.Z.L. acknowledge the Australian Research Council for providing the funding (DP130103708) and acknowledge National Computational Infrastructure at Australian National University for providing the computational resource. D.S.S. was supported as part of the Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center funded by U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award #DE-SC0012577. E.F.M. and G.L. acknowledge support from the Australian Research Council through IC150100019. G.L., J.S. and E.F.M. thank Professors Yinong Liu and Michael Johns, Drs Michael Moldover and Hanjun Fang for helpful discussions.