Temperature-dependent rearrangement of gas molecules in ultramicroporous materials for tunable adsorption of CO2 and C2H2

Zhaoqiang Zhang, Yinlin Chen, Kungang Chai, Chengjun Kang, Shing Bo Peh, He Li, Junyu Ren, Xiansong Shi, Xue Han, Catherine Dejoie, Sarah J. Day, Sihai Yang () and Dan Zhao ()
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Zhaoqiang Zhang: National University of Singapore
Yinlin Chen: The University of Manchester
Kungang Chai: Guangxi University
Chengjun Kang: National University of Singapore
Shing Bo Peh: National University of Singapore
He Li: National University of Singapore
Junyu Ren: National University of Singapore
Xiansong Shi: National University of Singapore
Xue Han: Beijing Normal University
Catherine Dejoie: The European Synchrotron Radiation Facility
Sarah J. Day: Harwell Science Campus
Sihai Yang: The University of Manchester
Dan Zhao: National University of Singapore

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract The interactions between adsorbed gas molecules within porous metal-organic frameworks are crucial to gas selectivity but remain poorly explored. Here, we report the modulation of packing geometries of CO2 and C2H2 clusters within the ultramicroporous CUK-1 material as a function of temperature. In-situ synchrotron X-ray diffraction reveals a unique temperature-dependent reversal of CO2 and C2H2 adsorption affinities on CUK-1, which is validated by gas sorption and dynamic breakthrough experiments, affording high-purity C2H2 (99.95%) from the equimolar mixture of C2H2/CO2 via a one-step purification process. At low temperatures ( 10) and capacity (170 cm3 g−1) owing to the formation of CO2 tetramers that simultaneously maximize the guest-guest and host-guest interactions. At room temperature, conventionally selective adsorption of C2H2 is observed. The selectivity reversal, structural robustness, and facile regeneration of CUK-1 suggest its potential for producing high-purity C2H2 by temperature-swing sorption.

Date: 2023
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DOI: 10.1038/s41467-023-39319-2

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