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

Author

Listed:
  • 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
    Peking University)

  • Dan Zhao

    (National University of Singapore)

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.

Suggested Citation

  • 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 & Dan Zhao, 2023. "Temperature-dependent rearrangement of gas molecules in ultramicroporous materials for tunable adsorption of CO2 and C2H2," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39319-2
    DOI: 10.1038/s41467-023-39319-2
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