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Aligned macrocycle pores in ultrathin films for accurate molecular sieving

Author

Listed:
  • Zhiwei Jiang

    (Imperial College London
    Queen Mary University of London)

  • Ruijiao Dong

    (Imperial College London
    Shanghai Jiao Tong University)

  • Austin M. Evans

    (Northwestern University
    University of Florida)

  • Niklas Biere

    (Bielefeld University)

  • Mahmood A. Ebrahim

    (Imperial College London)

  • Siyao Li

    (Imperial College London)

  • Dario Anselmetti

    (Bielefeld University)

  • William R. Dichtel

    (Northwestern University)

  • Andrew G. Livingston

    (Imperial College London
    Queen Mary University of London)

Abstract

Polymer membranes are widely used in separation processes including desalination1, organic solvent nanofiltration2,3 and crude oil fractionation4,5. Nevertheless, direct evidence of subnanometre pores and a feasible method of manipulating their size is still challenging because of the molecular fluctuations of poorly defined voids in polymers6. Macrocycles with intrinsic cavities could potentially tackle this challenge. However, unfunctionalized macrocycles with indistinguishable reactivities tend towards disordered packing in films hundreds of nanometres thick7–9, hindering cavity interconnection and formation of through-pores. Here, we synthesized selectively functionalized macrocycles with differentiated reactivities that preferentially aligned to create well-defined pores across an ultrathin nanofilm. The ordered structure was enhanced by reducing the nanofilm thickness down to several nanometres. This orientated architecture enabled direct visualization of subnanometre macrocycle pores in the nanofilm surfaces, with the size tailored to ångström precision by varying the macrocycle identity. Aligned macrocycle membranes provided twice the methanol permeance and higher selectivity compared to disordered counterparts. Used in high-value separations, exemplified here by enriching cannabidiol oil, they achieved one order of magnitude faster ethanol transport and threefold higher enrichment than commercial state-of-the-art membranes. This approach offers a feasible strategy for creating subnanometre channels in polymer membranes, and demonstrates their potential for accurate molecular separations.

Suggested Citation

  • Zhiwei Jiang & Ruijiao Dong & Austin M. Evans & Niklas Biere & Mahmood A. Ebrahim & Siyao Li & Dario Anselmetti & William R. Dichtel & Andrew G. Livingston, 2022. "Aligned macrocycle pores in ultrathin films for accurate molecular sieving," Nature, Nature, vol. 609(7925), pages 58-64, September.
  • Handle: RePEc:nat:nature:v:609:y:2022:i:7925:d:10.1038_s41586-022-05032-1
    DOI: 10.1038/s41586-022-05032-1
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    Cited by:

    1. Bowen Gan & Lu Elfa Peng & Wenyu Liu & Lingyue Zhang & Li Ares Wang & Li Long & Hao Guo & Xiaoxiao Song & Zhe Yang & Chuyang Y. Tang, 2024. "Ultra-permeable silk-based polymeric membranes for vacuum-driven nanofiltration," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Banan Alhazmi & Gergo Ignacz & Maria Vincenzo & Mohamed Nejib Hedhili & Gyorgy Szekely & Suzana P. Nunes, 2024. "Ultraselective Macrocycle Membranes for Pharmaceutical Ingredients Separation in Organic Solvents," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. Jihoon Choi & Keonwoo Choi & YongSung Kwon & Daehun Kim & Youngmin Yoo & Sung Gap Im & Dong-Yeun Koh, 2024. "Ultrathin organosiloxane membrane for precision organic solvent nanofiltration," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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