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Chemical control of structure and guest uptake by a conformationally mobile porous material

Author

Listed:
  • Alexandros P. Katsoulidis

    (University of Liverpool)

  • Dmytro Antypov

    (University of Liverpool)

  • George F. S. Whitehead

    (University of Liverpool)

  • Elliot J. Carrington

    (University of Liverpool)

  • Dave J. Adams

    (University of Liverpool
    University of Glasgow)

  • Neil G. Berry

    (University of Liverpool)

  • George R. Darling

    (University of Liverpool)

  • Matthew S. Dyer

    (University of Liverpool)

  • Matthew J. Rosseinsky

    (University of Liverpool)

Abstract

Metal–organic frameworks (MOFs) are crystalline synthetic porous materials formed by binding organic linkers to metal nodes: they can be either rigid1,2 or flexible3. Zeolites and rigid MOFs have widespread applications in sorption, separation and catalysis that arise from their ability to control the arrangement and chemistry of guest molecules in their pores via the shape and functionality of their internal surface, defined by their chemistry and structure4,5. Their structures correspond to an energy landscape with a single, albeit highly functional, energy minimum. By contrast, proteins function by navigating between multiple metastable structures using bond rotations of the polypeptide6,7, where each structure lies in one of the minima of a conformational energy landscape and can be selected according to the chemistry of the molecules that interact with the protein. These structural changes are realized through the mechanisms of conformational selection (where a higher-energy minimum characteristic of the protein is stabilized by small-molecule binding) and induced fit (where a small molecule imposes a structure on the protein that is not a minimum in the absence of that molecule)8. Here we show that rotation about covalent bonds in a peptide linker can change a flexible MOF to afford nine distinct crystal structures, revealing a conformational energy landscape that is characterized by multiple structural minima. The uptake of small-molecule guests by the MOF can be chemically triggered by inducing peptide conformational change. This change transforms the material from a minimum on the landscape that is inactive for guest sorption to an active one. Chemical control of the conformation of a flexible organic linker offers a route to modifying the pore geometry and internal surface chemistry and thus the function of open-framework materials.

Suggested Citation

  • Alexandros P. Katsoulidis & Dmytro Antypov & George F. S. Whitehead & Elliot J. Carrington & Dave J. Adams & Neil G. Berry & George R. Darling & Matthew S. Dyer & Matthew J. Rosseinsky, 2019. "Chemical control of structure and guest uptake by a conformationally mobile porous material," Nature, Nature, vol. 565(7738), pages 213-217, January.
  • Handle: RePEc:nat:nature:v:565:y:2019:i:7738:d:10.1038_s41586-018-0820-9
    DOI: 10.1038/s41586-018-0820-9
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    Citations

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    1. Yifan Gu & Jia-Jia Zheng & Ken-ichi Otake & Shigeyoshi Sakaki & Hirotaka Ashitani & Yoshiki Kubota & Shogo Kawaguchi & Ming-Shui Yao & Ping Wang & Ying Wang & Fengting Li & Susumu Kitagawa, 2023. "Soft corrugated channel with synergistic exclusive discrimination gating for CO2 recognition in gas mixture," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Ryunosuke Hayashi & Shohei Tashiro & Masahiro Asakura & Shinya Mitsui & Mitsuhiko Shionoya, 2023. "Effector-dependent structural transformation of a crystalline framework with allosteric effects on molecular recognition ability," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. Yangyang Xu & Tu Sun & Tengwu Zeng & Xiangyu Zhang & Xuan Yao & Shan Liu & Zhaolin Shi & Wen Wen & Yingbo Zhao & Shan Jiang & Yanhang Ma & Yue-Biao Zhang, 2023. "Symmetry-breaking dynamics in a tautomeric 3D covalent organic framework," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Xiaojun Ding & Jing Chen & Gang Ye, 2024. "Supramolecular polynuclear clusters sustained cubic hydrogen bonded frameworks with octahedral cages for reversible photochromism," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    5. Yong Peng & Hanting Xiong & Peixin Zhang & Zhiwei Zhao & Xing Liu & Shihui Tang & Yuan Liu & Zhenliang Zhu & Weizhen Zhou & Zhenning Deng & Junhui Liu & Yao Zhong & Zeliang Wu & Jingwen Chen & Zhenyu , 2024. "Interaction-selective molecular sieving adsorbent for direct separation of ethylene from senary C2-C4 olefin/paraffin mixture," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    6. Jabadurai Jayapaul & Sanna Komulainen & Vladimir V. Zhivonitko & Jiří Mareš & Chandan Giri & Kari Rissanen & Perttu Lantto & Ville-Veikko Telkki & Leif Schröder, 2022. "Hyper-CEST NMR of metal organic polyhedral cages reveals hidden diastereomers with diverse guest exchange kinetics," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. Qingju Wang & Jianbo Hu & Lifeng Yang & Zhaoqiang Zhang & Tian Ke & Xili Cui & Huabin Xing, 2022. "One-step removal of alkynes and propadiene from cracking gases using a multi-functional molecular separator," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    8. Yan Su & Ken-ichi Otake & Jia-Jia Zheng & Ping Wang & Qing Lin & Susumu Kitagawa & Cheng Gu, 2024. "Diffusion-rate sieving of propylene and propane mixtures in a cooperatively dynamic porous crystal," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    9. Lei Wei & Tu Sun & Zhaolin Shi & Zezhao Xu & Wen Wen & Shan Jiang & Yingbo Zhao & Yanhang Ma & Yue-Biao Zhang, 2022. "Guest-adaptive molecular sensing in a dynamic 3D covalent organic framework," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    10. Yun Li & Bo Zhao & Jin-Peng Xue & Jing Xie & Zi-Shuo Yao & Jun Tao, 2021. "Giant single-crystal-to-single-crystal transformations associated with chiral interconversion induced by elimination of chelating ligands," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    11. Jin-Peng Xue & Yang Hu & Bo Zhao & Zhi-Kun Liu & Jing Xie & Zi-Shuo Yao & Jun Tao, 2022. "A spin-crossover framework endowed with pore-adjustable behavior by slow structural dynamics," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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