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Electron-catalysed molecular recognition

Author

Listed:
  • Yang Jiao

    (Northwestern University)

  • Yunyan Qiu

    (Northwestern University)

  • Long Zhang

    (Northwestern University)

  • Wei-Guang Liu

    (California Institute of Technology)

  • Haochuan Mao

    (Northwestern University
    Northwestern University)

  • Hongliang Chen

    (Northwestern University
    Zhejiang University
    ZJU-Hangzhou Global Scientific and Technological Innovation Center)

  • Yuanning Feng

    (Northwestern University)

  • Kang Cai

    (Northwestern University
    Nankai University)

  • Dengke Shen

    (Northwestern University
    Anhui University)

  • Bo Song

    (Northwestern University)

  • Xiao-Yang Chen

    (Northwestern University)

  • Xuesong Li

    (Northwestern University)

  • Xingang Zhao

    (Northwestern University)

  • Ryan M. Young

    (Northwestern University
    Northwestern University)

  • Charlotte L. Stern

    (Northwestern University)

  • Michael R. Wasielewski

    (Northwestern University
    Northwestern University)

  • R. Dean Astumian

    (University of Maine)

  • William A. Goddard

    (California Institute of Technology)

  • J. Fraser Stoddart

    (Northwestern University
    Zhejiang University
    ZJU-Hangzhou Global Scientific and Technological Innovation Center
    University of New South Wales)

Abstract

Molecular recognition1–4 and supramolecular assembly5–8 cover a broad spectrum9–11 of non-covalently orchestrated phenomena between molecules. Catalysis12 of such processes, however, unlike that for the formation of covalent bonds, is limited to approaches13–16 that rely on sophisticated catalyst design. Here we establish a simple and versatile strategy to facilitate molecular recognition by extending electron catalysis17, which is widely applied18–21 in synthetic covalent chemistry, into the realm of supramolecular non-covalent chemistry. As a proof of principle, we show that the formation of a trisradical complex22 between a macrocyclic host and a dumbbell-shaped guest—a molecular recognition process that is kinetically forbidden under ambient conditions—can be accelerated substantially on the addition of catalytic amounts of a chemical electron source. It is, therefore, electrochemically possible to control23 the molecular recognition temporally and produce a nearly arbitrary molar ratio between the substrates and complexes ranging between zero and the equilibrium value. Such kinetically stable supramolecular systems24 are difficult to obtain precisely by other means. The use of the electron as a catalyst in molecular recognition will inspire chemists and biologists to explore strategies that can be used to fine-tune non-covalent events, control assembly at different length scales25–27 and ultimately create new forms of complex matter28–30.

Suggested Citation

  • Yang Jiao & Yunyan Qiu & Long Zhang & Wei-Guang Liu & Haochuan Mao & Hongliang Chen & Yuanning Feng & Kang Cai & Dengke Shen & Bo Song & Xiao-Yang Chen & Xuesong Li & Xingang Zhao & Ryan M. Young & Ch, 2022. "Electron-catalysed molecular recognition," Nature, Nature, vol. 603(7900), pages 265-270, March.
  • Handle: RePEc:nat:nature:v:603:y:2022:i:7900:d:10.1038_s41586-021-04377-3
    DOI: 10.1038/s41586-021-04377-3
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    Citations

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    Cited by:

    1. Yitao Wu & Meiqi Tang & Zeju Wang & Le Shi & Zhangyi Xiong & Zhijie Chen & Jonathan L. Sessler & Feihe Huang, 2023. "Pillararene incorporated metal–organic frameworks for supramolecular recognition and selective separation," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    2. Heng Li & Zhijin Li & Chen Lin & Juli Jiang & Leyong Wang, 2024. "Precise recognition of benzonitrile derivatives with supramolecular macrocycle of phosphorylated cavitand by co-crystallization method," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. 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.
    4. Mittelman, Gur & Eran, Ronen & Zhivin, Lev & Eisenhändler, Ohad & Luzon, Yossi & Tshuva, Moshe, 2023. "The potential of renewable electricity in isolated grids: The case of Israel in 2050," Applied Energy, Elsevier, vol. 349(C).
    5. Prakash, Abhijith & Ashby, Rohan & Bruce, Anna & MacGill, Iain, 2023. "Quantifying reserve capabilities for designing flexible electricity markets: An Australian case study with increasing penetrations of renewables," Energy Policy, Elsevier, vol. 177(C).

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