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  3. Programmable Molecular Dethreading Towards Tunable Drug Release.
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  3. Programmable Molecular Dethreading Towards Tunable Drug Release.

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Programmable molecular dethreading towards tunable drug release.

Shen Sheng1, Yuanhe Li2, Ryan Ray Yen Lee1

  • 1Department of Pharmacy and Pharmaceutical Sciences National University of Singapore 4 Science Drive 2, Singapore, Singapore.

Nature Communications
|October 23, 2025

View abstract on PubMed

Summary
This summary is machine-generated.

Researchers engineered molecular machines by controlling pseudorotaxane dethreading. This breakthrough allows tunable molecular motion, paving the way for programmable drug delivery systems and advanced biomedical applications.

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Nanotechnology

Background:

  • Precise control of molecular motion is crucial for developing artificial molecular machines.
  • Pseudorotaxane dethreading is a key process in interlocked architectures for regulating molecular motion.
  • Predictable and programmable control over dethreading kinetics remains a significant challenge.

Purpose of the Study:

  • To achieve systematic modulation of pseudorotaxane dethreading behavior through component engineering.
  • To establish structure-kinetic relationships governing dethreading pathways.
  • To demonstrate the potential of engineered pseudorotaxanes in drug delivery applications.

Main Methods:

  • Utilized a pseudorotaxane platform with 24-crown-8-based macrocycles and adjustable benzylic amine stoppers.
  • Performed systematic component engineering to modulate dethreading kinetics.
  • Employed crystallographic analyses and computational modeling to elucidate dethreading mechanisms.
  • Functionalized pseudorotaxane assemblies with the anticancer agent camptothecin for proof-of-concept studies.

    • Main Results:

    • Demonstrated continuous tunability of activation energies for dethreading within the range of 22 to 30 kcal/mol, with fine resolution.
    • Elucidated the dethreading pathway and structure-kinetic relationships using crystallographic and computational methods.
    • Showcased a consistent correlation between dethreading rates and cytotoxic potency in camptothecin-functionalized pseudorotaxanes.

    Conclusions:

    • Developed a generalizable strategy for designing programmable drug delivery systems by engineering molecular machines.
    • Bridged molecular-scale mechanical motion with biological effects through controlled pseudorotaxane dethreading.
    • Laid the foundation for advanced molecular machines in biomedical applications using a novel pseudorotaxane toolkit.