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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Chemical Biology

Background:

  • Molecular recognition is crucial for biological processes, driving research into artificial hosts.
  • Designing artificial hosts for multiple guests (≥4) presents significant challenges in principles and quantification.
  • Existing artificial host designs often lack the complexity to mimic intricate biological recognition events.

Purpose of the Study:

  • To synthesize and characterize novel artificial host systems capable of complex multiguest binding.
  • To investigate the dynamic conformational adaptability of artificial hosts in response to multiple guests.
  • To explore advanced host-guest binding scenarios and their quantification.

Main Methods:

  • Synthesis of rhombic dodecahedral cages [(Zn/Fe)8Pd6-MOC-16].
  • Analysis of host-guest binding events using Nuclear Magnetic Resonance (NMR) and Electrospray Ionization Mass Spectrometry (ESI-MS).
  • Investigation of conformational dynamics through metal-center lability.

Main Results:

  • Two rhombic dodecahedral cages with 12 adaptive pockets were successfully synthesized.
  • These cages demonstrated the ability to capture a wide range of guests (4-24), exhibiting complex binding scenarios.
  • The host-guest interactions displayed a broad dynamic-fit, allowing conformational adjustments beyond traditional induced-fit or conformational selection models.
  • NMR and ESI-MS revealed the complexity of binding events and highlighted challenges in quantifying affinities for multiple guests.

Conclusions:

  • The developed cages exhibit exceptional high-order and hierarchical encapsulation, showcasing a sophisticated dynamic-fit mechanism.
  • These findings advance the understanding of artificial host design for complex molecular recognition.
  • The study underscores the necessity of employing multiple analytical techniques for reliable characterization of multiguest binding events.