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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Nanotechnology

Background:

  • Controlling supramolecular polymer composition and aggregation state is crucial.
  • Stabilizing out-of-equilibrium states allows for on-demand release and thermodynamic evolution.
  • Stimuli-responsive containers can trap and redirect supramolecular polymers.

Purpose of the Study:

  • To investigate the use of redox-responsive organosilica nanocages (OSCs) for controlling supramolecular polymer self-assembly.
  • To demonstrate the ability to stabilize kinetically trapped species and release them on demand.
  • To study the self-assembly pathway modulation within complex media, including living cells.

Main Methods:

  • Utilized organosilica nanocages (OSCs) as redox-responsive nanocontainers.
  • Employed a luminescent platinum compound (Pt) to visualize self-assembly and aggregation states via photoluminescence.
  • Investigated the encapsulation and release of Pt aggregates within OSCs triggered by redox stimuli.
  • Monitored supramolecular aggregate evolution within living cells.

Main Results:

  • OSCs successfully encapsulated kinetically trapped, orange-emitting Pt species, preventing their evolution to stable, blue-emitting fibers.
  • Redox-triggered degradation of OSCs enabled on-demand release of trapped Pt species, restoring their self-assembly towards the stable state.
  • Demonstrated control over self-assembly pathways within complex media, including successful intracellular release and fiber formation in living cells.

Conclusions:

  • On-demand confinement using stimuli-responsive nanocontainers is a viable strategy for temporally stabilizing transient species.
  • This approach allows for precise modulation of complex self-assembly pathways in supramolecular polymerization.
  • The study provides a novel method for controlling dynamic processes in supramolecular chemistry with potential applications in complex environments.