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LCST polymers with UCST behavior.

Marzieh Najafi1, Mehdi Habibi2, Remco Fokkink3

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Soft Matter
|January 13, 2021
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Summary
This summary is machine-generated.

Dense dispersions of thermosensitive polymer micelles exhibit glassy behavior near their critical temperature. Micelle size and packing influence mechanical properties, offering insights for designing tunable nanoparticles.

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Area of Science:

  • Polymer Science
  • Materials Science
  • Soft Matter Physics

Background:

  • Investigating temperature-dependent behavior of dense dispersions is crucial for understanding material properties.
  • Flower-like micelles with thermosensitive blocks offer tunable characteristics.
  • Poly(N-isopropylacrylamide) (PNIPAM) is a well-known thermosensitive polymer.

Purpose of the Study:

  • To investigate the temperature-dependent behavior of dense dispersions of core crosslinked flower-like micelles.
  • To understand the relationship between micelle packing, volume fraction, and mechanical properties.
  • To provide insights for designing novel thermosensitive PNIPAM nanoparticles.

Main Methods:

  • Preparation of flower-like micelles using ABA block copolymers with PEG and PNIPAM blocks.
  • Stabilization of micellar core using native chemical ligation (NCL).
  • Characterization of micelle size, packing, and mechanical properties (storage modulus) at various concentrations and temperatures.

Main Results:

  • Micelles showed a radius of ~35 nm above the lower critical solution temperature (LCST) and ~48 nm below the LCST due to PNIPAM hydration.
  • Concentrated dispersions (≥7.5 wt%) exhibited glassy state behavior below a critical temperature (Tc: 28 °C).
  • Storage moduli demonstrated a universal dependence on effective volume fraction, increasing significantly above φ = 1.2, consistent with a disordered lattice model.

Conclusions:

  • Dense dispersions of core crosslinked flower-like micelles display thermosensitive glassy behavior.
  • Micelle packing and effective volume fraction are key determinants of mechanical properties.
  • Findings enable molecular design of thermosensitive PNIPAM nanoparticles with controllable structural and mechanical properties.