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Three-Component Supramolecular System with Multistimuli-Responsive Properties in Water.

Bin Wang1, Hua-Ji Liu2, Xiao-Bin Fu3

  • 1Department of Chemistry, School of Sciences, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Wei Jin Road 92, Tianjin, 300072, P. R. China.

Chemistry, an Asian Journal
|June 3, 2015
PubMed
Summary

This study details the creation of novel supramolecular complexes using hyperbranched polyethylenimine, PABA, and alpha-cyclodextrin. These complexes display unique thermoresponsive behaviors influenced by component concentrations, pH, and light-induced isomerization.

Keywords:
light-responsivepolymerssupramolecular complexesthermoresponsive

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Area of Science:

  • Supramolecular Chemistry
  • Polymer Science
  • Materials Science

Background:

  • Hyperbranched polyethylenimine terminated with isobutyramide groups (HPEI-IBAm) is a versatile polymer scaffold.
  • 4-(phenylazo)benzoic acid (PABA) is an azobenzene derivative capable of photoisomerization.
  • α-cyclodextrin (α-CD) is a cyclic oligosaccharide known for its host-guest complexation abilities.

Purpose of the Study:

  • To assemble and characterize three-component supramolecular complexes of HPEI-IBAm, PABA, and α-CD.
  • To investigate the thermoresponsive properties of these complexes, focusing on cloud point temperature (Tcp).
  • To explore the influence of component concentrations, pH, and photoisomerization on the complex's behavior.

Main Methods:

  • Formation of three-component supramolecular complexes at pH≈7.
  • Characterization using NMR spectroscopy ((1)H and 2D ROESY).
  • UV/Vis spectrometric titration to assess complex stoichiometry and binding.
  • Cloud point temperature (Tcp) measurements to evaluate thermoresponsive behavior.
  • Photoisomerization studies using UV/Vis light irradiation.

Main Results:

  • Successful assembly of HPEI-IBAm/PABA/α-CD supramolecular complexes confirmed by NMR.
  • Complexation studies indicated limited α-CD content and incomplete PABA complexation.
  • The complexes exhibited thermoresponsive behavior, with Tcp significantly affected by α-CD concentration, PABA concentration, and pH.
  • Increasing α-CD concentration initially caused a sharp rise in Tcp, followed by a gradual increase.
  • pH variations (≈7 to ≈9) had differential effects on Tcp depending on α-CD concentration.
  • Trans-to-cis photoisomerization of PABA units decreased the Tcp, a different outcome compared to two-component systems.

Conclusions:

  • The three-component supramolecular complexes demonstrate tunable thermoresponsive properties.
  • The interplay between component ratios, pH, and photoisomerization offers a pathway for designing smart materials.
  • Photoisomerization of azobenzene moieties provides a light-triggered mechanism to modulate the complex's aqueous behavior.