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Design of polyelectrolyte core-shells with DNA to control TMPyP binding.

Vanda Vaz Serra1, Raquel Teixeira2, Suzana M Andrade2

  • 1Centro de Química Estrutural, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais 1, 1049-001 Lisboa, Portugal; Unidade de Química Orgânica e Produtos Naturais, Departamento de Química, Universidade de Aveiro, Portugal.

Colloids and Surfaces. B, Biointerfaces
|June 11, 2016
PubMed
Summary

DNA adsorption onto polyelectrolyte core-shells alters interactions with 5,10,15,20-tetrakis(4-N-methylpyridiniumyl)porphyrin (TMPyP). This enhances TMPyP uptake and favors intercalation into GC-rich DNA regions.

Keywords:
DNAFluorescence Lifetime Imaging (FLIM)Polyelectrolyte core-shellsPorphyrins

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Area of Science:

  • Materials Science
  • Biochemistry
  • Nanotechnology

Background:

  • Polyelectrolyte multilayers (PEM) are versatile nanomaterials with tunable properties.
  • 5,10,15,20-tetrakis(4-N-methylpyridiniumyl)porphyrin (TMPyP) is a cationic porphyrin with DNA binding capabilities.
  • Understanding DNA-polyelectrolyte interactions is crucial for developing advanced biomaterials.

Purpose of the Study:

  • To investigate the influence of DNA adsorption on TMPyP interactions within poly(sodium 4-styrenesulfonate) (PSS)/poly(allylamine hydrochloride) (PAH) core-shell structures.
  • To characterize the conformational changes of DNA upon adsorption and TMPyP encapsulation.
  • To explore the potential of these core-shells as platforms for controlled drug delivery or sensing.

Main Methods:

  • Layer-by-layer (LbL) adsorption to create PSS/PAH polyelectrolyte core-shells.
  • Steady-state and time-resolved fluorescence spectroscopy to monitor TMPyP-DNA interactions.
  • Fluorescence Lifetime Imaging Microscopy (FLIM) for spatial analysis of TMPyP distribution.
  • Circular dichroism (CD) spectroscopy to assess DNA conformational changes.

Main Results:

  • DNA adsorption significantly increased TMPyP uptake within the PSS/PAH core-shells.
  • DNA adsorption altered specific DNA/TMPyP interactions, favoring porphyrin intercalation into GC-rich regions.
  • DNA exhibited significant conformational changes upon adsorption, which were reversible upon TMPyP encapsulation.

Conclusions:

  • Polyelectrolyte core-shells provide a dynamic environment that modulates DNA-TMPyP interactions.
  • The observed changes in TMPyP uptake and binding specificity highlight the potential of these systems for targeted molecular interactions.
  • Reversible DNA conformational changes offer possibilities for stimuli-responsive material design.