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Orthogonal self-assembly in folding block copolymers.

Nobuhiko Hosono1, Martijn A J Gillissen, Yuanchao Li

  • 1Institute for Complex Molecular Systems, Laboratory of Macromolecular and Organic Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands.

Journal of the American Chemical Society
|November 28, 2012
PubMed
Summary

Researchers created ABA triblock copolymers that fold into single-chain polymeric nanoparticles (SCPNs) using orthogonal self-assembly of benzene-1,3,5-tricarboxamide (BTA) and 2-ureidopyrimidinone (UPy) motifs for compartmentalized nanostructures.

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Area of Science:

  • Polymer Chemistry
  • Supramolecular Chemistry
  • Nanotechnology

Background:

  • ABA triblock copolymers offer a versatile platform for creating complex macromolecular architectures.
  • Orthogonal self-assembly enables the precise control over polymer folding and the formation of nanostructures.
  • Single-chain polymeric nanoparticles (SCPNs) are promising for various applications due to their unique properties.

Purpose of the Study:

  • To synthesize and characterize ABA triblock copolymers with two complementary association motifs.
  • To investigate the orthogonal self-assembly of these motifs for the formation of single-chain polymeric nanoparticles (SCPNs).
  • To demonstrate the formation of compartmentalized SCPNs with distinct microdomains.

Main Methods:

  • Atom-transfer radical polymerization (ATRP) for copolymer synthesis.
  • Postfunctionalization to introduce o-nitrobenzyl-protected 2-ureidopyrimidinone (UPy) and benzene-1,3,5-tricarboxamide (BTA) moieties.
  • Two-step thermal/photoirradiation treatment for sequential self-assembly.
  • Variable-temperature NMR, circular dichroism spectroscopy, size-exclusion chromatography (SEC), small-angle X-ray scattering (SAXS), and atomic force microscopy (AFM) for characterization.

Main Results:

  • Successful synthesis of ABA triblock copolymers with UPy and BTA motifs.
  • Demonstration of orthogonal, intramolecular self-assembly of BTA (helical aggregates) and UPy (dimers) upon sequential stimuli (temperature reduction and photoirradiation).
  • Formation of compartmentalized SCPNs with significant reduction in polymer size (30-60% observed via SEC).
  • Evidence of distinct microdomains within the SCPNs, mimicking protein secondary structures.

Conclusions:

  • Orthogonal self-assembly of complementary motifs in ABA triblock copolymers leads to the formation of compartmentalized SCPNs.
  • The sequential and non-interfering nature of BTA and UPy self-assembly allows for controlled single-chain folding.
  • The resulting SCPNs possess a compartmentalized interior, offering potential for applications requiring distinct microenvironments.