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Micelle formation is an intricate process that hinges on the properties of amphiphilic or amphipathic molecules and the conditions of the system in which they are found. Amphiphilic molecules, which have both hydrophilic (water-attracting) and hydrophobic (water-repelling) parts, play a critical role in this process.In aqueous environments, these molecules arrange themselves such that their hydrophilic heads are turned towards the water phase, while their hydrophobic tails are oriented away...
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pH and amphiphilic structure direct supramolecular behavior in biofunctional assemblies.

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Area of Science:

  • Supramolecular chemistry
  • Materials science
  • Nanotechnology

Background:

  • Supramolecular self-assembly enables control over nanostructure morphology and response to stimuli.
  • Developing stimuli-responsive systems is crucial for targeted drug delivery.

Purpose of the Study:

  • To engineer pH-sensitive peptide amphiphiles (PAs) that control nanostructure shape in response to tumor microenvironments.
  • To assess the impact of pH-induced morphological transitions on drug encapsulation and tumor accumulation.

Main Methods:

  • Synthesized two peptide amphiphiles (PAs) incorporating an oligo-histidine H6 sequence.
  • Investigated self-assembly into nanofibers or spherical micelles based on aliphatic tail placement.
  • Evaluated pH-dependent disassembly and reversible morphological changes between pH 6.0 and 6.5.
  • Assessed encapsulation efficiency of camptothecin (CPT) in different nanostructures.
  • Quantified tumor accumulation of pH-sensitive nanofibers versus controls.

Main Results:

  • PAs formed distinct nanoscale morphologies (nanofibers or spherical micelles) controlled by aliphatic tail position.
  • Both PA types exhibited reversible disassembly in acidic conditions (pH 6.0-6.5) due to histidine protonation.
  • H6-based nanofibers achieved up to 60% camptothecin encapsulation efficiency, a sevenfold increase over spherical micelles.
  • pH-sensitive nanofibers demonstrated enhanced tumor accumulation compared to spherical micelles and non-morphology-changing nanofibers.

Conclusions:

  • Morphological transitions of supramolecular nanostructures triggered by pH changes significantly impact drug encapsulation and tumor accumulation.
  • Molecular design of supramolecular self-assembly can be tuned to enhance the pharmacologic properties of nanomedicines.
  • pH-sensitive peptide amphiphiles offer a promising platform for developing advanced cancer nanotherapeutics.