Journal
POLYMERS
Volume 12, Issue 5, Pages -Publisher
MDPI
DOI: 10.3390/polym12051185
Keywords
hydrophobically functionalized polyelectrolytes; modified poly(acrylic acid); pH-sensitive structures; self-aggregation in aqueous solution; NMR diffusometry; molecular dynamics simulations
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Funding
- National Science Center Poland [2017/25/B/ST4/02450]
- Polish Ministry of Science and Higher Education [0401/0194/17]
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One of the most important properties of hydrophobically functionalized polyelectrolytes (HF-PEs) and their assemblies is their ability to encapsulate hydrophobic/amphiphilic agents and provide release on demand of the entrapped payload. The aim of the present work was to synthesize and study self-organization behavior in aqueous solution of hydrophobically functionalized poly(acrylic acid) (PAA) comprising the ester-type pH labile moiety with various degrees of hydrophobization and side-chain lengths in the absence and presence of appropriate mono- and polyvalent electrolytes (i.e., NaCl or CaCl2). The synthesis and purification of hydrophobically functionalized PAA were performed under mild conditions in order to avoid chemical degradation of the polymers. The modified polyelectrolytes self-assembly in aqueous systems was monitored using diffusion-ordered nuclear magnetic resonance (DOSY NMR). The performed studies, supported by the all-atoms molecular dynamics simulations, revealed a strong dependence of polyelectrolyte self-assembled state on concentration-specific concentration regions with the coexistence of both smaller and larger aggregates were observed (values of hydrodynamic diameter D-H around one nanometer and between two to six nanometers, respectively). Our investigations enabled us to gain crucial information about the self-assembly of the hydrophobically functionalized poly(acrylic acid) and opened the possibility of understanding and predicting its performance under various conditions.
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