The role of hydrophobic modification on hyaluronic acid dynamics and self-assembly. (15th February 2018)

• Record Type: Journal Article
• Authors: Payne, William M.; Svechkarev, Denis; Kyrychenko, Alexander; Mohs, Aaron M.
• Is Part Of: Carbohydrate polymers. Volume 182(2018)
• Page Start: 132
• Page End: 141
• Publication Date: 2018-02-15
• Subjects: HA hyaluronic acid -- CAC critical aggregation concentration -- DLS dynamic light scattering -- MD molecular dynamics -- Rg radius of gyration -- NMR nuclear magnetic resonance -- FF force field -- SAS solvent accessible surface; Polymeric nanoparticles -- Molecular dynamics -- Structure-property relationship -- Nanocarrier -- Self-assembly -- Computer-aided formulation design; Polysaccharides -- Periodicals; Polysaccharides -- Periodicals; Polysaccharides -- Périodiques; Electronic journals; 547.78
• DOI: 10.1016/j.carbpol.2017.10.054
• Languages: English
• ISSNs: 0144-8617

Abstract

Graphical abstract: Highlights: Colloidal properties of HA-based nanomaterials result from single strand dynamics. Results of MD simulations are supported experimentally. Trends observed in silico are also observed in bulk solution experiments. Abstract: The advent of nanomedicine has rejuvenated the need for increased understanding of the fundamental physicochemical properties of polymeric amphiphiles. Hyaluronic acid (HA) is a hydrophilic polysaccharide that is frequently conjugated to hydrophobic moieties and then used to entrap dyes and therapeutics. Here, we develop computational models to examine the effects of the hydrophobic modification on supramolecular behavior among three systematically designed HA derivatives substituted with alkyl chains of increasing length. Our simulations coalesce with experimentally obtained results to demonstrate the dependence of supramolecular behavior on intramolecular forces. We show that the formation of clearly defined hydrophobic domains in samples of octadecylamine-modified HA compared to HA conjugates with shorter alkyl chains is a result of more favorable hydrophobic interactions. Trends in hydrodynamic radius and polydispersity are observed in experimental results that coalesce with theoretical calculations, suggesting that supramolecular properties are dependent on the physicochemical characteristics of individual polymer strands.