Dynamic Light Scattering Study of Self-Assembly of HPMA Hybrid Graft Copolymers
- 22 January 2008
- journal article
- research article
- Published by American Chemical Society (ACS) in Biomacromolecules
- Vol. 9 (2), 510-517
- https://doi.org/10.1021/bm701001f
Abstract
The time course of self-assembly of a hybrid hydrogel system was investigated using dynamic light scattering (DLS) techniques. The self-assembling system consisted of a hydrophilic synthetic N-(2-hydroxypropyl)methacrylamide (HPMA) polymer backbone and a pair of oppositely charged peptide grafts (CCE and CCK). These two distinct pentaheptad peptides were anticipated to act as physical cross-linkers by the formation of antiparallel coiled−coil heterodimers. Equimolar mixture of HPMA graft copolymers CCE-P and CCK-P solutions (where P is the HPMA copolymer backbone) with total concentration from 1.25 to 10 mg/mL were measured at a scattering angle 90° and room temperature. A critical extension of average relaxation time was observed with increasing concentration and incubation time. To reveal the role of coiled−coil grafts in the self-assembly process, a pair of modified random coil peptides, CCEw and CCKy, was designed. The DLS evaluation of HPMA copolymer conjugates (CCEw-P and CCKy-P) at total concentration of 10 mg/mL demonstrated that no association occurred after 28 h of incubation. Moreover, addition of a competing peptide (CCK) or a denaturant (guanidium chloride, GndHCl) to the self-assembled CCE-P/CCK-P hydrogels resulted in partial disassembly or collapse of the hydrogel clusters. These results correlated to changes in the secondary structure of peptides (grafts) as measured by circular dichroism spectroscopy (CD). These investigations supported the hypothesis that the self-assembly of CCE-P/CCK-P into hybrid hydrogels is mediated by the formation of coiled−coil heterodimers.This publication has 36 references indexed in Scilit:
- Hydrogels as smart biomaterialsPolymer International, 2007
- Growth Factor Mediated Assembly of Cell Receptor-Responsive HydrogelsJournal of the American Chemical Society, 2007
- Refolding Hydrogels Self-Assembled from N-(2-Hydroxypropyl)methacrylamide Graft Copolymers by Antiparallel Coiled-Coil FormationBiomacromolecules, 2006
- Hybrid Hydrogels Self-Assembled from HPMA Copolymers Containing Peptide GraftsMacromolecular Bioscience, 2006
- Reversible Hydrogels from Self-Assembling Genetically Engineered Protein Block CopolymersBiomacromolecules, 2005
- Synthetic biomaterials as instructive extracellular microenvironments for morphogenesis in tissue engineeringNature Biotechnology, 2005
- Hybrid hydrogels assembled from synthetic polymers and coiled-coil protein domainsNature, 1999
- Reversible Hydrogels from Self-Assembling Artificial ProteinsScience, 1998
- Long‐term experience with poly(glycol monomethacrylate) gel in plastic operations of the noseJournal of Biomedical Materials Research, 1975
- Hydrophilic Gels for Biological UseNature, 1960