Synthesis and physicochemical characterization of end-linked poly(ethylene glycol)-co-peptide hydrogels formed by Michael-type addition

M. P. Lutolf, J. A. Hubbell

Research output: Contribution to journalArticle

484 Citations (Scopus)

Abstract

The synthesis of novel hybrid hydrogels by stepwise copolymerization of multiarm vinyl sulfone-terminated poly(ethylene glycol) macromers and α-Ω cysteine oligopeptides via Michael-type additions is described. Cross-linking kinetics, studied by in situ rheometry, can be controlled by pH and the presence of charged amino acid residues in close proximity to the Cys, which modulates the pKa of the thiol group. These end-linked networks were characterized by their equilibrium swelling in water, by their viscoelastic properties in the swollen state, and by their soluble fraction. It was demonstrated that structure and properties are very sensitive to the preparation state including stoichiometry and precursor concentration and less sensitive to the pH during cross-linking. For each network the concentration of elastically active chains (v) was calculated from experimentally determined sol fractions using Miller-Macosko theory and compared to values obtained from swelling and rheometry studies and by calculation from Flory's classical network models. Hydrogels were also prepared with varying macromer structures, and their properties were shown to respond to both macromer functionality and molecular weight.

Original languageEnglish
Pages (from-to)713-722
Number of pages10
JournalBiomacromolecules
Volume4
Issue number3
DOIs
StatePublished - May 1 2003
Externally publishedYes

Fingerprint

Hydrogels
Ethylene Glycol
Peptides
Polyethylene glycols
Swelling
Oligopeptides
Polymethyl Methacrylate
Sols
Sulfhydryl Compounds
Stoichiometry
Copolymerization
Cysteine
Amino acids
Molecular Weight
Molecular weight
Amino Acids
Kinetics
Water
divinyl sulfone

ASJC Scopus subject areas

  • Organic Chemistry
  • Biochemistry, Genetics and Molecular Biology(all)
  • Polymers and Plastics
  • Materials Chemistry

Cite this

Synthesis and physicochemical characterization of end-linked poly(ethylene glycol)-co-peptide hydrogels formed by Michael-type addition. / Lutolf, M. P.; Hubbell, J. A.

In: Biomacromolecules, Vol. 4, No. 3, 01.05.2003, p. 713-722.

Research output: Contribution to journalArticle

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