Partitioning and diffusion of solutes in hydrogels of poly(ethylene oxide)

Merrill, Edward W.; Dennison, Kathleen Anne; Sung, Cynthia

doi:10.1016/0142-9612(93)90154-t

Cited by 233 publications

(211 citation statements)

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“…PEG-DOPA hydrogels were characterized by determination of the average molecular weight between crosslinks (M h c ) as determined from equilibrium swelling data and application of the Flory-Rehner equation. 21,22 Disk-shaped hydrogels with a thickness of 1 mm were formed by addition of oxidizing reagents to aqueous PEG-DOPA solutions and gelation in a PTFE mold for 48 h. The gels were cut into disks of 4 mm diameter, and the mass of the relaxed gel (W r ) was determined. The gels were placed in excess distilled water and allowed to reach equilibrium before the mass of the swollen gels (W s ) was measured.…”

Section: Methodsmentioning

confidence: 99%

“…21 φ was determined experimentally using the method of Gnanou et al 27 Monofunctional IV was cross-linked by the addition of various oxidizing reagents and analyzed using GPC-MALLS 24 h after the initiation of oxidation. In general, GPC results showed two peaks, with one peak having molecular weight between a monomer and a dimer of IV while the molecular weight of the second peak corresponded to a multimer (M h w,s IV g 3M h w,o…”

Section: Methodsmentioning

confidence: 99%

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Synthesis and Gelation of DOPA-Modified Poly(ethylene glycol) Hydrogels

2002

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3,4-Dihydroxyphenylalanine (DOPA) residues are known for their ability to impart adhesive and curing properties to mussel adhesive proteins. In this paper, we report the preparation of linear and branched DOPAmodified poly(ethylene glycol)s (PEG-DOPAs) containing one to four DOPA endgroups. Gel permeation chromatography-multiple-angle laser light scattering analysis of methoxy-PEG-DOPA in the presence of oxidizing reagents (sodium periodate, horseradish peroxidase, and mushroom tyrosinase) revealed the formation of oligomers of methoxy-PEG-DOPA, presumably resulting from oxidative polymerization of DOPA endgroups. In the case of PEG-DOPAs containing two or more DOPA endgroups, oxidative polymerization resulted in polymer network formation and rapid gelation. The amount of time required for gelation of aqueous PEG-DOPA solutions was found to be as little as 1 min and was dependent on the polymer architecture as well as the type and concentration of oxidizing reagent used. Analysis of reaction mixtures by UV-vis spectroscopy allowed the identification of reaction intermediates and the elucidation of reaction pathways. On the basis of the observed reaction intermediates, oxidation of the catechol side chain of DOPA resulted in the formation of highly reactive DOPA-quinone, which further reacted to form cross-linked products via one of several pathways, depending on the presence or absence of N-terminal protecting groups on the PEG-DOPA. N-Boc protected PEG-DOPA cross-linked via phenol coupling and quinone methide tanning pathways, whereas PEG-DOPA containing a free amino group cross-linked via a pathway that resembled melanogenesis. Similar differences were observed for the rate of gel formation as well as the molecular weight between cross-links (M h c ), calculated using equilibrium swelling and the FloryRehner equation.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Synthesis and Gelation of DOPA-Modified Poly(ethylene glycol) Hydrogels

2002

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“…Polyethylene oxide (PEO) is a hydrophilic polymer commonly used in biomedical applications to reduce protein adsorption [1] or improve biocompatibility [2]. The exact mechanism of protein resistance is not known, however PEO density, chain length, conformation, lack of charge, and its interactions with water are all known to affect protein resistance [3][4][5][6].…”

Section: Introductionmentioning

confidence: 99%

X-ray Spectromicroscopy Study of Protein Adsorption to a Polystyrene−Polylactide Blend

et al. 2009

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Abstract:Synchrotron-based X-ray photoemission electron microscopy (X-PEEM) was used to characterize the near surface composition of polyethylene oxide (PEO) combined with 1.5, 5, and 10 wt-% pentaerythritol triacrylate (PETA) cross-linker. It was found that as the concentration of PETA increased, it became the dominant component in the top 10 nm of the film surface. The same surfaces were also exposed to human serum albumin (HSA) and the distributions of the protein relative to PEO and PETA were measured with X-PEEM. A positive correlation was found between levels of PETA and HSA at the surface. Above PETA concentrations of 5 wt-%, HSA adsorption was significant, which suggests high levels of PETA (often used to immobilize PEO by cross-linking) can significantly reduce the non-fouling properties of PEO.

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“…where l is the average bond length (0.146 nm, calculated based on C-C and C-O bond lengths) and C n is the characteristic ratio of the polymer (4.0 for PEG) 28 . Finally, mesh size of the hydrogel can be calculated from equation 8: Hydrogel properties can similarly be tuned by adjusting the amount of PEG used in the formation of hydrogels.…”

Section: Amino Acid Deletion Mw Change (G/mol)mentioning

confidence: 99%

Microwave-assisted Functionalization of Poly(ethylene glycol) and On-resin Peptides for Use in Chain Polymerizations and Hydrogel Formation

Hove

Wilson

Benoit

2013

JoVE

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One of the main benefits to using poly(ethylene glycol) (PEG) macromers in hydrogel formation is synthetic versatility. The ability to draw from a large variety of PEG molecular weights and configurations (arm number, arm length, and branching pattern) affords researchers tight control over resulting hydrogel structures and properties, including Young's modulus and mesh size. This video will illustrate a rapid, efficient, solventfree, microwave-assisted method to methacrylate PEG precursors into poly(ethylene glycol) dimethacrylate (PEGDM). This synthetic method provides much-needed starting materials for applications in drug delivery and regenerative medicine. The demonstrated method is superior to traditional methacrylation methods as it is significantly faster and simpler, as well as more economical and environmentally friendly, using smaller amounts of reagents and solvents. We will also demonstrate an adaptation of this technique for on-resin methacrylamide functionalization of peptides. This on-resin method allows the N-terminus of peptides to be functionalized with methacrylamide groups prior to deprotection and cleavage from resin. This allows for selective addition of methacrylamide groups to the N-termini of the peptides while amino acids with reactive side groups (e.g. primary amine of lysine, primary alcohol of serine, secondary alcohols of threonine, and phenol of tyrosine) remain protected, preventing functionalization at multiple sites. This article will detail common analytical methods (proton Nuclear Magnetic Resonance spectroscopy ( ; H-NMR) and Matrix Assisted Laser Desorption Ionization Time of Flight mass spectrometry (MALDI-ToF)) to assess the efficiency of the functionalizations. Common pitfalls and suggested troubleshooting methods will be addressed, as will modifications of the technique which can be used to further tune macromer functionality and resulting hydrogel physical and chemical properties. Use of synthesized products for the formation of hydrogels for drug delivery and cell-material interaction studies will be demonstrated, with particular attention paid to modifying hydrogel composition to affect mesh size, controlling hydrogel stiffness and drug release.

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Partitioning and diffusion of solutes in hydrogels of poly(ethylene oxide)

Cited by 233 publications

References 10 publications

Synthesis and Gelation of DOPA-Modified Poly(ethylene glycol) Hydrogels

Synthesis and Gelation of DOPA-Modified Poly(ethylene glycol) Hydrogels

X-ray Spectromicroscopy Study of Protein Adsorption to a Polystyrene−Polylactide Blend

Microwave-assisted Functionalization of Poly(ethylene glycol) and On-resin Peptides for Use in Chain Polymerizations and Hydrogel Formation

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