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Acid-Cleavable Poly(ethylene glycol) Hydrogels Displaying Protein Release at pH?5.

ABSTRACT: PEG is the gold standard polymer for pharmaceutical applications, however it lacks degradability. Degradation under physiologically relevant pH as present in endolysosomes, cancerous and inflammatory tissues is crucial for many areas. The authors present anionic ring-opening copolymerization of ethylene oxide with 3,4-epoxy-1-butene (EPB) and subsequent modification to introduce acid-degradable vinyl ether groups as well as methacrylate (MA) units, enabling radical cross-linking. Copolymers with different molar ratios of EPB, molecular weights (M_n ) up to 10?000?g?mol^-1 and narrow dispersities (?<1.05) were prepared. Both the P(EG-co-isoEPB)MA copolymer and the hydrogels showed pH-dependent, rapid hydrolysis at pH?5-6 and long-term storage stability at neutral pH (pH?7.4). By designing the degree of polymerization and content of degradable vinyl ether groups, the release time of an entrapped protein OVA-Alexa488 can be tailored from a few hours to several days (hydrolysis half-life time t_1/2 at pH?5: 13?h to 51?h).

SUBMITTER: Ewald J

PROVIDER: S-EPMC7079179 | biostudies-literature | 2020 Mar

REPOSITORIES: biostudies-literature

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Acid-Cleavable Poly(ethylene glycol) Hydrogels Displaying Protein Release at pH 5.

Ewald Johannes J Blankenburg Jan J Worm Matthias M Besch Laura L Unger Ronald E RE Tremel Wolfgang W Frey Holger H Pohlit Hannah H

Chemistry (Weinheim an der Bergstrasse, Germany) 20200218 13

PEG is the gold standard polymer for pharmaceutical applications, however it lacks degradability. Degradation under physiologically relevant pH as present in endolysosomes, cancerous and inflammatory tissues is crucial for many areas. The authors present anionic ring-opening copolymerization of ethylene oxide with 3,4-epoxy-1-butene (EPB) and subsequent modification to introduce acid-degradable vinyl ether groups as well as methacrylate (MA) units, enabling radical cross-linking. Copolymers with ...[more]

PMID: 31850549

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Project description:Growth factors have been shown to be potent mediators of osteogenesis. However, their use in tissue-engineered scaffolds not only can be costly but also can induce undesired responses in surrounding tissues. Thus, the ability to specifically induce osteogenic differentiation in the absence of exogenous growth factors through manipulation of scaffold material properties would be desirable for bone regeneration. Previous research indicates that addition of inorganic or hydrophobic components to organic, hydrophilic scaffolds can enhance multipotent stem cell (MSC) osteogenesis. However, the combined impact of scaffold inorganic content and hydrophobicity on MSC behavior has not been systematically explored, particularly in three-dimensional (3D) culture systems. The aim of the present study was therefore to examine the effects of simultaneous increases in scaffold hydrophobicity and inorganic content on MSC osteogenic fate decisions in a 3D culture environment toward the development of intrinsically osteoinductive scaffolds. Mouse 10T½ MSCs were encapsulated in a series of novel scaffolds composed of varying levels of hydrophobic, inorganic poly(dimethylsiloxane) (PDMS) and hydrophilic, organic poly(ethylene glycol) (PEG). After 21 days of culture, increased levels of osteoblast markers, runx2 and osteocalcin, were observed in scaffolds with increased PDMS content. Bone extracellular matrix (ECM) molecules, collagen I and calcium phosphate, were also elevated in formulations with higher PDMS:PEG ratios. Importantly, this osteogenic response appeared to be specific in that markers for chondrocytic, smooth muscle cell, and adipocytic lineages were not similarly affected by variations in scaffold PDMS content. As anticipated, the increase in scaffold hydrophobicity accompanying increasing PDMS levels was associated with elevated scaffold serum protein adsorption. Thus, scaffold inorganic content combined with alterations in adsorbed serum proteins may underlie the observed cell behavior.

Dataset Information

Acid-Cleavable Poly(ethylene glycol) Hydrogels Displaying Protein Release at pH?5.

Publications

Acid-Cleavable Poly(ethylene glycol) Hydrogels Displaying Protein Release at pH 5.

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