Chitosan-g-hematin: Enzyme-mimicking polymeric catalyst for adhesive hydrogels

Phenol derivative-containing adhesive hydrogels has been widely recognized as having potential for biomedical applications, but their conventional production methods, utilizing a moderate/strong base, alkaline buffers, the addition of oxidizing agents or the use of enzymes, require alternative appro...

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Bibliographic Details
Published in:Acta biomaterialia 2014-01, Vol.10 (1), p.224-233
Main Authors: Ryu, Ji Hyun, Lee, Yuhan, Do, Min Jae, Jo, Sung Duk, Kim, Jee Seon, Kim, Byung-Soo, Im, Gun-Il, Park, Tae Gwan, Lee, Haeshin
Format: Article
Language:English
Subjects:
Adhesion tests
Adhesives - pharmacology
Animals
Biocompatibility
Buffers
Catalysis - drug effects
Catalysts
Catechol
Cell Survival - drug effects
Chitosan
Chitosan - analogs & derivatives
Chitosan - chemical synthesis
Chitosan - chemistry
Chitosan - pharmacology
Cross-Linking Reagents - chemistry
Enzymes
Enzymes - metabolism
Gelation
Hematin
Hemin - analogs & derivatives
Hemin - chemical synthesis
Hemin - chemistry
Hemin - pharmacology
Horseradish peroxidase
Hydrogel
Hydrogels
Hydrogels - pharmacology
Hydrogen-Ion Concentration - drug effects
Mice
NIH 3T3 Cells
Polymers - pharmacology
Solubility - drug effects
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Summary:Phenol derivative-containing adhesive hydrogels has been widely recognized as having potential for biomedical applications, but their conventional production methods, utilizing a moderate/strong base, alkaline buffers, the addition of oxidizing agents or the use of enzymes, require alternative approaches to improve their biocompatibility. In this study, we report a polymeric, enzyme-mimetic biocatalyst, hematin-grafted chitosan (chitosan-g-hem), which results in effective gelation without the use of alkaline buffers or enzymes. Furthermore, gelation occurs under mild physiological conditions. Chitosan-g-hem biocatalyst (0.01%, w/v) has excellent catalytic properties, forming chitosan–catechol hydrogels rapidly (within 5min). In vivo adhesive force measurement demonstrated that the hydrogel formed by the chitosan-g-hem activity showed an increase in adhesion force (33.6±5.9kPa) compared with the same hydrogel formed by pH-induced catechol oxidation (20.6±5.5kPa) in mouse subcutaneous tissue. Using the chitosan-g-hem biocatalyst, other catechol-functionalized polymers (hyaluronic acid–catechol and poly(vinyl alcohol)–catechol) also formed hydrogels, indicating that chitosan-g-hem can be used as a general polymeric catalyst for preparing catechol-containing hydrogels.
ISSN:1742-7061
1878-7568
DOI:10.1016/j.actbio.2013.09.014