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 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 5 min). In vivo adhesive force measurement demonstrated that the hydrogel formed by the chitosan-g-hem activity showed an increase in adhesion force (33.6 ± 5.9 kPa) compared with the same hydrogel formed by pH-induced catechol oxidation (20.6 ± 5.5 kPa) 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.
Graduate School of Nanoscience and Technology (WCU), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea; Molecular-level Interface Research Center, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea.
Ji Hyun
JH
Ryu
Yuhan
Y
Lee
Min Jae
MJ
Do
Sung Duk
SD
Jo
Jee Seon
JS
Kim
Byung-Soo
BS
Kim
Gun-Il
GI
Im
Tae Gwan
TG
Park
Haeshin
H
Lee
D000269:Adhesives / Q000494:pharmacology*; D000818:Animals; D002384:Catalysis / Q000187:drug effects; D002470:Cell Survival / Q000187:drug effects; D048271:Chitosan / Q000031:analogs & derivatives* / Q000138:chemical synthesis / Q000737:chemistry / Q000494:pharmacology*; D003432:Cross-Linking Reagents / Q000737:chemistry; D004798:Enzymes / Q000378:metabolism*; D006427:Hemin / Q000031:analogs & derivatives* / Q000138:chemical synthesis / Q000737:chemistry / Q000494:pharmacology; D020100:Hydrogels / Q000494:pharmacology*; D006863:Hydrogen-Ion Concentration / Q000187:drug effects; D051379:Mice; D041681:NIH 3T3 Cells; D011108:Polymers / Q000494:pharmacology*; D012995:Solubility / Q000187:drug effects
D000269:Adhesives; D003432:Cross-Linking Reagents; D004798:Enzymes; D020100:Hydrogels; D011108:Polymers; D006427:Hemin; D048271:Chitosan
Catechol; Chitosan; Hematin; Horseradish peroxidase; Hydrogel