期刊
MACROMOLECULAR RAPID COMMUNICATIONS
卷 41, 期 14, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/marc.202000287
关键词
hydrogels; non-covalent gelation; supramolecular chemistry; tetrazine click chemistry
资金
- National Institute of Arthritis and Musculoskeletal and Skin Diseases of the National Institutes of Health [R21 AR071625]
The discovery of tetrazine click-induced secondary interactions is reported as a promising new tool for polymeric biomaterial synthesis. This phenomenon is first demonstrated as a tool for poly(ethylene glycol) (PEG) hydrogel assembly via purely non-covalent interactions and is shown to yield robust gels with storage moduli one to two orders of magnitude higher than other non-covalent crosslinking methods. In addition, tetrazine click-induced secondary interactions also enhance the properties of covalently crosslinked hydrogels. A head-to-head comparison of PEG hydrogels crosslinked with tetrazine-norbornene and thiol-norbornene click chemistry reveals an approximately sixfold increase in storage modulus and unprecedented resistance to hydrolytic degradation in tetrazine click-crosslinked gels without substantial differences in gel fraction. Molecular dynamic simulations attribute these differences to the presence of secondary interactions between the tetrazine-norbornene cycloaddition products, which are absent in the thiol-norbornene crosslinked gels.
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