期刊
BIOMACROMOLECULES
卷 14, 期 8, 页码 2814-2821出版社
AMER CHEMICAL SOC
DOI: 10.1021/bm400637s
关键词
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资金
- National Natural Science Foundation of China [NSFC 51003070, 51103093, 51173126, 51273137, 51273139]
- National Science Fund for Distinguished Young Scholars [51225302]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
In situ forming hydrogels were developed from 4-arm poly(ethylene glycol)-methacrylate (PEG-4-MA) and -tetrazole (PEG-4-Tet) derivatives through catalyst-free and bioorthogonal tetrazole-alkene photo-click chemistry. PEG-4-MA and PEG-4-Tet (M-n = 10 kg/mol) were soluble at 37 degrees C in phosphate buffer (PB, pH 7.4, 10 mM) at total polymer concentrations ranging from 20 to 60 wt % but formed fluorescent hydrogels upon 365 nm UV irradiation at an intensity of 20.6, 30.7, or 60 mW/cm(2). The gelation times ranged from ca. 50 s to 5 min, and storage moduli varied from 0.65 to 25.2 kPa depending on polymer concentrations and degrees of Tet substitution in PEG-4-Tet conjugates. The cell experiments via an indirect contact assay demonstrated that these tetrazole-alkene photo-click PEG hydrogels were noncytotoxic. The high specificity of photo-click reaction renders thus obtained PEG hydrogels particularly interesting for controlled protein release. Notably, in vitro release studies showed that cytochrome c (CC), gamma-globulins (Ig), and recombinant human interleukin-2 (rhLL-2) all were released from PEG hydrogels in a sustained and quantitative manner over a period of 14-20 days. Importantly, released CC and rhIL-2 exhibited comparable biological activities to native CC and rhIL-2, respectively. These results confirm that tetrazole-alkene photo-click reaction is highly compatible with these loaded proteins. This photo-controlled, specific, efficient, and catalyst-free click chemistry provides a new and versatile strategy to in situ forming hydrogels that hold tremendous potentials for protein delivery and tissue engineering.
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