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A series of mussel-inspired pH-responsive self-healing hydrogels based on gelatin crosslinked by oxidized tannic acid (GLT-OTAs) were prepared and used as controlled drug delivery systems (CDDS). An antiphlogistic drug, indomethacin (IDMC) was used as model drug to be immobilized into the hydrogels. The obtained hydrogel samples were characterized by Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD) and scanning electron microscopy (SEM). Mechanical stability, biocompatibility and self-healing property of the hydrogels were estimated, respectively. Swelling and drug release behaviors of these hydrogels were measured in phosphate buffered saline (PBS) with pH 7.4 (simulated intestinal fluid) and HCl solution with pH 1.2 (simulated gastric fluid) at 37 °C. Effect of the OTA content on the structures and characteristics of all samples was discussed. FTIR spectra revealed the covalent cross-linking between gelatin and OTA induced by Michael addition and Schiff base reaction. Both XRD and FTIR all showed the drug (IDMC) was loaded successfully and existed steadily. GLT-OTA hydrogels had satisfactory biocompatibility, superior self-healing. Results also illustrated that the mechanical strength, internal structure, the swelling and drug release behaviors of the GLT-OTAs hydrogel were greatly affected by the OTA content. With increasing the OTA content, the mechanical stability of GLT-OTAs hydrogel became better and better, and their internal structure became more and more compact. The swelling degree (SD) and cumulative drug release of all hydrogel samples tended to decrease with increasing OTA content and both had obvious pH responsiveness. For each hydrogel sample, the cumulative drug release in PBS at pH 7.4 was greater than that in HCl solution at pH 1.2. These results indicated that the obtained GLT-OTAs hydrogel had promising potential to be used as effective pH-responsive and self-healing drug delivery materials.

Mussel-inspired self-healing hydrogel based on gelatin and oxidized tannic acid for pH-responsive controlled drug release