Bilayered HA/CS/PEGDA hydrogel with good biocompatibility and self-healing property for potential application in osteochondral defect repair

doi:10.1016/j.jmst.2017.11.016

材料科学与技术 ›› 2018, Vol. 34 ›› Issue (6): 1016-1025.DOI: 10.1016/j.jmst.2017.11.016

所属专题： Biomaterials 2018

收稿日期:2017-03-08 修回日期:2017-03-14 接受日期:2017-03-23 出版日期:2018-06-10 发布日期:2018-06-05
作者简介:
¹These authors contributed equally to this work.

Bilayered HA/CS/PEGDA hydrogel with good biocompatibility and self-healing property for potential application in osteochondral defect repair

Baihao You^a^b,1, Qingtao Li^b^c,1, Hua Dong^a^b, Tao Huang^d, Xiaodong Cao^a^b^*(), Hua Liao^d^**()

^aSchool of Materials Science and Engineering, South China University of Technology, Guangzhou 510641, China
^bNational Engineering Research Centre for Tissue Restoration and Reconstruction, Guangzhou 510006, China
^cSchool of Medicine, South China University of Technology, Guangzhou 510006, China
^dDepartment of Anatomy, Guangdong Provincial Key Laboratory of Construction and Detection in Tissue Engineering, Southern Medical University, Guangzhou 510515, China

Received:2017-03-08 Revised:2017-03-14 Accepted:2017-03-23 Online:2018-06-10 Published:2018-06-05
Contact: Cao Xiaodong,Liao Hua

摘要/Abstract

Abstract:

The fabrication of osteochondral tissue engineering scaffolds comprised of different layers is a big challenge. Herein, bilayers comprised of double network hydrogels with or without nano hydroxyapatite (HAp) were developed by exploiting the radical reaction of poly(ethylene glycol) diacrylate (PEGDA) and the Schiff-base reaction of N-carboxyethyl chitosan (CEC) and oxidized hyaluronic acid sodium (OHA) for osteochondral tissue engineering. The bilayered osteochondral scaffold was successfully fabricated based on the superior self-healing property of both hydrogels and evaluated by scanning electron microscopy, macroscopic observation and mechanical measurements. In addition, the hydrogels exhibited good biocompatibility as demonstrated by the in vitro cytotoxicity and in vivo implantation tests. The results indicated that the bilayered hydrogel had great potential for application in osteochondral tissue engineering.

Key words: Bilayered hydrogel, Self-healing, Osteochondral scaffold, Chitosan, Hyaluronic acid

. [J]. 材料科学与技术, 2018, 34(6): 1016-1025.

Baihao You, Qingtao Li, Hua Dong, Tao Huang, Xiaodong Cao, Hua Liao. Bilayered HA/CS/PEGDA hydrogel with good biocompatibility and self-healing property for potential application in osteochondral defect repair[J]. J. Mater. Sci. Technol., 2018, 34(6): 1016-1025.

图/表 10

Fig. 1. (A) Synthesis steps of CEC and OHA. (B) Schematic of the double networks of SC and SS hydrogels.

Fig. 2. (A) FTIR spectra of CS, CEC, HA and OHA, the arrows indicate the characteristic peaks. (B) 1H NMR spectra in D2O of CEC, the peaks labeled by 1, 2 were the methyl protons of acetamido and the methylene protons of carboxyethyl, respectively.

Fig. 3. The macroscopic self-healing property of PEGDA, SC and SS hydrogels. (A) Two pieces of each kind of hydrogels were prepared and one was stained with rhodamine B. (B) All the hydrogels were cut into 4 pieces and recombined with alternate colors. (C) After healing for 2 h, all the hydrogels turned red. (D, E) When PBS was added, PEGDA hydrogel was separated into 4 pieces immediately, while SC and SS hydrogels still remained integrity, even after immersing in PBS for 24 h.

Fig. 4. The rheological measurements of SC and SS hydrogels. (A) G' and G” of SS hydrogel on strain sweep. G' and G” in continuous step strain (1% strain → 100% strain → 1% strain) measurements: (B) SC hydrogel and (C) SS hydrogel.

Fig. 5. (A) Preparation of the bilayered osteochondral scaffold and (B) its micro and macro (inserted image) morphology after lyophilization. Scale bar: 100 μm. (C) The macroscopic self-healing property of the osteochondral scaffold.

Fig. 6. (A) Weight swelling ratio and (B) volume swelling ratio of SC and SS hydrogels.

Fig. 7. (A) Compressive stress-strain curves and (B) compressive modulus of SC and SS hydrogels before and after healing for 30 min. (C) The healing efficiency of SC and SS hydrogels.

Fig. 8. (A) Compressive stress-strain curve and (B) compressive modulus of SO hydrogel. (C) Schematic of the push-out experiment evaluating interfacial integration performance of SO hydrogel. (D) Interfacial integration stress of SO hydrogel enhanced by prolonging the healing time.

Fig. 9. Live/dead staining of the rabbit BMSCs encapsulated in (A) SC and (B) SS hydrogels after 3 days of cultivation. (C) Cell viability at day 1, 3, 5, 7 detected by CCK-8 assay.

Fig. 10. Histological observation of the (A, C) SC hydrogel and (B, D) SS hydrogel being implanted subcutaneously, on (A, B) day 10 and (C, D) day 20 post-implanting. The right of the red dash lines, the implant. Scale bar: 100 μm.

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Bilayered HA/CS/PEGDA hydrogel with good biocompatibility and self-healing property for potential application in osteochondral defect repair

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