期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 6, 页码 7592-7608出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c21260
关键词
injectable hydrogel; phosphate-functionalized chitosan; supramolecular combination; osteogenesis; angiogenesis
资金
- Natural Science Foundation of China [82172432, 82102568, 82001319]
- National & Local Joint Engineering Research Center of Orthopedic Biomaterials [XMHT20190204007]
- Shenzhen Sustainable Development Project [KCXFZ20201221173411031]
- Shenzhen High-level Hospital Construction Fund
- Shenzhen Key Medical Discipline Construction Fund [SZXK023]
- National Science Foundation of Guangdong Province [2019A1515011290]
- Guangdong Basic and Applied Basic Research Foundation [2019A1515110983]
- San-Ming Project of Medicine in Shenzhen [SZSM201612092]
- Bethune Charitable Foundation
- CSPC Osteoporosis Research Foundation Project [G-X-2020-1107-21]
By incorporating MgO nanoparticles into a water-soluble phosphocreatine-functionalized chitosan hydrogel, the researchers were able to overcome the limitations of chitosan-based injectable hydrogels in terms of osteogenic, angiogenic, and mechanical properties. The CSMP-MgO injectable hydrogels showed excellent performance in promoting bone regeneration both in vitro and in vivo.
Natural polysaccharide (NPH)-based injectable hydrogels have shown great potential for critical-sized bone defect repair. However, their osteogenic, angiogenic, and mechanical properties are insufficient. Here, MgO nanoparticles (NPs) were incorporated into a newly synthesized water-soluble phosphocreatine-functionalized chitosan (CSMP) water solution to form an injectable hydrogel (CSMP-MgO) via supramolecular combination between phosphate groups in CSMP and magnesium in MgO NPs to circumvent these drawbacks of chitosan-based injectable hydrogels. Water-soluble chitosan deviate CSMP was first synthesized by grafting methacrylic anhydride and phosphocreatine into a chitosan chain in a one-step lyophilization process. The phosphocreatine in this hydrogel not only provides sites to combine with MgO NPs to form supramolecular binding but also serves as the reservoir to control Mg2+ release. As a result, the lyophilized CSMP-MgO hydrogels presented a porous structure with some small holes in the pore wall, and the pore diameters ranged from 50 to 100 mu m. The CSMP-MgO injectable hydrogels were restricted from swelling in DI water (lowest swelling ratio was 16.0 +/- 1.1 g/g) and presented no brittle failure during compression even at a strain above 85% (maximum compressive strength was 195.0 kPa) versus the control groups (28.0 and 41.3 kPa for CSMP and CSMP-MgO (0.5) hydrogels), with regulated Mg2+ release in a stable and sustained manner. The CSMP-MgO injectable hydrogels promoted in vitro calcium phosphate (hydroxyapatite (HA) and tetracalcium phosphate (TTCP)) deposition in supersaturated calcium phosphate solution and presented no cytotoxicity to MC3T3-E1 cells; the CSMP-MgO hydrogel promoted MC3T3-E1 cell osteogenic differentiation with upregulation of BSP, OPN, and Osterix osteogenic gene expression and mineralization and HUVEC tube formation. Among them, CSMP-MgO (5) presented most of these properties. Moreover, this hydrogel (CSMP-MgO (5)) showed an excellent ability to promote new bone formation in critical-sized calvarial defects in rats. Thus, the CSMP-MgO injectable hydrogel shows great promise for bone regeneration.
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