Biomed-X Center, Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China.
Biomed-X Center, Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China; Department of Orthopaedic and Traumatology, The University of Hong Kong, 21 Sassoon Road, Pokfulam, Hong Kong, China.
Acta Biomater. 2019 Jul 1;92:336-350. doi: 10.1016/j.actbio.2019.05.027. Epub 2019 May 11.
Various coatings have been used to slow down the corrosion rate of biomedical magnesium alloys. However, these coatings usually act only as passive barriers. It is much more desirable to endow such coatings with active, biocorrosion-responsive self-repairing capacity. In the present work, a self-healing coating system (denoted as "silk-PA") was constructed in the form of a sandwich architecture of fluoride precoating (bottom), silk-phytic acid (PA) coating (middle), and silk fibroin coating (top). Here, PA was loaded in the middle coating as a corrosion inhibitor by harnessing its strong chelating ability toward dissolving Mg and Ca ions. The self-healing property was evaluated by scratch and SVET tests, and the corrosion resistance was evaluated by in vitro immersion and electrochemical measurements. The results showed that the silk-PA manifested intriguing self-healing capacity with pH responsiveness, hence profiting the corrosion resistance of the Mg-1Ca alloy. The biocompatibility and osteogenic activity of the coating system were further evaluated using MC3T3-E1 cells, and it demonstrated favorable responses in multiple cellular behaviors, i.e., adherence, spreading, proliferation, and differentiation. These findings open new opportunities in the study of self-healing coatings for protection against corrosion in biomedical Mg alloys. STATEMENT OF SIGNIFICANCE: In the present study, a self-healing coating system with pH stimuli-responsiveness and osteogenic activity was fabricated on Mg-1Ca alloy by integrating a silk fibroin barrier coating, a silk fibrin/phytic acid composite coating, and a fluoride precoating. This coating system demonstrated interesting self-healing ability as compared to traditional surface modification layers. Furthermore, the self-healing ability enhanced the corrosion resistance of biomedical magnesium alloys, while effective compositions of the coating system endowed the substrate with osteogenic activity. This work provides some new insights into smart surface modification for biomedical Mg alloys.
各种涂层已被用于减缓生物医学镁合金的腐蚀速率。然而，这些涂层通常仅作为被动屏障。更理想的是为这些涂层赋予主动的、生物腐蚀响应的自修复能力。在本工作中，构建了一种自修复涂层体系（表示为“丝-PA”），其形式为氟化物预处理涂层（底层）、丝-植酸（PA）涂层（中层）和丝素蛋白涂层（顶层）的三明治结构。这里，通过利用 PA 对溶解的 Mg 和 Ca 离子的强螯合能力，将其负载在中间涂层中作为腐蚀抑制剂。通过划痕和 SVET 测试评估了自修复性能，通过体外浸泡和电化学测量评估了耐腐蚀性。结果表明，丝-PA 表现出有趣的 pH 响应自修复能力，从而提高了 Mg-1Ca 合金的耐腐蚀性。进一步使用 MC3T3-E1 细胞评估了涂层体系的生物相容性和成骨活性，它在多种细胞行为，即粘附、铺展、增殖和分化方面表现出良好的响应。这些发现为生物医学镁合金腐蚀防护用自修复涂层的研究开辟了新的机会。
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