电泳沉积制备微弧氧化钛表面氧化镁涂层及其生物学性能

doi:10.15541/jim20230198

无机材料学报 ›› 2023, Vol. 38 ›› Issue (12): 1441-1448.DOI: 10.15541/jim20230198

所属专题：【生物材料】骨骼与齿类组织修复(202312)

电泳沉积制备微弧氧化钛表面氧化镁涂层及其生物学性能

杜佳恒¹^,²(), 范鑫丽³^,⁴, 肖东琴², 尹一然¹, 李忠¹, 贺葵¹, 段可¹()

1.西南医科大学附属医院骨与关节外科, 四川省骨科置入器械研发及应用技术工程实验室, 泸州 646000
2.川北医学院第二临床学院, 南充市中心医院组织工程与干细胞研究所, 南充 637000
3.山东大学齐鲁医学院口腔医学院, 口腔医院口腔颌面外科, 济南 250012
4.山东省口腔组织再生重点实验室, 山东省口腔生物材料与组织再生工程实验室, 山东省口腔疾病临床医学研究中心, 济南 250012

收稿日期:2023-04-18 修回日期:2023-06-03 出版日期:2023-10-15 网络出版日期:2023-10-15
通讯作者: 段可, 教授. E-mail: keduan@swmu.edu.cn
作者简介:杜佳恒(1997-), 男, 硕士研究生. E-mail: dujiaheng1011@163.com
基金资助:
国家自然科学基金面上项目(52071277);四川省科技计划(2020YFS0455);四川省科技计划(2022YFS0628);泸州市-西南医科大学合作项目(2020LZXNYDZ08);泸州市-西南医科大学合作项目(2020LZXNYDF02);西南医科大学产学研项目(2022CXY03);泸县西南医科大学联合课题(2020LXXNYKD-01)

Electrophoretic Coating of Magnesium Oxide on Microarc-oxidized Titanium and Its Biological Properties

DU Jiaheng¹^,²(), FAN Xinli³^,⁴, XIAO Dongqin², YIN Yiran¹, LI Zhong¹, HE Kui¹, DUAN Ke¹()

1. Engineering Laboratory of Orthopaedic Implant Device R&D and Application Technology, Sichuan Province, Department of Bone and Joint Surgery, Affiliated Hospital of Southwest Medical University, Luzhou 646000, China
2. Research Institute of Tissue Engineering and Stem Cells, Nanchong Central Hospital, the Second Clinical College of North Sichuan Medical College, Nanchong 637000, China
3. Department of Oral and Maxillofacial Surgery, Qilu School of Stomatology, Stomatological Hospital of Shandong University, Jinan 250012, China
4. Shandong Key Laboratory of Oral Tissue Regeneration, Shandong Engineering Laboratory of Oral Biomaterials and Tissue Regeneration, Shandong Clinical Medical Research Center for Oral Diseases, Jinan 250012, China

Received:2023-04-18 Revised:2023-06-03 Published:2023-10-15 Online:2023-10-15
Contact: DUAN Ke, professor. E-mail: keduan@swmu.edu.cn
About author:DU Jiaheng (1997-), male, Master candidate. E-mail: dujiaheng1011@163.com
Supported by:
National Natural Science Foundation of China(52071277);Science & Technology Program of Sichuan Province(2020YFS0455);Science & Technology Program of Sichuan Province(2022YFS0628);Luzhou-SWMU Cooperation Program(2020LZXNYDZ08);Luzhou-SWMU Cooperation Program(2020LZXNYDF02);Industry-University Research Project of SWMU(2022CXY03);Luxian-SWMU Joint Project(2020LXXNYKD-01)

摘要/Abstract

摘要：

骨科钛内置物存在感染的风险, 需要开发具有抗菌性、生物相容性且不易产生耐药性的表面涂层。通过电泳沉积15、30、45、60 s在微弧氧化(MAO)的钛表面制备了4组纳米氧化镁(MgO)涂层。MgO颗粒在MAO表面形成均匀涂层, 覆盖率随电泳时间延长。与金黄色葡萄球菌共培养6 h后, 4组样品抗菌率分别为1%、69%、83%、84%; 共培养24 h后抗菌率分别为81%、86%、89%、98%。显微观察发现MgO沉积样品表面黏附细菌密度、活细菌比例均随沉积时间延长而减少。与小鼠成骨细胞共培养1 d后, 4组样品存活率(相对空白孔板中所接种细胞)分别为108%、89%、53%、27%, 5 d后分别为139%、117%、112%、66%。荧光显微观察发现MAO样品表面未见死细胞, 而MgO沉积样品表面死细胞比例随沉积时间延长而增加, 但在实验周期(5 d)内均<5%。本研究表明电泳沉积30 s制备的MgO涂层具有良好的体外抗菌性和生物相容性。

关键词: 钛, 内置物, 抗菌, 微弧氧化, 氧化镁, 电泳沉积

Abstract:

Titanium orthopaedic implants present a risk of infection and require the development of antibacterial, but still biocompatible and non-resistant coatings. Magnesium oxide (MgO) coatings were prepared on micro-arc oxidized titanium by electrophoretic deposition for 15, 30, 45, or 60 s. Nano-sized MgO particles agglomerated to form homogeneous coatings with surface coverage increasing with the duration of deposition. The four groups produced antibacterial rates of 1%, 69%, 83%, and 84% after co-cultured with S. aureus for 6 h, and 81%, 86%, 89%, and 98% after co-cultured for 24 h. Electron and fluorescence microscopies showed decreasing density of bacterial cells and proportion of living cells with increasing time of deposition. Mouse osteoblasts seeded on the four groups had survival rates of 108%, 89%, 53%, and 27% on day 1, and 139%, 117%, 112%, and 66% on day 5. Proportion of dead cells on the coated samples increased with increasing time of deposition but less than 5% on day 5. These results indicate that MgO coatings prepared by electrophoretic deposition for 30 s is reasonable in vitro antibacterial activities and cytocompatibility.

Key words: titanium, implant, antibacterial, micro-arc oxidation, magnesium oxide, electrophoretic deposition

中图分类号:

R318

杜佳恒, 范鑫丽, 肖东琴, 尹一然, 李忠, 贺葵, 段可. 电泳沉积制备微弧氧化钛表面氧化镁涂层及其生物学性能[J]. 无机材料学报, 2023, 38(12): 1441-1448.

DU Jiaheng, FAN Xinli, XIAO Dongqin, YIN Yiran, LI Zhong, HE Kui, DUAN Ke. Electrophoretic Coating of Magnesium Oxide on Microarc-oxidized Titanium and Its Biological Properties[J]. Journal of Inorganic Materials, 2023, 38(12): 1441-1448.

图/表 11

图1 (a, b) 纳米MgO的低、高倍SEM形貌及(c)纳米MgO/丙酮悬浊液浊度随时间的变化曲线

Fig. 1 (a, b) Low and high-power SEM images of nano-MgO powder used and (c) variation of turbidity of nano-MgO/acetone suspension with time

图2 样品的SEM表面形貌

Fig. 2 SEM images of samples MAO at low (a) and high (b) magnification ratios; (c) MAO-MgO15; (d) MAO-MgO30; (e) MAO-MgO45; (f) MAO-MgO60

图3 样品的(a) EDS谱图和(b) Mg元素面分布图

Fig. 3 (a) EDS spectra and (b) Mg mappings of samples All scale bars: 40 μm

图4 样品的SEM截面形貌和Mg元素面分布

Fig. 4 Sectional SEM images and Mg mappings of samples (a, e) MAO-MgO15; (b, f) MAO-MgO30; (c, g) MAO-MgO45; (d, h) MAO-MgO60

图5 各组样品XRD谱图

Fig. 5 XRD patterns of samples

图6 各组样品镁离子累计释放量

Fig. 6 Cumulative release of Mg2+ from samples (a) MAO-MgO15; (b) MAO-MgO30; (c) MAO-MgO45; (d) MAO-MgO60

图7 (a)各组样品与细菌共培养24 h后冲洗液涂板形成菌落的典型照片及(b)共培养后的抗菌率

Fig. 7 (a) Representative photographs of colonies formed on samples after co-cultured with S. aureus for 24 h, and (b) antibacterial rates Numbers 2, 3 and 4 indicating MAO vs. MAO-MgO30, MAO-MgO45, MAO-MgO60, respectively (p<0.05)

图8 各组样品与细菌共培养24 h并活/死染色后的荧光显微照片

Fig. 8 Micrographs of samples after Live/Dead fluorescent staining on co-cultured S. aureus for 24 h Red pixels: Dead S. aureus cells; Green pixels: Alive S. aureus cells; All scale bars: 100 μm

图9 样品接种细菌培养24 h后表面SEM形貌

Fig. 9 SEM micrographs of samples (a) MAO and (b-e) MAO-MgO15 to MAO-MgO60 after co-culture with S. aureus for 24 h; Red arrows pointing to S. aureus cells

图10 细胞接种在样品表面培养1~5 d后的相对存活率

Fig. 10 Viability of rat osteoblasts after co-culture on samples for 1, 3 and 5 d Numbers 3, 4 and 5 indicating MAO vs. MAO-MgO30, MAO-MgO45, MAO-MgO60, respectively (p<0.05)

图11 各组样品与细胞共培养5 d并活/死染色后的荧光显微照片

Fig. 11 Images of samples after Live/Dead fluorescent staining on co-cultured rat osteoblasts for 5 d Red pixels: Dead cells; Green pixels: Alive cells; All scale bars: 100 μm

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电泳沉积制备微弧氧化钛表面氧化镁涂层及其生物学性能

Electrophoretic Coating of Magnesium Oxide on Microarc-oxidized Titanium and Its Biological Properties

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