由痕量 Mn(III) 耦合 H 空位驱动的 ROS 生成使羟基磷灰石的有效抗菌活性,Journal of Materials Chemistry B

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由痕量 Mn(III) 耦合 H 空位驱动的 ROS 生成使羟基磷灰石的有效抗菌活性
Journal of Materials Chemistry B ( IF 6.1 ) Pub Date : 2021-3-17 , DOI: 10.1039/d1tb00098e
Ming Wang ₁ , Miao Li , Yunli Wang , Yiran Shao , Yingchun Zhu , Shiping Yang

Affiliation

羟基磷灰石（HA）由于其生物相容性和生物活性在医学应用中引起了广泛关注。然而，HA的感染问题仍然是植入失败的主要原因之一。因此，迫切需要赋予HA生物材料抗菌活性。在此，高抗菌活性是通过在空气中通过简单的热处理策略在 HA 中引入痕量 Mn ³⁺和 H 空位图片 ID：d1tb00098e-t1.gif

对来实现的。理论结果表明Mn ³⁺优先取代HA 结构中的Ca(2) 位点，在相邻的OH ^-位点出现电荷补偿H 空位。抗菌试验表明，Mn-HA 对两种大肠杆菌均具有抗菌活性。和金黄色葡萄球菌的痕量 Mn 含量在 ppm 水平，这表明 Mn ³⁺和图片 ID：d1tb00098e-t2.gif

中心可能在抗菌过程中起重要作用。Mn ³⁺和图片 ID：d1tb00098e-t3.gif

Mn-HA 中的对分别作为氧化和还原中心，然后可以共同参与CoQ/CoQH ₂氧化还原循环并协同促进CoQ˙ ^-和ROS自由基的积累。这种增强的 ROS 产生是赋予 Mn-HA 有效抗菌活性的主要因素。此外，体外生物活性测定表明，Mn-HA 材料表现出增强的成骨活性和良好的生物相容性。因此，这项工作不仅提供了一种可行的方法来控制 HA 中 Mn 元素的氧化态，而且还提出了一种新的痕量 Mn ³⁺掺杂的 HA 在组织工程中的潜在应用。

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Efficient antibacterial activity of hydroxyapatite through ROS generation motivated by trace Mn(III) coupled H vacancies

Hydroxyapatite (HA) has attracted wide attention for medical application due to its biocompatibility and bioactivity. However, the infection problems of HA remain among the leading reasons for implantation failure. Thus, it is urgent to endow HA biomaterials with antibacterial activity. Herein, the high antibacterial activity was achieved by introducing trace Mn³⁺ and H vacancy Image ID:d1tb00098e-t1.gif

couples in HA through a facile heat-treatment strategy in air. The theoretical results indicated that Mn³⁺ was preferentially substituted for the Ca(2) site in the HA structure with a charge-compensating H vacancy appearing at the adjacent OH⁻ site. The antibacterial tests showed that Mn-HA possessed antibacterial activity towards both E. coli and S. aureus with trace Mn content at the ppm level, and implied that Mn³⁺ and Image ID:d1tb00098e-t2.gif

centers may play an important role in the antibacterial process. The Mn³⁺ and Image ID:d1tb00098e-t3.gif

couples in Mn-HA, serving as oxidative and reductive centers respectively, could then collectively participate in the CoQ/CoQH₂ redox cycling and synergistically facilitate the accumulation of CoQ˙⁻ and ROS radicals. This enhanced ROS production was the main factor to endow Mn-HA with efficient antibacterial activity. Moreover, the in vitro bioactivity assay showed that Mn-HA materials exhibited enhanced osteogenic activity and good biocompatibility. Therefore, this work not only provides a feasible method to control the oxidation state of Mn elements in HA, but also proposes a novel trace Mn³⁺-doped HA for potential applications in tissue engineering.

更新日期：2021-04-12

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