Manganoporphyrin-Polyphenol Multilayer Capsules as Radical and Reactive Oxygen Species (ROS) Scavengers,Chemistry of Materials

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Manganoporphyrin-Polyphenol Multilayer Capsules as Radical and Reactive Oxygen Species (ROS) Scavengers
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-01-03 00:00:00 , DOI: 10.1021/acs.chemmater.7b03502
Aaron Alford ₁ , Veronika Kozlovskaya ₁ , Bing Xue ₁ , Nirzari Gupta ₁ , William Higgins ₁ , Dana Pham-Hua ₂ , Lilin He ₃ , Volker S. Urban ₃ , Hubert M. Tse ₂ , Eugenia Kharlampieva ₁

Affiliation

Local modulation of oxidative stress is crucial for a variety of biochemical events including cellular differentiation, apoptosis, and defense against pathogens. Currently employed natural and synthetic antioxidants exhibit a lack of biocompatibility, bioavailability, and chemical stability, resulting in limited capability to scavenge reactive oxygen species (ROS). To mediate these drawbacks, we have developed a synergistic manganoporphyrin-polyphenol polymeric nanothin coating and hollow microcapsules with efficient antioxidant activity and controllable ROS modulation. These materials are produced by multilayer assembly of a natural polyphenolic antioxidant, tannic acid (TA), with a synthesized copolymer of polyvinylpyrrolidone containing a manganoporphyrin modality (MnP-PVPON) which mimics the enzymatic antioxidant superoxide dismutase. The redox activity of the copolymer is demonstrated to dramatically increase the antioxidant response of MnP-PVPON/TA capsules versus unmodified PVPON/TA capsules through reduction of a radical cationic dye and to significantly suppress the proliferation of superoxide via cytochrome C competition. Inclusion of MnP-PVPON as an outer layer enhances radical-scavenging activity as compared to localization of the layer in the middle or inner part of the capsule shell. In addition, we demonstrate that TA is crucial for the synergistic radical-scavenging activity of the MnP-PVPON/TA system which exhibits a combined superoxide dismutase-like ability and catalase-like activity in response to the free radical superoxide challenge. The MnP-PVPON/TA capsules exhibit a negligible, 8% loss of shell thickness upon free radical treatment, while PVPON/TA capsules lose 39% of their shell thickness due to the noncatalytic free-radical-scavenging of TA, as demonstrated by small angle neutron scattering (SANS). Finally, we have found the manganoporphyrin-polyphenol capsules to be nontoxic to splenocytes from NOD mice after 48 h incubation. Our study illustrates the strong potential of combining catalytic activity of manganoporphyrins with natural polyphenolic antioxidants to design efficient free-radical-scavenging materials that may eventually be used in antioxidant therapies and as free radical dissipating protective carriers of biomolecules for biomedical or industrial applications.

中文翻译：

锰卟啉-多酚多层胶囊作为自由基和活性氧（ROS）的清除剂

氧化应激的局部调节对于多种生化事件至关重要，包括细胞分化，凋亡和对病原体的防御。当前使用的天然和合成抗氧化剂表现出缺乏生物相容性，生物利用度和化学稳定性，导致清除活性氧（ROS）的能力有限。为了介导这些缺点，我们开发了具有协同作用的锰卟啉-多酚聚合物纳米薄涂层和具有有效抗氧化剂活性和可控ROS调节的中空微胶囊。这些材料是通过将天然多酚抗氧化剂鞣酸（TA）与包含模拟卟啉抗氧化剂超氧化物歧化酶的锰卟啉模态（MnP-PVPON）的聚乙烯吡咯烷酮的合成共聚物进行多层组装而生产的。与未改性的PVPON / TA胶囊相比，该共聚物的氧化还原活性通过减少自由基阳离子染料而显着提高了MnP-PVPON / TA胶囊的抗氧化反应，并通过细胞色素C竞争显着抑制了超氧化物的增殖。与该层在胶囊壳的中部或内部的定位相比，包含MnP-PVPON作为外层可增强自由基清除活性。此外，我们证明TA对于MnP-PVPON / TA系统的协同自由基清除活性至关重要，该体系在响应自由基超氧化物的反应中表现出组合的超氧化物歧化酶样能力和过氧化氢酶样活性。MnP-PVPON / TA胶囊在自由基处理后的壳厚损失可忽略不计，为8％，小角度中子散射（SANS）表明，由于TA的非催化自由基清除作用，PVPON / TA胶囊损失了39％的壳厚度。最后，我们发现锰卟啉-多酚胶囊对48小时孵育后的NOD小鼠脾细胞无毒。我们的研究表明，锰卟啉与天然多酚类抗氧化剂结合起来具有强大的潜力，可以设计出有效的自由基清除材料，这些材料最终可用于抗氧化剂治疗，并作为消散自由基的生物分子保护载体，用于生物医学或工业应用。我们发现锰卟啉-多酚胶囊对48小时孵育后的NOD小鼠脾细胞无毒。我们的研究表明，锰卟啉与天然多酚类抗氧化剂结合起来具有强大的潜力，可以设计出有效的自由基清除材料，这些材料最终可用于抗氧化剂治疗，并作为消散自由基的生物分子保护载体，用于生物医学或工业应用。我们发现，锰卟啉-多酚胶囊对48小时孵育后的NOD小鼠脾细胞无毒。我们的研究表明，锰卟啉与天然多酚类抗氧化剂结合起来具有强大的潜力，可以设计出有效的自由基清除材料，这些材料最终可用于抗氧化剂治疗，并作为消散自由基的生物分子保护载体，用于生物医学或工业应用。

更新日期：2018-01-03

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