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首页> 外文期刊>ACS applied materials & interfaces >Metal-Organic Framework/Chitosan Hybrid Materials Promote Nitric Oxide Release from S-Nitrosoglutathione in Aqueous Solution
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Metal-Organic Framework/Chitosan Hybrid Materials Promote Nitric Oxide Release from S-Nitrosoglutathione in Aqueous Solution

机译：金属有机框架/壳聚糖杂交材料从水溶液中促进S-Nitrosogluthathione的一氧化氮释放

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It has been previously demonstrated that copper-based metalorganic frameworks (MOFs) accelerate formation of the therapeutically active molecule nitric oxide (NO) from S-nitrosothiols (RSNOs). Because RSNOs are naturally present in blood, this function is hypothesized to permit the controlled production of NO through use of MOF-based blood-contacting materials. The practical implementation of MOFs in this application typically requires incorporation within a polymer support, yet this immobilization has been shown to impair the ability of the MOF to interact with the NO-forming RSNO substrate. Here, the water-stable, copper-based MOF H-3[(Cu4Cl)(3)-(BTTri)(8)] (H(3)BTTri = 1,3,5-tris(1H- 1,2,3-triazol-5-yl)benzene), or Cu-BTTri, was incorporated within the naturally derived polysaccharide chitosan to form membranes that were evaluated for their ability to enhance NO generation from the RSNO S-nitrosoglutathione (GSNO). This is the first report to evaluate MOF-induced NO release from GSNO, the most abundant small-molecule RSNO. At a 20 mu M initial GSNO concentration (pH 7.4 phosphate buffered saline, 37 degrees C), chitosan/Cu-BTTri membranes induced the release of 97 +/- 3% of theoretical NO within approximately 4 h, corresponding to a 65-fold increase over the baseline thermal decomposition of GSNO. Furthermore, incorporation of Cu-BTTri within hydrophilic chitosan did not impair the activity of the MOF, unlike earlier efforts using hydrophobic polyurethane or poly(vinyl chloride). The reuse of the membranes continued to enhance NO production from GSNO in subsequent experiments, suggesting the potential for continued use. Additionally, the major organic product of Cu-BTTri-promoted GSNO decomposition was identified as oxidized glutathione via mass spectrometry, confirming prior hypotheses. Structural analysis by pXRD and assessment of copper leaching by ICP-AES indicated that Cu-BTTri retains crystallinity and exhibits no significant degradation following exposure to GSNO. Taken together, these findings provide insight into the function and utility of polymer/Cu-BTTri systems and may support the development of future MOF-based biomaterials.
机译：先前已经证明，基于铜的金属有机框架（MOF）从S-亚硝基硫醇（RSNOS）加速形成治疗活性分子一氧化物（NO）。由于RSNOS自然存在于血液中，因此假设该功能以允许通过使用基于MOF的血液接触材料进行控制的产生。本申请中的MOF的实际实施通常需要在聚合物载体内掺入，但已经显示该固定化损害MOF与无成形RSNO基材相互作用的能力。这里，水稳态，铜基MOF H-3 [（CU 4 Cl）（3） - （BTTRI）（8）]（H（3）BTTRI = 1,3,5-三（1H- 1,2， 3-三唑-5-基）苯）或Cu-BTTRI纳入天然衍生的多糖壳聚糖，形成膜，以评价它们从rsno s-antosoglutathione（Gsno）的不产生产生的能力。这是第一个评估MOF诱导的报告诱导的GSNO释放，这是最丰富的小分子RSNO。在20μm初始GSNO浓度（pH 7.4磷酸盐缓冲盐水，37℃）中，壳聚糖/ Cu-BTTRI膜诱导释放97 +/- 3％的理论不在约4小时内，对应于65倍增加GSNO的基线热分解。此外，与使用疏水性聚氨酯或聚（氯乙烯）的早期努力不同，掺入亲水性壳聚糖内的Cu-Bttri并未损害MOF的活性。膜的再利用继续增强从后续实验中的GSNO生产，表明继续使用的可能性。另外，通过质谱法将Cu-BTTRI促进的GSNO分解的主要有机产物鉴定为氧化谷胱甘肽，确认先前假设。通过PXRD的结构分析和ICP-AES的铜浸出评估表明Cu-BTTRI保持结晶度，并且在暴露于GSNO后没有显着降解。这些发现结合在一起，可以深入了解聚合物/ Cu-BTTRI系统的功能和效用，并可以支持未来基于MOF的生物材料的发展。

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