Metal-Organic Framework/Chitosan Hybrid Materials Promote Nitric Oxide Release from S-Nitrosoglutathione in Aqueous Solution.
Metal-Organic Framework/Chitosan Hybrid Materials Promote Nitric Oxide Release from S-Nitrosoglutathione in Aqueous Solution.
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DOI：
10.1021/acsami.6b14937
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发表时间：
2017-02-15
影响因子：
9.5
通讯作者：
Reynolds MM
中科院分区：
文献类型：
--
作者：
Neufeld MJ;Lutzke A;Tapia JB;Reynolds MM
已有研究表明，铜基金属−有机骨架(MOF)可促进S亚硝硫醇(RSNO)生成治疗活性分子一氧化氮(NO)。由于RSNO天然存在于血液中，这一功能被假设为允许通过使用基于MOF的血液接触材料来控制NO的产生。在这种应用中，MOF的实际实施通常需要结合在聚合物载体中，然而这种固定化已经被证明削弱了MOF与形成NO的RSNO底物相互作用的能力。将水稳定的铜基MOF H3[(Cu4Cl)3-(BTTri)8](H3BTTri=1，3，5-三(1H-1，2，3-三唑-5-基)苯)，或铜-BTTri，加入到天然衍生的多糖壳聚糖中，形成膜，评价其促进天然多糖壳聚糖生成NO的能力。这是第一个评估MOF诱导GSNO释放NO的报告，GSNO是含量最丰富的小分子RSNO。在初始浓度为20μM(pH 7.4的磷酸盐缓冲液，37℃)下，壳聚糖/铜BTTri膜在约4 h内释放出97±3%的理论NO，相当于GSnO基线热分解的65倍。此外，与以前使用疏水性聚氨酯或聚氯乙烯不同，在亲水性壳聚糖中掺入铜-BTTri不会损害MOF的活性。在随后的实验中，膜的重复使用继续提高了GSNO的产量，这表明了继续使用的潜力。此外，通过质谱分析，确定了铜-BTTri促进GSNO分解的主要有机产物为氧化谷胱甘肽，证实了先前的假设。X射线粉末衍射结构分析和电感耦合等离子体原子发射光谱分析表明，在GSNO作用下，Cu-BTTri保持了结晶度，没有明显的降解。综上所述，这些发现为聚合物/铜-BTTri体系的功能和用途提供了洞察，并可能支持未来基于MOF的生物材料的发展。
It has been previously demonstrated that copper-based metal−organic 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 H3[(Cu4Cl)3-(BTTri)8] (H3BTTri = 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 μM initial GSNO concentration (pH 7.4 phosphate buffered saline, 37 °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.
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影响因子：
14
作者：
Lu, Yuan;Slomberg, Danielle L.;Schoenfisch, Mark H.
通讯作者：
Schoenfisch, Mark H.
一氧化氮产生聚合物的血流相容性，该聚合物在体外循环模型中催化S-硝基硫醇分解。
影响因子：
14
作者：
Major, Terry C.;Brant, David O.;Burney, Charles P.;Amoako, Kagya A.;Annich, Gail M.;Meyerhoff, Mark E.;Handa, Hitesh;Bartlett, Robert H.
通讯作者：
Bartlett, Robert H.
影响因子：
19
作者：
Harding, Jacqueline L.;Metz, Jarid M.;Reynolds, Melissa M.
通讯作者：
Reynolds, Melissa M.
影响因子：
5.7
作者：
Dai T;Tanaka M;Huang YY;Hamblin MR
通讯作者：
Hamblin MR
DOI：
10.1039/p29960000481
发表时间：
1996-04-01
期刊：
JOURNAL OF THE CHEMICAL SOCIETY-PERKIN TRANSACTIONS 2
影响因子：
--
作者：
Dicks, AP;Swift, HR;Cox, BG
通讯作者：
Cox, BG