Structurally Diverse Nitric Oxide-Releasing Poly(propylene Imine) Dendrimers.

Structurally Diverse Nitric Oxide-Releasing Poly(propylene Imine) Dendrimers.
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DOI:
10.1021/cm201628z
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发表时间:
2011-09-27
期刊:
Chemistry of materials : a publication of the American Chemical Society
影响因子:
--
通讯作者:
Schoenfisch MH
Schoenfisch MH
中科院分区:
其他
文献类型:
--
作者:
Lu Y;Sun B;Li C;Schoenfisch MH

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以环氧丙烷(PO)、氧化苯乙烯(SO)、丙烯腈(ACN)、聚乙二醇甲基丙烯酸酯(平均Mn = 480) (PEG)或1,2-环氧-9-癸烯(ED)为原料,采用开环或共轭加成反应,一步合成了结构各异的二胺官能化聚丙烯亚胺(PPI)树状大分子。在碱性溶液中,与NO气体反应生成了二氮二醇型n -二氮二醇型一氧化氮供体。所制备的树突状支架的NO储存和释放动力学具有差异(总NO量为0.9 ~ 3.8 μmol /mg,半衰期为0.3 ~ 4.9 h),说明外部化学修饰(如空间环境、疏水性等)对重氮二酸酯稳定性/分解的重要性。通过在一个大分子支架的外部结合两个供体系统,证明了可调节的NO释放。此外,研究人员还建立了一个数学模型,利用两种单一一氧化氮供体系统的一氧化氮释放数据,模拟了双重一氧化氮释放动力学。本文描述的方法通过解锁一系列材料,根据外部修饰,作为生物医学聚合物或独立疗法的掺杂剂,扩展了no释放大分子支架的范围和范围。
Structurally diverse secondary amine-functionalized poly(propylene imine) (PPI) dendrimers capable of tunable nitric oxide (NO) release were synthesized in a straightforward, one-step manner using ring-opening or conjugate-addition reactions with propylene oxide (PO), styrene oxide (SO), acrylonitrile (ACN), poly(ethylene glycol) methyl ether acrylate (average Mn = 480) (PEG) or 1,2-epoxy-9-decene (ED). N-Diazeniumdiolate nitric oxide donors were formed on the resulting secondary amine-functionalized G2–G5 PPI dendrimers by reaction with NO gas in basic solution. The NO storage and release kinetics for the resulting dendritic scaffolds were diverse (0.9–3.8 μmol NO/mg totals and 0.3 to 4.9 h half lives), illustrating the importance of the exterior chemical modification (e.g., steric environments, hydrophobicity, etc.) on diazeniumdiolate stability/decomposition. Tunable NO release was demonstrated by combining two donor systems on the exterior of one macromolecular scaffold. Additionally, a mathematical model was developed that allows for the simulation of dual NO release kinetics using the NO release data from the two single NO donor systems. The approaches described herein extend the range and scope of NO-releasing macromolecular scaffolds by unlocking a series of materials for use as dopants in biomedical polymers or stand-alone therapeutics depending on the exterior modification.
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