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Self-Assembly of Amphiphilic Copolymers with Sequence-Controlled Alternating Hydrophilic–Hydrophobic Pendant Side Chains
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-03-27 , DOI: 10.1021/acsapm.0c00204 Krishna Gopal Goswami 1 , Sourav Mete 1 , Sutapa Som Chaudhury 2 , Pintu Sar 1 , Evgenii Ksendzov 3 , Chitrangada Das Mukhopadhyay 2 , Sergei V. Kostjuk 3, 4, 5 , Priyadarsi De 1
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-03-27 , DOI: 10.1021/acsapm.0c00204 Krishna Gopal Goswami 1 , Sourav Mete 1 , Sutapa Som Chaudhury 2 , Pintu Sar 1 , Evgenii Ksendzov 3 , Chitrangada Das Mukhopadhyay 2 , Sergei V. Kostjuk 3, 4, 5 , Priyadarsi De 1
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To design versatile ordered nanomorphologies from the alternating sequence-controlled amphiphilic copolymers, in the current work, we have investigated the self-assembly behavior of a series of alternating copolymers, prepared through the reversible addition–fragmentation chain transfer (RAFT) polymerization of methoxy poly(ethylene glycol) (mPEG) functionalized styrene (VBP) and fatty acid attached maleimide (MF) monomers. The copolymers efficiently induced self-aggregation of the pendant side chains to afford both micelle and vesicle nanostructures in aqueous medium depending on the amphiphilicity of the side chains, as evident from dynamic light scattering (DLS) and transmission electron microscopy (TEM) analysis. The copolymers also induced thermoresponsive phase transition in water with lower critical solution temperatures (LCST) in the range of 69–88 °C depending on the mPEG side chain lengths, as determined from UV–vis spectroscopy. The hydrophobic dye and hydrophilic drug loading abilities of the synthesized copolymers were investigated using nile red and doxorubicin hydrochloride (DOX·HCl) as model compounds, respectively. The copolymers further formed reverse micelles in hexane owing to the presence of hydrophobic fatty acid pendants in the side chains, for which hexane is a good solvent. Additionally, the in vitro cytotoxicity study was performed for the synthesized alternating copolymers which revealed their nontoxic nature up to 500 μg/mL polymer concentration. Thus, the current work represents a fundamental strategy to construct biocompatible polymeric nanostructures from amphiphilic alternating copolymers, endowing noteworthy features for potential advantages.
中文翻译：
具有序列控制的交替亲水-疏水侧链侧链的两亲共聚物的自组装
为了从交替序列控制的两亲共聚物设计通用的有序纳米形态，在当前工作中，我们研究了通过可逆的加成-断裂链转移（RAFT）聚合甲氧基多聚体制备的一系列交替共聚物的自组装行为。 （乙二醇）（mPEG）官能化苯乙烯（VBP）和脂肪酸连接的马来酰亚胺（MF）单体。该共聚物有效地引起侧链侧链的自聚集，从而根据侧链的两亲性在水性介质中同时提供胶束和囊泡纳米结构，这可从动态光散射（DLS）和透射电子显微镜（TEM）分析中看出。共聚物还可以在水中以较低的临界溶液温度（LCST）在69-88°C的范围内引起热响应相变，这取决于mPEG侧链的长度，这是通过紫外可见光谱确定的。以尼罗红和盐酸阿霉素（DOX·HCl）为模型化合物分别研究了合成共聚物的疏水染料和亲水药物负载能力。由于在侧链中存在疏水性脂肪酸侧基，该共聚物在己烷中进一步形成了反胶束，而己烷是良好的溶剂。此外，对合成的交替共聚物进行了体外细胞毒性研究，结果表明，当聚合物浓度达到500μg/ mL时，它们的无毒性质。因此，当前的工作代表了一种由两亲性交替共聚物构建生物相容性聚合物纳米结构的基本策略，具有明显的潜在优势。
更新日期：2020-03-27
中文翻译：
具有序列控制的交替亲水-疏水侧链侧链的两亲共聚物的自组装
为了从交替序列控制的两亲共聚物设计通用的有序纳米形态，在当前工作中，我们研究了通过可逆的加成-断裂链转移（RAFT）聚合甲氧基多聚体制备的一系列交替共聚物的自组装行为。 （乙二醇）（mPEG）官能化苯乙烯（VBP）和脂肪酸连接的马来酰亚胺（MF）单体。该共聚物有效地引起侧链侧链的自聚集，从而根据侧链的两亲性在水性介质中同时提供胶束和囊泡纳米结构，这可从动态光散射（DLS）和透射电子显微镜（TEM）分析中看出。共聚物还可以在水中以较低的临界溶液温度（LCST）在69-88°C的范围内引起热响应相变，这取决于mPEG侧链的长度，这是通过紫外可见光谱确定的。以尼罗红和盐酸阿霉素（DOX·HCl）为模型化合物分别研究了合成共聚物的疏水染料和亲水药物负载能力。由于在侧链中存在疏水性脂肪酸侧基，该共聚物在己烷中进一步形成了反胶束，而己烷是良好的溶剂。此外，对合成的交替共聚物进行了体外细胞毒性研究，结果表明，当聚合物浓度达到500μg/ mL时，它们的无毒性质。因此，当前的工作代表了一种由两亲性交替共聚物构建生物相容性聚合物纳米结构的基本策略，具有明显的潜在优势。
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