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Role of Solvophobic Sequences in Amphiphilic Hyperbranched Polymers during Self-Assembly and Photoresponsiveness
Macromolecules ( IF 5.1 ) Pub Date : 2024-08-28 , DOI: 10.1021/acs.macromol.4c01851 Ankita Kumari 1 , Raj Kumar Roy 1
Macromolecules ( IF 5.1 ) Pub Date : 2024-08-28 , DOI: 10.1021/acs.macromol.4c01851 Ankita Kumari 1 , Raj Kumar Roy 1
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Self-assembly of amphiphilic molecules is a simple and effective method for creating various nanoscale shapes such as spheres, rods, cylinders, and vesicles. The arrangement of amphiphilic molecules during self-assembly is influenced by various factors. These factors include the balance between hydrophobic and hydrophilic components, length of solvophobic segments, amphiphile structure, temperature, and concentration. This study explores how the sequence of grafted solvophobic segments influences the self-assembled morphology and stimuli-responsive behavior. Herein, the desired amphiphiles were prepared by reacting the peripheral alkyne-terminated hyperbranched polyester core with two distinct azide-functionalized amphiphiles using Cu-catalyzed click transformations. The solvophobic sequences of these two amphiphiles differed by azide functionality positioning. For the Set-1 amphiphile, the azide group presented at the hydrophilic chain ends, while for the Set-2 amphiphile, it was the opposite. Furthermore, the solvophobic segments of these two amphiphiles were connected via a photoresponsive azobenzene spacer. Despite the similar hydrophobic/hydrophilic balance, the self-assembly of these two HBP-amphiphiles exhibited disparities in morphologies and photoresponsive behavior. HBP-1 amphiphile (HBP-OEG-Azo-C12) is self-assembled into a vesicular structure, whereas the HBP-2 amphiphile (HBP-C12-Azo-OEG) is self-assembled into spherical micelles. The photoresponsiveness of these two amphiphiles was investigated by assessing the release of guest molecules. A photophysical study revealed that the vesicular morphology of HBP-1 exhibits controlled release of guest molecules, while self-assembled HBP-2 initiates burst releases. Spectroscopic and microscopic imaging techniques were employed to gain insight into the mechanism for these differences. The sequence of grafted solvophobic units appears to influence the geometry of the self-segregated segments and the stability of the self-assembled structure, resulting in different morphologies and responsive functions.
中文翻译：
两亲性超支化聚合物中疏溶剂序列在自组装和光响应过程中的作用
两亲性分子的自组装是一种简单而有效的方法，用于创建各种纳米级形状，例如球体、棒状、圆柱体和囊泡。自组装过程中两亲性分子的排列受到多种因素的影响。这些因素包括疏水性和亲水性组分之间的平衡、疏溶剂链段的长度、两亲结构、温度和浓度。本研究探讨了接枝疏溶剂片段的序列如何影响自组装形态和刺激响应行为。在此，通过使用铜催化的点击转化使外围的炔封端的超支化聚酯核与两种不同的叠氮官能化的两亲物反应来制备所需的两亲物。这两种两亲物的疏溶剂序列因叠氮化物官能团的定位而不同。对于Set-1两亲物，叠氮化物基团出现在亲水链末端，而对于Set-2两亲物，则相反。此外，这两种两亲物的疏溶剂链段通过光响应偶氮苯间隔基连接。尽管疏水/亲水平衡相似，但这两种 HBP 两亲物的自组装在形态和光响应行为方面表现出差异。 HBP-1 两亲物 (HBP-OEG-Azo-C12) 自组装成囊泡结构，而 HBP-2 两亲物 (HBP-C12-Azo-OEG) 自组装成球形胶束。通过评估客体分子的释放来研究这两种两亲物的光响应性。光物理研究表明，HBP-1 的囊泡形态表现出客体分子的受控释放，而自组装的 HBP-2 则引发爆发释放。 采用光谱和显微成像技术来深入了解这些差异的机制。接枝疏溶剂单元的序列似乎影响自分离链段的几何形状和自组装结构的稳定性，导致不同的形态和响应功能。
更新日期：2024-08-28
中文翻译：
两亲性超支化聚合物中疏溶剂序列在自组装和光响应过程中的作用
两亲性分子的自组装是一种简单而有效的方法，用于创建各种纳米级形状，例如球体、棒状、圆柱体和囊泡。自组装过程中两亲性分子的排列受到多种因素的影响。这些因素包括疏水性和亲水性组分之间的平衡、疏溶剂链段的长度、两亲结构、温度和浓度。本研究探讨了接枝疏溶剂片段的序列如何影响自组装形态和刺激响应行为。在此，通过使用铜催化的点击转化使外围的炔封端的超支化聚酯核与两种不同的叠氮官能化的两亲物反应来制备所需的两亲物。这两种两亲物的疏溶剂序列因叠氮化物官能团的定位而不同。对于Set-1两亲物，叠氮化物基团出现在亲水链末端，而对于Set-2两亲物，则相反。此外，这两种两亲物的疏溶剂链段通过光响应偶氮苯间隔基连接。尽管疏水/亲水平衡相似，但这两种 HBP 两亲物的自组装在形态和光响应行为方面表现出差异。 HBP-1 两亲物 (HBP-OEG-Azo-C12) 自组装成囊泡结构，而 HBP-2 两亲物 (HBP-C12-Azo-OEG) 自组装成球形胶束。通过评估客体分子的释放来研究这两种两亲物的光响应性。光物理研究表明，HBP-1 的囊泡形态表现出客体分子的受控释放，而自组装的 HBP-2 则引发爆发释放。 采用光谱和显微成像技术来深入了解这些差异的机制。接枝疏溶剂单元的序列似乎影响自分离链段的几何形状和自组装结构的稳定性，导致不同的形态和响应功能。
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