Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers,ACS Macro Letters

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Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers
ACS Macro Letters ( IF 5.1 ) Pub Date : 2019-11-01 , DOI: 10.1021/acsmacrolett.9b00721
Shifeng Nian , Huada Lian ₁ , Zihao Gong , Mikhail Zhernenkov ₂ , Jian Qin ₁ , Li-Heng Cai

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Linear–bottlebrush–linear (LBBL) triblock copolymers represent an emerging system for creating multifunctional nanostructures. Their self-assembly depends on molecular architecture but remains poorly explored. We synthesize polystyrene-block-bottlebrush polydimethylsiloxane-block-polystyrene triblock copolymers with controlled molecular architecture and use them as a model system to study the self-assembly of LBBL polymers. Unlike classical stiff rod-flexible linear block copolymers that are prone to form highly ordered nanostructures such as lamellae, at small weight fractions of the linear blocks, LBBL polymers self-assemble to a disordered sphere phase, regardless of the bottlebrush stiffness. Microscopically, characteristic lengths increase with the bottlebrush stiffness by a power of 2/3, which is captured by a scaling analysis. Macroscopically, the formed nanostructures are ultrasoft, reprocessable elastomers with shear moduli of about 1 kPa, two orders of magnitude lower than that of conventional polydimethylsiloxane elastomers. Our results provide insights on exploiting the self-assembly of LBBL polymers to create soft functional nanostructures.

中文翻译：

分子结构指导线性-瓶刷-线性三嵌段共聚物自组装成柔软的可再加工弹性体

线性-刷子-线性 (LBBL) 三嵌段共聚物代表了一种用于创建多功能纳米结构的新兴系统。它们的自组装取决于分子结构，但仍缺乏探索。我们合成聚苯乙烯-嵌段-刷子聚二甲基硅氧烷-嵌段-具有受控分子结构的聚苯乙烯三嵌段共聚物，并将其用作模型系统来研究 LBBL 聚合物的自组装。与易于形成高度有序的纳米结构（如薄片）的经典刚性棒-柔性线性嵌段共聚物不同，LBBL 聚合物在线性嵌段的重量分数较小时，会自组装成无序的球形相，而不管刷子的刚度如何。在显微镜下，特征长度随瓶刷刚度增加 2/3 的幂，这是通过缩放分析捕获的。从宏观上看，形成的纳米结构是超软、可再加工的弹性体，剪切模量约为 1 kPa，比传统的聚二甲基硅氧烷弹性体低两个数量级。

更新日期：2019-11-01

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