Gaining Structural Control by Modification of Polymerization Rate in Ring-Opening Polymerization-Induced Crystallization-Driven Self-Assembly

IF 4.7 Q1 POLYMER SCIENCE ACS polymers Au Pub Date : 2022-08-26 DOI:10.1021/acspolymersau.2c00027
Paul Joshua Hurst, Annissa A. Graham and Joseph P. Patterson*, 
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引用次数: 3

Abstract

Polymerization-induced self-assembly (PISA) has become an important one pot method for the preparation of well-defined block copolymer nanoparticles. In PISA, morphology is typically controlled by changing molecular architecture and polymer concentration. However, several computational and experimental studies have suggested that changes in polymerization rate can lead to morphological differences. Here, we demonstrate that catalyst selection can be used to control morphology independent of polymer structure and concentration in ring-opening polymerization-induced crystallization-driven self-assembly (ROPI-CDSA). Slower rates of polymerization give rise to slower rates of self-assembly, resulting in denser lamellae and more 3D structures when compared to faster rates of polymerization. Our explanation for this is that the fast samples transiently exist in a nonequilibrium state as self-assembly starts at a higher solvophobic block length when compared to the slow polymerization. We expect that subsequent examples of rate variation in PISA will allow for greater control over morphological outcome.

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通过改变开环聚合诱导结晶驱动自组装的聚合速率获得结构控制
聚合诱导自组装(PISA)已成为制备具有良好定义的嵌段共聚物纳米颗粒的一种重要方法。在PISA中,形态通常通过改变分子结构和聚合物浓度来控制。然而,一些计算和实验研究表明,聚合速率的变化可以导致形态差异。在这里,我们证明了催化剂的选择可以用来控制开环聚合诱导结晶驱动自组装(ROPI-CDSA)的形态,而不依赖于聚合物的结构和浓度。较慢的聚合速度导致较慢的自组装速度,与较快的聚合速度相比,导致更密集的片层和更多的3D结构。我们对此的解释是,与缓慢聚合相比,快速样品在自组装开始时具有更高的疏溶剂嵌段长度,因此瞬态存在于非平衡状态。我们期望PISA中随后的速率变化示例将允许对形态学结果进行更大的控制。
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