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Log Poct/SA Predicts the Thermoresponsive Behavior of P(DMA-co-RA) Statistical Copolymers
ACS Macro Letters ( IF 5.8 ) Pub Date : 2022-03-22 , DOI: 10.1021/acsmacrolett.1c00776
Irem Akar 1 , Jeffrey C Foster 1 , Xiyue Leng 1 , Amanda K Pearce 1 , Robert T Mathers 2 , Rachel K O'Reilly 1
Affiliation  

Polymers that exhibit a lower critical solution temperature (LCST) have been of great interest for various biological applications such as drug or gene delivery, controlled release systems, and biosensing. Tuning the LCST behavior through control over polymer composition (e.g., upon copolymerization of monomers with different hydrophobicity) is a widely used method, as the phase transition is greatly affected by the hydrophilic/hydrophobic balance of the copolymers. However, the lack of a general method that relates copolymer hydrophobicity to their temperature response leads to exhaustive experiments when seeking to obtain polymers with desired properties. This is particularly challenging when the target copolymers are comprised of monomers that individually form nonresponsive homopolymers, that is, only when copolymerized do they display thermoresponsive behavior. In this study, we sought to develop a predictive relationship between polymer hydrophobicity and cloud point temperature (TCP). A series of statistical copolymers were synthesized based on hydrophilic N,N-dimethyl acrylamide (DMA) and hydrophobic alkyl acrylate monomers, and their hydrophobicity was compared using surface area-normalized octanol/water partition coefficients (Log Poct/SA). Interestingly, a correlation between the Log Poct/SA of the copolymers and their TCPs was observed for the P(DMA-co-RA) copolymers, which allowed TCP prediction of a demonstrative copolymer P(DMA-co-MMA). These results highlight the strong potential of this computational tool to improve the rational design of copolymers with desired temperature responses prior to synthesis.

中文翻译:

Log Poct/SA 预测 P(DMA-co-RA) 统计共聚物的热响应行为

具有较低临界溶解温度 (LCST) 的聚合物在药物或基因递送、控释系统和生物传感等各种生物应用中引起了极大的兴趣。通过控制聚合物组成(例如,在具有不同疏水性的单体共聚时)来调整 LCST 行为是一种广泛使用的方法,因为相变受共聚物的亲水/疏水平衡影响很大。然而,在寻求获得具有所需性能的聚合物时,缺乏将共聚物疏水性与其温度响应相关联的通用方法导致进行详尽的实验。当目标共聚物由单独形成无响应均聚物的单体组成时,这尤其具有挑战性,即 只有在共聚时,它们才会显示出热响应行为。在这项研究中,我们试图建立聚合物疏水性和浊点温度之间的预测关系(CP )。基于亲水性NN-二甲基丙烯酰胺(DMA)和疏水性丙烯酸烷基酯单体合成了一系列统计共聚物,并使用表面积归一化辛醇/水分配系数(Log P oct /SA)比较了它们的疏水性。有趣的是,对于 P(DMA-co-RA) 共聚物,观察到共聚物的 Log P oct /SA 与其 T CP 之间的相关性使得T CP可以预测示范共聚物P(DMA- co-MMA)。这些结果突出了这种计算工具在改进合成前具有所需温度响应的共聚物的合理设计方面的巨大潜力。
更新日期:2022-03-22
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