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Grafting Density Governs the Thermoresponsive Behavior of P(OEGMA-co-RMA) Statistical Copolymers.
ACS Macro Letters ( IF 5.1 ) Pub Date : 2020-07-27 , DOI: 10.1021/acsmacrolett.0c00461 Irem Akar 1 , Robert Keogh 1, 2 , Lewis D Blackman 2 , Jeffrey C Foster 1 , Robert T Mathers 3 , Rachel K O'Reilly 1
ACS Macro Letters ( IF 5.1 ) Pub Date : 2020-07-27 , DOI: 10.1021/acsmacrolett.0c00461 Irem Akar 1 , Robert Keogh 1, 2 , Lewis D Blackman 2 , Jeffrey C Foster 1 , Robert T Mathers 3 , Rachel K O'Reilly 1
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Thermoresponsive copolymers that exhibit a lower critical solution temperature (LCST) have been exploited to prepare stimuli-responsive materials for a broad range of applications. It is well understood that the LCST of such copolymers can be controlled by tuning molecular weight or through copolymerization of two known thermoresponsive monomers. However, no general methodology has been established to relate polymer properties to their temperature response in solution. Herein, 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 oligoethylene glycol monomethyl ether methacrylate (OEGMA) and hydrophobic alkyl methacrylate monomers and their hydrophobicity was compared using surface area-normalized partition coefficients (log Poct/SA). However, while some insight was gained by comparing TCP and hydrophobicity values, further statistical analysis on both experimental and literature data showed that the molar percentage of comonomer (i.e., grafting density) was the strongest influencer of TCP, regardless of the comonomer used. The lack of dependence of TCP on comonomer chemistry implies that a broad range of functional, thermoresponsive materials can be prepared based on OEGMA by simply tuning grafting density.
中文翻译：
接枝密度控制 P(OEGMA-co-RMA) 统计共聚物的热响应行为。
具有较低临界溶解温度（LCST）的热响应共聚物已被用来制备具有广泛应用的刺激响应材料。众所周知，此类共聚物的LCST可以通过调节分子量或通过两种已知的热响应单体的共聚来控制。然而，尚未建立将聚合物特性与其在溶液中的温度响应联系起来的通用方法。在此，我们试图建立聚合物疏水性和浊点温度（ T CP ）之间的预测关系。基于亲水性低聚乙二醇单甲醚甲基丙烯酸酯（OEGMA）和疏水性甲基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分配系数（log P oct /SA）比较了它们的疏水性。然而，虽然通过比较T CP和疏水性值获得了一些见解，但对实验和文献数据的进一步统计分析表明，共聚单体的摩尔百分比（即接枝密度）是T CP的最强影响因素，无论使用何种共聚单体。 T CP对共聚单体化学的依赖性意味着，通过简单地调节接枝密度，可以基于 OEGMA 制备各种功能性热响应材料。
更新日期：2020-08-18
中文翻译：
接枝密度控制 P(OEGMA-co-RMA) 统计共聚物的热响应行为。
具有较低临界溶解温度（LCST）的热响应共聚物已被用来制备具有广泛应用的刺激响应材料。众所周知，此类共聚物的LCST可以通过调节分子量或通过两种已知的热响应单体的共聚来控制。然而，尚未建立将聚合物特性与其在溶液中的温度响应联系起来的通用方法。在此，我们试图建立聚合物疏水性和浊点温度（ T CP ）之间的预测关系。基于亲水性低聚乙二醇单甲醚甲基丙烯酸酯（OEGMA）和疏水性甲基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分配系数（log P oct /SA）比较了它们的疏水性。然而，虽然通过比较T CP和疏水性值获得了一些见解，但对实验和文献数据的进一步统计分析表明，共聚单体的摩尔百分比（即接枝密度）是T CP的最强影响因素，无论使用何种共聚单体。 T CP对共聚单体化学的依赖性意味着，通过简单地调节接枝密度，可以基于 OEGMA 制备各种功能性热响应材料。
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