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Tuning the thermoresponsive properties of PEG-based fluorinated polymers and stimuli responsive drug release for switchable 19F magnetic resonance imaging
Polymer Chemistry ( IF 4.1 ) Pub Date : 2021-09-08 , DOI: 10.1039/d1py00602a Adil Usman 1, 2 , Cheng Zhang 1, 2 , Jiacheng Zhao 1, 2 , Hui Peng 1, 2 , Nyoman D. Kurniawan 3 , Changkui Fu 1, 2 , David J. T. Hill 1, 4 , Andrew K. Whittaker 1, 2
Polymer Chemistry ( IF 4.1 ) Pub Date : 2021-09-08 , DOI: 10.1039/d1py00602a Adil Usman 1, 2 , Cheng Zhang 1, 2 , Jiacheng Zhao 1, 2 , Hui Peng 1, 2 , Nyoman D. Kurniawan 3 , Changkui Fu 1, 2 , David J. T. Hill 1, 4 , Andrew K. Whittaker 1, 2
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A series of terpolymers of styrene, oligoethylene glycol methyl ether methacrylate and 2,2,2-trifluoroethyl acrylate were synthesized by free radical polymerization. The lower critical solution temperature (LCST) of the polymers was tuned to close to physiological temperature by controlling the hydrophobic (styrene) content. The thermoresponsive properties of the polymers were studied by nuclear magnetic resonance spectroscopy, UV-vis spectroscopy and dynamic light scattering experiments. The effect of styrene content on 1H and 19F NMR, 19F T2 relaxation times and 19F magnetic resonance imaging (MRI) was examined in detail at various temperatures. It was observed that above the LCST the 19F MR imaging intensity drops, as a consequence of enhanced dipolar interactions involving 19F spins. These results aided the design of a thermo- and pH-responsive 19F MRI agent by incorporation of a hydrophobic model drug via an acid cleavable hydrazone linkage. It was demonstrated that with the release of the model hydrophobic drug, the LCST of the polymer was elevated due to reduced hydrophobicity, enhancing the 19F MRI signal at the given measurement temperature. The results provide the basis for the development of switchable 19F MR-guided theranostic platforms for targeted drug delivery of hydrophobic chemotherapeutic drugs as well as quantifying the amount of drug released at the target site.
中文翻译：
调整基于 PEG 的氟化聚合物的热响应特性和用于可切换 19F 磁共振成像的刺激响应药物释放
通过自由基聚合合成了一系列苯乙烯、低聚乙二醇甲基醚甲基丙烯酸酯和2,2,2-三氟乙基丙烯酸酯的三元共聚物。通过控制疏水性（苯乙烯）含量，将聚合物的下临界溶解温度 (LCST) 调整到接近生理温度。通过核磁共振光谱、紫外-可见光谱和动态光散射实验研究了聚合物的热响应特性。在不同温度下详细检查了苯乙烯含量对1 H 和19 F NMR、19 F T 2弛豫时间和19 F 磁共振成像 (MRI) 的影响。据观察，在 LCST 以上由于涉及19 F 自旋的偶极相互作用增强， 19 F MR 成像强度下降。这些结果有助于通过酸可裂解腙键结合疏水模型药物来设计热响应和 pH 响应19 F MRI 试剂。结果表明，随着模型疏水性药物的释放，聚合物的 LCST 由于疏水性降低而升高，从而增强了给定测量温度下的19 F MRI 信号。研究结果为switchable 19的开发提供了依据F MR 引导的治疗诊断平台，用于疏水性化疗药物的靶向药物递送以及量化靶位点释放的药物量。
更新日期：2021-09-10
中文翻译：
调整基于 PEG 的氟化聚合物的热响应特性和用于可切换 19F 磁共振成像的刺激响应药物释放
通过自由基聚合合成了一系列苯乙烯、低聚乙二醇甲基醚甲基丙烯酸酯和2,2,2-三氟乙基丙烯酸酯的三元共聚物。通过控制疏水性（苯乙烯）含量，将聚合物的下临界溶解温度 (LCST) 调整到接近生理温度。通过核磁共振光谱、紫外-可见光谱和动态光散射实验研究了聚合物的热响应特性。在不同温度下详细检查了苯乙烯含量对1 H 和19 F NMR、19 F T 2弛豫时间和19 F 磁共振成像 (MRI) 的影响。据观察，在 LCST 以上由于涉及19 F 自旋的偶极相互作用增强， 19 F MR 成像强度下降。这些结果有助于通过酸可裂解腙键结合疏水模型药物来设计热响应和 pH 响应19 F MRI 试剂。结果表明，随着模型疏水性药物的释放，聚合物的 LCST 由于疏水性降低而升高，从而增强了给定测量温度下的19 F MRI 信号。研究结果为switchable 19的开发提供了依据F MR 引导的治疗诊断平台，用于疏水性化疗药物的靶向药物递送以及量化靶位点释放的药物量。
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