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Synthesis and Thermoresponsive Properties of Biocompatible and Biodegradable Triblock Copolymers Bearing Linear or Y‐Shaped OEG Pendants
Macromolecular Chemistry and Physics ( IF 2.5 ) Pub Date : 2019-12-18 , DOI: 10.1002/macp.201900421 Xiongliang He 1 , Xiaodan Wang 2 , Rongtao Zhou 2 , Hua Lu 3 , Shifang Luan 2 , Haoyu Tang 1, 4
Macromolecular Chemistry and Physics ( IF 2.5 ) Pub Date : 2019-12-18 , DOI: 10.1002/macp.201900421 Xiongliang He 1 , Xiaodan Wang 2 , Rongtao Zhou 2 , Hua Lu 3 , Shifang Luan 2 , Haoyu Tang 1, 4
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Biocompatible and biodegradable thermoresponsive polymers are of great interest in “smart” biomedical applications. Herein, triblock copolymers (6a and 6b) comprised of hydrophobic poly(propylene glycol) (PPG) and OEGylated polypeptides bearing Y‐shaped or linear pendants are prepared by ring‐opening polymerization of reactive N‐carboxyanhydride monomers and subsequent side chain modification of polypeptides. OEGylated triblock copolymer bearing Y‐shaped (6a) or linear pendants (6b) with similar main chain length and the same amount of oligo(ethylene glycol) (OEG) units are successfully prepared as verified by 1H NMR, FTIR, and GPC. CD analysis reveals that 6a with Y‐shaped OEG pendants shows thermal‐ or salt‐induced destabilization of α‐helical conformation in water. Both 6a and 6b show reversible lower critical solution temperature (LCST)‐type phase transitions in DI H2O or PBS. Incorporation of a PPG segment leads to a significant decrease of the LCST‐type cloud point temperature (Tcp). Consequently, 6a and 6b show Tcp to human body temperature at low polymer concentrations (≤0.5 mg mL−1 in PBS). Moreover, 6a and 6b show low in vitro cytotoxicity and biodegradability in the presence of proteinase K. The results indicate that the thermoresponsive properties of LCST‐type polymers can be readily tuned by constructing Y‐shaped pendants as well as incorporation of hydrophobic polymer building blocks.
中文翻译：
具有线性或Y型OEG吊坠的生物相容性和可生物降解的三嵌段共聚物的合成和热响应性能
生物相容性和可生物降解的热响应性聚合物在“智能”生物医学应用中备受关注。在此，三元共聚物（6a和6b）由疏水性聚丙二醇（PPG）和带有Y形或线性侧基的OEG酰化多肽组成，是通过反应性N-羧基酐单体的开环聚合反应以及随后对多肽进行侧链修饰而制备的。如1所示，成功制备了具有类似主链长度和相同数量的低聚（乙二醇）（OEG）单元的Y型（6a）或线性侧基（6b）的OEG化三嵌段共聚物1 H NMR，FTIR和GPC。CD分析表明，带有Y形OEG悬垂物的6a表现出热或盐诱导的水中α螺旋构象的失稳。6a和6b均在DI H 2 O或PBS中显示出可逆的较低临界溶液温度（LCST）型相变。PPG段的引入会导致LCST型浊点温度（T cp）的显着降低。因此，图6a和6b在低聚合物浓度（≤0.5mg mL -1）下显示出对人体温度的T cp。在PBS中）。此外，6a和6b在存在蛋白酶K的情况下显示出较低的体外细胞毒性和生物降解性。结果表明，可以通过构建Y型悬垂物以及掺入疏水性聚合物构建基团来轻松调节LCST型聚合物的热响应特性。 。
更新日期：2019-12-18
中文翻译：
具有线性或Y型OEG吊坠的生物相容性和可生物降解的三嵌段共聚物的合成和热响应性能
生物相容性和可生物降解的热响应性聚合物在“智能”生物医学应用中备受关注。在此，三元共聚物（6a和6b）由疏水性聚丙二醇（PPG）和带有Y形或线性侧基的OEG酰化多肽组成，是通过反应性N-羧基酐单体的开环聚合反应以及随后对多肽进行侧链修饰而制备的。如1所示，成功制备了具有类似主链长度和相同数量的低聚（乙二醇）（OEG）单元的Y型（6a）或线性侧基（6b）的OEG化三嵌段共聚物1 H NMR，FTIR和GPC。CD分析表明，带有Y形OEG悬垂物的6a表现出热或盐诱导的水中α螺旋构象的失稳。6a和6b均在DI H 2 O或PBS中显示出可逆的较低临界溶液温度（LCST）型相变。PPG段的引入会导致LCST型浊点温度（T cp）的显着降低。因此，图6a和6b在低聚合物浓度（≤0.5mg mL -1）下显示出对人体温度的T cp。在PBS中）。此外，6a和6b在存在蛋白酶K的情况下显示出较低的体外细胞毒性和生物降解性。结果表明，可以通过构建Y型悬垂物以及掺入疏水性聚合物构建基团来轻松调节LCST型聚合物的热响应特性。 。
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