具有刷上超支化臂结构的核壳共聚物：合成、双热响应行为和纳米载体,Macromolecules

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具有刷上超支化臂结构的核壳共聚物：合成、双热响应行为和纳米载体
Macromolecules ( IF 5.1 ) Pub Date : 2021-09-03 , DOI: 10.1021/acs.macromol.1c00813
Jun Zhang ₁ , Bixin Jin ₁ , Gang Tang ₁ , Yunjun Luo _{1,

2} , Xiaoyu Li _{1,

2,

3}

Affiliation

合成并详细表征了一系列具有刷上超支化臂结构的核壳共聚物。这些共聚物是通过阳离子开环聚合 (CROP) 和叠氮化物-炔“点击”化学的组合制备的。初级超支化聚醚核 (HPEHO) 是通过 3-乙基-3-(羟甲基) 氧杂环丁烷 (EHO) 的 CROP 合成的。随后，通过表氯醇 (ECH) 的 CROP 制备缩水甘油叠氮化物聚合物 (GAP) 线性臂的外层，然后进行氯原子的叠氮化。最后通过“点击”反应将聚（乙二醇）（PEG）接枝到 GAP 链上，以获得两亲核壳结构。这些核壳共聚物在水溶液中表现出较低的临界溶解温度 (LCST) 型行为。LCST 浊点 (CP) 温度不仅随着聚合物浓度的增加而降低，而且还取决于分子结构，随着 PEG 刷长度和 GAP 臂长度的增加而增加。更有趣的是，虽然游离 PEG 链完全溶于 THF，但在 THF 中观察到这些核壳共聚物的上临界溶解温度 (UCST) 转变，并且随着 GAP 线性臂长度和浓度的增加，CP 向更高温度移动。最后，PEG 外壳和疏水性内部聚醚核使这些共聚物成为水溶液中疏水性货物分子的理想纳米载体。更有趣的是，虽然游离 PEG 链完全溶于 THF，但在 THF 中观察到这些核壳共聚物的上临界溶解温度 (UCST) 转变，并且随着 GAP 线性臂长度和浓度的增加，CP 向更高温度移动。最后，PEG 外壳和疏水性内部聚醚核使这些共聚物成为水溶液中疏水性货物分子的理想纳米载体。更有趣的是，虽然游离 PEG 链完全溶于 THF，但在 THF 中观察到这些核壳共聚物的上临界溶解温度 (UCST) 转变，并且随着 GAP 线性臂长度和浓度的增加，CP 向更高温度移动。最后，PEG 外壳和疏水性内部聚醚核使这些共聚物成为水溶液中疏水性货物分子的理想纳米载体。

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Core–Shell Copolymers with Brush-on-Hyperbranched Arm Architecture: Synthesis, Dual Thermoresponsive Behaviors, and Nanocarriers

A series of core–shell copolymers with brush-on-hyperbranched arm architecture were synthesized and characterized in detail. These copolymers were prepared via the combination of cationic ring-opening polymerization (CROP) and azide-alkyne “click” chemistry. The primary hyperbranched polyether core (HPEHO) was synthesized via the CROP of 3-ethyl-3-(hydroxymethyl)oxetane (EHO). Subsequently, the outer layer of glycidyl azide polymer (GAP) linear arms was prepared through the CROP of epichlorohydrin (ECH), followed by azidation of the chlorine atoms. Poly(ethylene glycol) (PEG) was last grafted onto the GAP chains via “click” reaction to obtain an amphiphilic core–shell structure. These core–shell copolymers exhibited a lower critical solution temperature (LCST)-type behavior in aqueous solutions. The LCST cloud point (CP) temperature not only decreased with an increasing polymer concentration but also was dependent on the molecular architecture that it increased upon increasing the PEG brush lengths and GAP arm lengths. More interestingly, while the free PEG chains were completely soluble in THF, an upper critical solution temperature (UCST) transition was observed for these core–shell copolymers in THF, and the CP shifted toward higher temperatures with increasing GAP linear arm lengths and concentrations. Last, the PEG outer shell and hydrophobic interior polyether core made these copolymers decent nanocarriers for hydrophobic cargo molecules in aqueous solutions.

更新日期：2021-09-28

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