Song Jun, Wei Yanlong, Hu Jiwen, Liu Guojun, Huang Zhengzhu, Lin Shudong, Liu Feng, Mo Yangmiao, Tu Yuanyuan, Ou Ming
Guangzhou Institute of Chemistry, Chinese Academy of Sciences, Guangzhou, 510650, P. R. China.
Key Laboratory of Cellulose and Lignocellulosics Chemistry, Chinese Academy of Sciences, Guangzhou, 510650, P. R. China.
Chemistry. 2018 Jan 2;24(1):212-221. doi: 10.1002/chem.201704328. Epub 2017 Dec 4.
In this work pH-responsive porous nanocapsules have been successfully prepared from a ternary graft copolymer, poly(glycidyl methacrylate)-g-[poly(2-cinnamoyloxyethyl methacrylate)-r-poly(ethylene glycol) methyl ether-r-poly(2-diethylaminoethyl methacrylate)] or PGMA-g-(PCEMA-r-MPEG-r-PDEAEMA). The graft copolymers were fabricated by grafting three types of polymer chains onto the backbone polymer by using click chemistry. These ternary copolymers underwent self-assembly to form vesicles in a DMF/water solvent mixture. While the MPEG chains served as the corona and stabilized the vesicles, the vesicle wall was composed of a dominant PCEMA continuous phase that was interspersed by PDEAEMA domains. After photo-cross-linking, the PDEAEMA domains were embedded in the structurally locked PCEMA wall. By decreasing the pH of the external solution, we were able to trigger the release of encapsulated pyrene due to the capsule wall becoming porous as a result of the PDEAEMA chains bearing positively charged amine groups stretching into the water. While these pH-responsive porous nanocapsules exhibited potential applications in drug delivery, detection and catalysis, the strategy reported in this contribution also represented a new paradigm for the design and preparation of other novel stimuli-responsive porous nanocapsules.
在这项工作中，通过三元接枝共聚物聚（甲基丙烯酸缩水甘油酯）-g-[聚（甲基丙烯酸2-肉桂酰氧基乙酯）-r-聚（乙二醇）甲醚-r-聚（甲基丙烯酸2-二乙氨基乙酯）]或PGMA-g-(PCEMA-r-MPEG-r-PDEAEMA)成功制备了pH响应性多孔纳米胶囊。通过点击化学将三种类型的聚合物链接枝到主链聚合物上制备了接枝共聚物。这些三元共聚物在N,N-二甲基甲酰胺/水溶剂混合物中进行自组装形成囊泡。虽然MPEG链作为冠层并使囊泡稳定，但囊泡壁由占主导地位的PCEMA连续相组成，该连续相中散布着PDEAEMA域。光交联后，PDEAEMA域嵌入结构锁定的PCEMA壁中。通过降低外部溶液的pH值，由于带有带正电荷胺基的PDEAEMA链伸展到水中导致囊壁变得多孔，我们能够触发封装芘的释放。虽然这些pH响应性多孔纳米胶囊在药物递送、检测和催化方面显示出潜在应用，但本论文报道的策略也代表了设计和制备其他新型刺激响应性多孔纳米胶囊的新范例。
