Zhou Zhun, Munyaradzi Oliver, Xia Xin, Green Da'Sean, Bong Dennis
Department of Chemistry and Biochemistry, The Ohio State University , 100 West 18th Avenue, Columbus, Ohio 43210, United States.
Biomacromolecules. 2016 Sep 12;17(9):3060-6. doi: 10.1021/acs.biomac.6b00960. Epub 2016 Aug 23.
We report herein a dual-purpose role for polyacidic domains in an aqueous-phase polymer amphiphile assembly. In addition to their typical role as ionized water-solubilizing and self-repulsive motifs, we find that polycarboxylic acid domains uniquely enable high levels of hydrophobic drug encapsulation. By attenuated total reflectance infrared spectroscopy, we find significant differences in the carbonyl stretching region of the nanoparticles formed by polyacidic amphiphiles relative to those in soluble, single-domain poly(acrylic acid), suggesting that stabilization may be derived from limited ionization of the carboxylate groups upon assembly. Acidic-hydrophobic diblock polyacrylates were prepared and coassembled with up to 60 wt % camptothecin (CPT) into nanoparticles, the highest loading reported to date. Controlled release of bioactive CPT from polymer nanoparticles is observed, as well as protection from human serum albumin-induced hydrolysis. Surface protection with PEG limits uptake of the CPT-loaded nanoparticles by MCF-7 breast cancer cells, as expected. Acidic-hydrophobic polymer amphiphiles thus have the hallmarks of a useful and general drug delivery platform and are readily accessible from living radical polymerization of cheap, commercially available monomers. We highlight here the potential utility of this common polymer design in high-capacity, controlled-release polymer nanoparticle systems.
我们在此报告了多酸性结构域在水相聚合物两亲物组装中的双重作用。除了其作为离子化水溶性和自排斥基序的典型作用外,我们发现多羧酸结构域独特地能够实现高水平的疏水药物包封。通过衰减全反射红外光谱,我们发现多酸性两亲物形成的纳米颗粒在羰基伸缩区域相对于可溶性单域聚丙烯酸存在显著差异,这表明组装时羧酸盐基团的有限电离可能产生了稳定性。制备了酸性-疏水性二嵌段聚丙烯酸酯,并与高达60 wt%的喜树碱(CPT)共组装成纳米颗粒,这是迄今为止报道的最高载药量。观察到生物活性CPT从聚合物纳米颗粒中的控释,以及对人血清白蛋白诱导水解的保护作用。正如预期的那样,用聚乙二醇进行表面保护限制了载CPT纳米颗粒被MCF-7乳腺癌细胞摄取。因此,酸性-疏水性聚合物两亲物具有有用且通用的药物递送平台的特征,并且可以通过廉价的市售单体的活性自由基聚合轻松获得。我们在此强调这种常见聚合物设计在高容量、控释聚合物纳米颗粒系统中的潜在用途。