Zhou Qing, Yang Tiehong, Qiao Youbei, Guo Songyan, Zhu Lin, Wu Hong
Department of Pharmaceutical Analysis, School of Pharmacy, Fourth Military Medical University, Xi'an, People's Republic of China.
Department of Pharmaceutical Sciences, Irma Lerma Rangel College of Pharmacy, Texas A&M University Health Science Center, Kingsville, Texas, USA.
Int J Nanomedicine. 2015 Mar 10;10:1941-52. doi: 10.2147/IJN.S78547. eCollection 2015.
In this study, a multifunctional poly(β-L-malic acid)-based nanoconjugate with a pH-dependent charge conversional characteristic was developed for tumor-specific drug delivery. The short branched polyethylenimine-modified poly(β-L-malic acid) (PEPM) was first synthesized. Then, the fragment HAb18 F(ab')2 and 2,3-dimethylmaleic anhydride were covalently attached to the PEPM to form the nanoconjugate, HDPEPM. In this nanoconjugate, the 2,3-dimethylmaleic anhydride, the shielding group, could shield the positive charge of the conjugate at pH 7.4, while it was selectively hydrolyzed in the tumor extracellular space (pH 6.8) to expose the previously-shielded positive charge. To study the anticancer activity, the anticancer drug, doxorubicin, was covalently attached to the nanoconjugate. The doxorubicin-loaded HDPEPM nanoconjugate was able to efficiently undergo a quick charge conversion from -11.62 mV to 9.04 mV in response to the tumor extracellular pH. The electrostatic interaction between the positively charged HDPEPM nanoconjugates and the negatively charged cell membrane significantly enhanced their cellular uptake, resulting in the enhanced anticancer activity. Also, the tumor targetability of the nanoconjugates could be further improved via the fragment HAb18 F(ab')2 ligand-receptor-mediated tumor cell-specific endocytosis.
在本研究中,开发了一种具有pH依赖性电荷转换特性的基于聚(β-L-苹果酸)的多功能纳米缀合物,用于肿瘤特异性药物递送。首先合成了短支链聚乙烯亚胺修饰的聚(β-L-苹果酸)(PEPM)。然后,将片段HAb18 F(ab')2和2,3-二甲基马来酸酐共价连接到PEPM上,形成纳米缀合物HDPEPM。在这种纳米缀合物中,屏蔽基团2,3-二甲基马来酸酐在pH 7.4时可屏蔽缀合物的正电荷,而在肿瘤细胞外空间(pH 6.8)中它会被选择性水解,以暴露先前被屏蔽的正电荷。为了研究其抗癌活性,将抗癌药物阿霉素共价连接到纳米缀合物上。负载阿霉素的HDPEPM纳米缀合物能够响应肿瘤细胞外pH值,有效地从-11.62 mV快速进行电荷转换至9.04 mV。带正电荷的HDPEPM纳米缀合物与带负电荷的细胞膜之间的静电相互作用显著增强了它们的细胞摄取,从而提高了抗癌活性。此外,纳米缀合物的肿瘤靶向性可通过片段HAb18 F(ab')2配体-受体介导的肿瘤细胞特异性内吞作用进一步提高。