Hsu Hao-Jui, Sen Soumyo, Pearson Ryan M, Uddin Sayam, Král Petr, Hong Seungpyo
Departments of Biopharmaceutical Sciences, Bioengineering, Chemistry, and Physics, University of Illinois at Chicago , Chicago, Illinois 60612, United States.
Macromolecules. 2014 Oct 14;47(19):6911-6918. doi: 10.1021/ma501258c. Epub 2014 Sep 30.
To systematically investigate the relationship among surface charge, PEG chain length, and nano-bio interactions of dendron-based micelles (DMs), a series of PEGylated DMs with various end groups (-NH, -Ac, and -COOH) and PEG chain lengths (600 and 2000 g/mol) are prepared and tested . The DMs with longer PEG chains (DM) do not interact with cells despite their positively charged surfaces. In sharp contrast, the DMs with shorter PEG chains (DM) exhibit charge-dependent cellular interactions, as observed in both and molecular dynamics (MD) simulation results. Furthermore, all DMs with different charges display enhanced stability for hydrophobic dye encapsulation compared to conventional linear-block copolymer-based micelles, by allowing only a minimal leakage of the dye . Our results demonstrate the critical roles of the PEG chain length and polymeric architecture on the terminal charge effect and the stability of micelles, which provides an important design cue for polymeric micelles.
为了系统地研究基于树枝状分子的胶束（DMs）的表面电荷、聚乙二醇（PEG）链长度与纳米-生物相互作用之间的关系，制备并测试了一系列具有不同端基（-NH、-Ac和-COOH）和PEG链长度（600和2000 g/mol）的聚乙二醇化DMs。具有较长PEG链的DMs（DM）尽管表面带正电荷，但不与细胞相互作用。与之形成鲜明对比的是，具有较短PEG链的DMs（DM）表现出电荷依赖性细胞相互作用，这在实验和分子动力学（MD）模拟结果中均有观察到。此外，与传统的基于线性嵌段共聚物的胶束相比，所有带不同电荷的DMs对疏水性染料包封均表现出更高的稳定性，染料泄漏极少。我们的结果证明了PEG链长度和聚合物结构在末端电荷效应和胶束稳定性方面的关键作用，这为聚合物胶束提供了重要的设计线索。
