School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue 639798, Singapore.
Phys Chem Chem Phys. 2015 May 7;17(17):11546-52. doi: 10.1039/c5cp01428j.
In this study, we employed the solvent-assisted lipid bilayer (SALB) formation method to fabricate charged membranes on solid supports. The SALB formation method exploits a ternary mixture of lipid-alcohol-aqueous buffer to deposit lamellar phase structures on solid supports upon gradual increase of the buffer fraction. Using the quartz crystal microbalance with dissipation (QCM-D) technique, we investigated the formation of negatively and positively charged membranes via the SALB formation method and directly compared with the vesicle fusion method on two different oxide films. Bilayers containing an increasing fraction of negatively charged DOPS lipid molecules were successfully formed on both SiO2 and Al2O3 substrates using the SALB formation method at physiological pH (7.5). In contrast, the vesicle fusion method did not support bilayer formation on Al2O3 and those containing more than 10% DOPS ruptured on SiO2 only under acidic conditions (pH 5). Characterization of the fraction of negatively charge DOPS by in situ annexin 5A binding assay revealed that the fraction of DOPS lipid molecules in the bilayers formed on Al2O3 is significantly higher than that formed on SiO2. This suggests that the SALB self-assembly of charged membranes is predominantly governed by the electrostatic interaction. Furthermore, our findings indicate that when multicomponent lipid mixtures are used, the relative fraction of lipids in the bilayer may differ from the fraction of lipids in the precursor mixture.
在这项研究中,我们采用溶剂辅助双层脂质体(SALB)形成方法在固体支持物上制备带电膜。SALB 形成方法利用脂质-醇-水缓冲液的三元混合物,在缓冲液部分逐渐增加的情况下,在固体支持物上沉积层状结构。我们使用石英晶体微天平(QCM-D)技术,通过 SALB 形成方法研究了带负电和带正电膜的形成,并直接与囊泡融合方法在两种不同的氧化物膜上进行了比较。在生理 pH(7.5)下,我们成功地使用 SALB 形成方法在 SiO2 和 Al2O3 基底上形成了含有越来越多的带负电 DOPS 脂质分子的双层。相比之下,囊泡融合方法在 Al2O3 上不支持双层形成,而在 SiO2 上只有在酸性条件(pH 5)下才会形成含有超过 10% DOPS 的双层破裂。通过原位 annexin 5A 结合测定法对带负电荷 DOPS 的分数进行了表征,结果表明在 Al2O3 上形成的双层中 DOPS 脂质分子的分数明显高于在 SiO2 上形成的双层。这表明带电荷膜的 SALB 自组装主要受静电相互作用控制。此外,我们的研究结果表明,当使用多组分脂质混合物时,双层中脂质的相对分数可能与前体混合物中脂质的分数不同。