Quaternary Ammonium-Terminated Films Formed from Mixed Bidentate Adsorbates Provide a High-Capacity Platform for Oligonucleotide Delivery
Quaternary Ammonium-Terminated Films Formed from Mixed Bidentate Adsorbates Provide a High-Capacity Platform for Oligonucleotide Delivery
复制标题
由混合双齿吸附物形成的季铵封端薄膜为寡核苷酸递送提供高容量平台
DOI：
10.1021/acsami.8b12244
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发表时间：
2018
影响因子：
9.5
通讯作者：
Lee, T. Randall
中科院分区：
文献类型：
--
作者：
Hoang, Johnson;Park, Chul Soon;Lee, Han Ju;Marquez, Maria D.;Zenasni, Oussama;Gunaratne, Preethi H.;Lee, T. Randall
季铵盐基团在表面的暴露使自组装单分子膜(SAM)可以作为固定寡核苷酸的结构平台。本研究描述了四种独特的含有两个不同氨端(即三甲基和三乙基)的双齿吸附体的自组装膜的制备，并与它们的单齿类似物进行了比较。我们的研究发现，与来自单齿类似物的自组装膜相比，来自双齿吸附体的自组装膜在寡核苷酸结合方面有相当大的增强作用。用椭偏仪、X射线光电子能谱、接触角测角法、偏振调制红外反射吸收光谱和电化学石英晶体微天平对自组装膜进行了分析。这些分析表明，寡核苷酸的固定化受到末端官能度和单层相对堆积密度的变化的影响。为了进一步加强寡核苷酸在这些SAM表面的固定化，我们探索了使用具有系统不同链长的脂族连接物的吸附来在金表面形成二元SAM。吸附物比例为50：50的混合单层显示最大的寡核苷酸结合力。这些研究为使用基于金的纳米颗粒和纳米壳传递寡核苷酸奠定了基础。
The exposure of quaternary ammonium groups on surfaces allows self-assembled monolayers (SAMs) to serve as architectural platforms for immobilizing oligonucleotides. The current study describes the preparation of SAMs derived from four unique bidentate adsorbates containing two different ammonium termini (i.e., trimethyl- and triethyl-) and comparison to their monodentate analogs. Our studies found that SAMs derived from the bidentate adsorbates offered considerable enhancements in oligonucleotide binding when compared to SAMs derived from their monodentate analogs. The generated SAMs were analyzed using ellipsometry, X-ray photoelectron spectroscopy, contact angle goniometry, polarization modulation infrared reflection-absorption spectroscopy, and electrochemical quartz crystal microbalance. These analyses showed that the immobilization of oligonucleotides was affected by changes in the terminal functionalities and the relative packing densities of the monolayers. In efforts to enhance further the immobilization of oligonucleotides on these SAM surfaces, we explored the use of adsorbates having aliphatic linkers with systematically varying chain lengths to form binary SAMs on gold. Mixed monolayers with 50:50 ratios of adsorbates showed the greatest oligonucleotide binding. These studies lay the groundwork for oligonucleotide delivery using gold-based nanoparticles and nanoshells.