Institute for NanoBioTechnology, Johns Hopkins University, Baltimore, Maryland 21218, United States.
Department of Chemical and Biomolecular Engineering, Johns Hopkins University, Baltimore, Maryland 21218, United States.
Bioconjug Chem. 2022 Nov 16;33(11):2035-2040. doi: 10.1021/acs.bioconjchem.2c00090. Epub 2022 Jun 14.
In this work, we demonstrate the formation of supramolecular architectures from the assembly of single-tail single stranded DNA (ssDNA)-amphiphiles. Short ssDNA sequences of 10 nucleotides that were either unstructured or formed G-quadruplex secondary structures were conjugated to a single 4-(hexadecyloxy)benzamide tail, either directly or through a polycarbon (C) spacer. Conjugation of the ssDNA to the tail did not interfere with the G-quadruplex secondary structure of the ssDNA sequence. The ssDNA-amphiphiles self-assembled into ellipsoidal micelles, vesicles, nanotapes, and nanotubes. These nanotubes appeared to be formed by the rolling up of nanotapes. The increase of the hydrophobic block of the ssDNA-amphiphiles through the addition of a C spacer led to an increase in wall thickness and nanotube diameter. The presence of π-π interactions, through the benzoic group, was verified via X-ray diffraction (XRD) and played a critical role in the formation of the different nanostructures. In contrast, ssDNA-amphiphiles with a single heptadecanoic acid tail self-assembled only into ellipsoidal micelles.
在这项工作中，我们展示了由单链 DNA（ssDNA）两亲物的组装形成的超分子结构。将 10 个核苷酸的短 ssDNA 序列连接到单个 4-（十六烷氧基）苯甲酰胺尾部，无论是直接连接还是通过聚碳酸酯（C）间隔物连接，这些 ssDNA 序列要么无结构，要么形成 G-四链体二级结构。ssDNA 与尾部的连接不干扰 ssDNA 序列的 G-四链体二级结构。ssDNA-两亲物自组装成椭圆形胶束、囊泡、纳米带和纳米管。这些纳米管似乎是由纳米带的卷起形成的。通过添加 C 间隔物增加 ssDNA-两亲物的疏水性块，导致壁厚度和纳米管直径增加。通过苯甲酰基存在的 π-π 相互作用，通过 X 射线衍射（XRD）得到了验证，并在形成不同的纳米结构中发挥了关键作用。相比之下，具有单个十七烷酸尾的 ssDNA-两亲物仅自组装成椭圆形胶束。
