Hu Shengqiang, Huang Po-Jung Jimmy, Wang Jianxiu, Liu Juewen
College of Chemistry and Chemical Engineering, Central South University, Changsha, China.
Department of Chemistry, Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo, ON, Canada.
Front Chem. 2019 Apr 16;7:198. doi: 10.3389/fchem.2019.00198. eCollection 2019.
Many DNA-functionalized nanomaterials and biosensors have been reported, but most have ignored the influence of DNA on the stability of nanoparticles. We observed that cytosine-rich DNA oligonucleotides can etch silver nanoparticles (AgNPs). In this work, we showed that phosphorothioate (PS)-modified DNA (PS-DNA) can etch AgNPs independently of DNA sequence, suggesting that the thio-modifications are playing the major role in etching. Compared to unmodified DNA (e.g., poly-cytosine DNA), the concentration of required PS DNA decreases sharply, and the reaction rate increases. Furthermore, etching by PS-DNA occurs quite independent of pH, which is also different from unmodified DNA. The PS-DNA mediated etching could also be controlled well by varying DNA length and conformation, and the number and location of PS modifications. With a higher activity of PS-DNA, the process of etching, ripening, and further etching was taken place sequentially. The etching ability is inhibited by forming duplex DNA and thus etching can be used to measure the concentration of complementary DNA.
许多DNA功能化的纳米材料和生物传感器已见报道,但大多数都忽略了DNA对纳米颗粒稳定性的影响。我们观察到富含胞嘧啶的DNA寡核苷酸能够蚀刻银纳米颗粒(AgNP)。在本研究中,我们发现硫代磷酸酯(PS)修饰的DNA(PS-DNA)能够独立于DNA序列蚀刻AgNP,这表明硫代修饰在蚀刻过程中起主要作用。与未修饰的DNA(如聚胞嘧啶DNA)相比,所需PS-DNA的浓度急剧降低,且反应速率增加。此外,PS-DNA介导的蚀刻与pH无关,这也与未修饰的DNA不同。PS-DNA介导的蚀刻还可以通过改变DNA长度和构象以及PS修饰的数量和位置得到很好的控制。由于PS-DNA具有更高的活性,蚀刻、熟化和进一步蚀刻的过程依次发生。形成双链DNA会抑制蚀刻能力,因此蚀刻可用于测量互补DNA的浓度。