Bioorganic Chemistry Laboratory, New Chemistry Unit and ‡Molecular Electronics Lab, Chemistry and Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research , Jakkur P.O., Bengaluru 560064, Karnataka, India.
ACS Appl Mater Interfaces. 2016 Nov 9;8(44):30362-30371. doi: 10.1021/acsami.6b10527. Epub 2016 Oct 28.
Reliable and ultrasensitive detection of mercury ions is of paramount importance for toxicology assessment, environmental protection, and human health. Herein, we present a novel optoelectronic approach based on nanoarchitectonics of small-molecule templated DNA system that consists of an adenine (A)-conjugated small organic semiconductor (BNA) and deoxyribo-oligothymidine (dT). This mutually templated dynamic chiral coassembly system (BNAn-dT) with tunable chiroptical, morphological, and electrical properties is tapped in to enable ultrasensitive and selective detection of inorganic and organometallic mercury in water. We observe a rapid transformation of the BNA-dT coassembly into a metallo-DNA duplex [dT-Hg-dT] in the presence of mercury, which is utilized for a chiro-optical and conductivity-based rapid and subnanomolar sensitivity (≥0.1 nM, 0.02 ppb) to mercury ions in water (∼100 times lower than United States Environmental Protection Agency tolerance limit). This ultrasensitive detection of inorganic and organometallic mercury is driven by a novel chemical design principle that allows strong mercury thymine interaction. This study is anticipated to inspire the development of future templated DNA nanotechnology-based optoelectronic devices for the rapid and ultrasensitive detection of numerous other toxic analytes.
可靠且超灵敏地检测汞离子对于毒理学评估、环境保护和人类健康至关重要。在此，我们提出了一种基于小分子模板 DNA 系统的纳米结构的光电新方法，该系统由腺嘌呤（A）共轭小分子有机半导体（BNA）和脱氧寡胸腺嘧啶（dT）组成。这种具有可调手性、形态和电性能的相互模板动态手性共组装系统（BNAn-dT）被用于在水中超灵敏和选择性地检测无机和有机汞。我们观察到，在汞存在下，BNA-dT 共组装迅速转化为金属-DNA 双链[ dT-Hg-dT]，可用于基于手性光学和电导率的快速和纳摩尔级灵敏度（≥0.1 nM，0.02 ppb）对水中的汞离子进行检测（比美国环境保护局的耐受限度低约 100 倍）。这种对无机和有机汞的超灵敏检测是由一种新的化学设计原理驱动的，该原理允许强的汞胸腺嘧啶相互作用。这项研究有望激发基于模板 DNA 纳米技术的光电设备的未来发展，用于快速和超灵敏地检测许多其他有毒分析物。
