Fan Daoqing, Fan Yongchao, Wang Erkang, Dong Shaojun
State Key Laboratory of Electro Analytical Chemistry , Changchun Institute of Applied Chemistry , Chinese Academy of Sciences , Changchun , Jilin 130022 , China . Email:
University of Chinese Academy of Sciences , Beijing , 100039 , China.
Chem Sci. 2018 Jul 19;9(34):6981-6987. doi: 10.1039/c8sc02482k. eCollection 2018 Sep 14.
Versatile DNA logic devices have exhibited magical power in molecular-level computing and data processing. During any type of data transmission, the appearance of erroneous bits (which have severe impacts on normal computing) is unavoidable. Luckily, the erroneous bits can be detected placing a parity generator (pG) at the sending module and a parity checker (pC) at the receiving module. However, all current DNA pG/pC systems use optical signals as outputs. In comparison, sensitive, facilely operated, electric-powered electrochemical outputs possess inherent advantages in terms of potential practicability and future integration with semiconductor transistors. Herein, taking an even pG/pC as a model device, we construct the first electrochemical DNA pG/pC system so far. Innovatively, a thrombin aptamer is integrated into the input-strand and it functions as a "nanoclaw" to selectively capture thrombin; the electrochemical impedance changes induced by the "nanoclaw/thrombin" complex are used as label-free outputs. Notably, this system is simple and can be operated within 2 h, which is comparable with previous fluorescent ones, but avoids the high-cost labeled-fluorophore and tedious nanoquencher. Moreover, taking non-interfering poly-T strands as additional inputs, a cascade logic circuit (OR-2 to 1 encoder) and a parity checker that could distinguish even/odd numbers from natural numbers (0 to 9) is also achieved based on the same system. This work not only opens up inspiring horizons for the design of novel electrochemical functional devices and complicated logic circuits, but also lays a solid foundation for potential logic-programmed target detection.
多功能DNA逻辑器件在分子级计算和数据处理中展现出了神奇的力量。在任何类型的数据传输过程中,错误比特(对正常计算有严重影响)的出现都是不可避免的。幸运的是,通过在发送模块放置一个奇偶校验生成器(pG)以及在接收模块放置一个奇偶校验检查器(pC),可以检测到这些错误比特。然而,目前所有的DNA pG/pC系统都使用光信号作为输出。相比之下,灵敏、易于操作的电动电化学输出在潜在实用性以及未来与半导体晶体管集成方面具有内在优势。在此,我们以一个偶数奇偶校验pG/pC作为模型器件,构建了迄今为止首个电化学DNA pG/pC系统。创新之处在于,将凝血酶适配体整合到输入链中,它作为一个“纳米爪”来选择性捕获凝血酶;由“纳米爪/凝血酶”复合物诱导的电化学阻抗变化被用作无标记输出。值得注意的是,该系统简单,可在2小时内完成操作,这与之前的荧光系统相当,但避免了高成本的标记荧光团和繁琐的纳米猝灭剂。此外,以不产生干扰的聚T链作为额外输入,基于同一系统还实现了一个级联逻辑电路(OR - 2到1编码器)以及一个能够从自然数(0到9)中区分偶数/奇数的奇偶校验检查器。这项工作不仅为新型电化学功能器件和复杂逻辑电路的设计开辟了令人鼓舞的前景,也为潜在的逻辑编程目标检测奠定了坚实基础。