State Key Laboratory of Developmental Biology of Freshwater Fish, Hunan Provincial Key Laboratory of Microbial Molecular Biology, College of Life Science , Hunan Normal University , Changsha 410081 , P. R. China.
ACS Appl Mater Interfaces. 2019 Mar 6;11(9):8904-8914. doi: 10.1021/acsami.8b22592. Epub 2019 Feb 21.
Inspired by information processing and communication of life based on complex molecular interactions, some artificial (bio)chemical systems have been developed for applications in molecular information processing or chemo/biosensing and imaging. However, little attention has been paid to simultaneously and comprehensively utilize the information computing, encoding, and molecular recognition capabilities of molecular-level systems (such as DNA-based systems) for multifunctional applications. Herein, a graphene-based steganographically aptasensing system was constructed for multifunctional application, which relies on specific molecular recognition and information encoding abilities of DNA aptamers ( Aeromonas hydrophila and Edwardsiella tarda-binding aptamers as models) and the selective adsorption and fluorescence quenching capacities of graphene oxide (GO). Although graphene-DNA systems have been widely used in biosensors and diagnostics, our proposed graphene-based aptasensing system can not only be utilized for fluorescence sensing and in vivo imaging of fish pathogens ( A. hydrophila and E. tarda), but can also function as a molecular-level logic computing system where the combination of matters (specific molecules or materials) as inputs produces the resulting product (matter level) or fluorescence (energy level) changes as two outputs. More importantly and interestingly, our graphene-based steganographically aptasensing system can also serve as a generally doubly cryptographic and steganographic system for sending different secret messages by using pathogen-binding DNA aptamers as information carriers, GO as a cover, and a pair of keys, that is, target pathogen as a public key, the encryption key used to encode or decode a message in DNA as a private key. Our study not only provides a novel nanobiosensing assay for rapid and effective sensing and in vivo imaging of fish pathogens, but also demonstrates a prototype of (bio)molecular steganography as an important and interesting extension direction of molecular information technology, which is helpful in probably promoting the development of multifunctional molecular-level devices or machines.
受基于复杂分子相互作用的生命信息处理和通讯的启发，人们已经开发出一些人工（生物）化学系统，用于分子信息处理或化学生物传感和成像等应用。然而，人们很少关注同时充分利用分子级系统（如基于 DNA 的系统）的信息计算、编码和分子识别能力，用于多功能应用。在此，构建了一种基于石墨烯的隐匿适体传感系统，用于多功能应用，该系统依赖于 DNA 适体（以嗜水气单胞菌和迟缓爱德华氏菌结合适体作为模型）的特定分子识别和信息编码能力，以及石墨烯氧化物（GO）的选择性吸附和荧光猝灭能力。虽然石墨烯-DNA 系统已广泛应用于生物传感器和诊断学中，但我们提出的基于石墨烯的适体传感系统不仅可用于鱼类病原体（嗜水气单胞菌和迟缓爱德华氏菌）的荧光传感和体内成像，还可用作分子级逻辑计算系统，其中物质（特定分子或材料）的组合作为输入，产生作为两个输出的产物（物质水平）或荧光（能量水平）变化。更重要的是，我们基于石墨烯的隐匿适体传感系统还可以作为一种通用的双重加密和隐匿系统，通过使用病原体结合 DNA 适体作为信息载体、GO 作为覆盖物和一对密钥（即目标病原体作为公钥、用于对 DNA 中的消息进行编码或解码的加密密钥作为私钥），发送不同的秘密消息。我们的研究不仅为快速、有效检测和体内成像鱼类病原体提供了一种新的纳米生物传感分析方法，而且还展示了（生物）分子隐匿术的原型，作为分子信息技术的一个重要而有趣的扩展方向，这有助于促进多功能分子级器件或机器的发展。
