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Encapsulation and Release of Recognition Probes Based on a Rigid Three-Dimensional DNA "Nanosafe-box" for Construction of a Electrochemical Biosensor.
Analytical Chemistry ( IF 6.7 ) Pub Date : 2020-01-09 , DOI: 10.1021/acs.analchem.9b03627 Min Qing 1, 2 , Shengliang Chen 1 , Shunbi Xie 2 , Ying Tang 2 , Jin Zhang 2 , Ruo Yuan 1
Analytical Chemistry ( IF 6.7 ) Pub Date : 2020-01-09 , DOI: 10.1021/acs.analchem.9b03627 Min Qing 1, 2 , Shengliang Chen 1 , Shunbi Xie 2 , Ying Tang 2 , Jin Zhang 2 , Ruo Yuan 1
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Herein a rigid three-dimensional (3D) DNA "nanosafe-box" (DNB) for encapsulation and release of a recognition probe (N3) is designed to construct an electrochemical biosensor with the use of electroactive two-dimensional metal-organic framework (2D MOF) nanosheets as signal tags for ultrasensitive detection of mercury ion (Hg2+). Initially, N3 is locked in the 3D cavity of DNB by blocker DNA. After addition of target Hg2+, exonuclease III (Exo-III) digestion is initiated to the liberate DNA "key" (K); thereby, the free K triggers a strand displacement reaction for exposing the prelocked N3 to successfully ligate dibenzocyclooctyne (DBCO)-tagged anchor via metal-catalyst-free click chemistry, in which amounts of 2D MOF nanosheets containing Co(II) as electron mediator are introduced accompanied by significant electrochemical response. Compared with traditional linear or stem-loop DNA nanostructure, the well-designed 3D DNB possesses remarkably enhanced mechanical rigidity and structural stability, resulting in improved accessibility of probes and increased loading amounts of signal tags. More importantly, by this way of encapsulation and release of recognition probes, the background signal is decreased dramatically, leading to increased sensitivity of the proposed biosensor. Consequently, this electrochemical biosensor exhibits outstanding analytical performance for Hg2+ detection with a low detection limit of 33 fM and dynamic linear range of 0.1 pM to 10 nM. This strategy offers an ingenious method for detection of metal ions and biomarkers, possessing potential applications in environmental tests and clinical diagnosis.
中文翻译：
基于刚性三维DNA“ Nanosafe-box”的识别探针的封装和释放，用于构建电化学生物传感器。
本文中，用于封装和释放识别探针（N3）的刚性三维（3D）DNA“纳米安全盒”（DNB）被设计为使用电活性二维金属有机框架（2D）来构建电化学生物传感器。 MOF）纳米片作为信号标签，用于超灵敏地检测汞离子（Hg2 +）。最初，N3被阻断剂DNA锁定在DNB的3D腔中。加入目标Hg2 +后，核酸外切酶III（Exo-III）消化开始，释放出DNA“ key”（K）；从而，游离K触发链置换反应，从而使预锁N3通过无金属催化剂的点击化学作用成功连接二苯并环辛炔（DBCO）标记的锚，其中引入了数量众多的含有Co（II）作为电子介体的2D MOF纳米片，并伴随着明显的电化学反应。与传统的线性或茎环DNA纳米结构相比，精心设计的3D DNB具有显着增强的机械刚度和结构稳定性，从而改善了探针的可及性并增加了信号标签的装载量。更重要的是，通过这种封装和释放识别探针的方式，背景信号显着降低，从而导致所提出的生物传感器的灵敏度提高。因此，该电化学生物传感器显示出出色的Hg2 +检测分析性能，检测限低至33 fM，动态线性范围为0.1 pM至10 nM。
更新日期：2020-01-10
中文翻译：
基于刚性三维DNA“ Nanosafe-box”的识别探针的封装和释放，用于构建电化学生物传感器。
本文中，用于封装和释放识别探针（N3）的刚性三维（3D）DNA“纳米安全盒”（DNB）被设计为使用电活性二维金属有机框架（2D）来构建电化学生物传感器。 MOF）纳米片作为信号标签，用于超灵敏地检测汞离子（Hg2 +）。最初，N3被阻断剂DNA锁定在DNB的3D腔中。加入目标Hg2 +后，核酸外切酶III（Exo-III）消化开始，释放出DNA“ key”（K）；从而，游离K触发链置换反应，从而使预锁N3通过无金属催化剂的点击化学作用成功连接二苯并环辛炔（DBCO）标记的锚，其中引入了数量众多的含有Co（II）作为电子介体的2D MOF纳米片，并伴随着明显的电化学反应。与传统的线性或茎环DNA纳米结构相比，精心设计的3D DNB具有显着增强的机械刚度和结构稳定性，从而改善了探针的可及性并增加了信号标签的装载量。更重要的是，通过这种封装和释放识别探针的方式，背景信号显着降低，从而导致所提出的生物传感器的灵敏度提高。因此，该电化学生物传感器显示出出色的Hg2 +检测分析性能，检测限低至33 fM，动态线性范围为0.1 pM至10 nM。
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