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A self-calibrating logic system and oxidase-based biosensor using Tb3+-doped carbon dots/DNA conjugates
Talanta ( IF 6.1 ) Pub Date : 2018-08-14 , DOI: 10.1016/j.talanta.2018.08.035
Zi-Han Chen , Xin-Yue Han , Ling-Xue Deng , Zi-Yang Lin , Fang-Ya Mu , Shengqiang Zhang , Guoyue Shi , Min Zhang

Tb3+-doped carbon dots (Tb3+@CDs) were prepared in a facile hydrothermal method by using ammonium citrate as carbon source and Tb3+ as dopant. A 15-bp GT-rich single-strand DNA (ssDNA) was introduced to sensitize Tb3+ via the antenna effect for generating two fluorescence signals (CDs and Tb3+), forming a conjugate of Tb3+@CDs/ssDNA. The ratiometric fluorescence of Tb3+@CDs/ssDNA could be reversibly regulated by Ag+ and Cys, in which the fluorescence peak at 546 nm of Tb3+ could be switched to “On” or “Off” as the signal indicator while the fluorescence peak at 444 nm of CDs remained constant as the build-in reference. The proposed Ag+/Cys-mediated reversible fluorescence changes in Tb3+@CDs/ssDNA was also proven for the design of a self-calibrating ratiometric fluorescence logic system. By integrated with the specific reaction between H2O2 and Cys, Tb3+@CDs/ssDNA was applied for ratiometric fluorescence detection of H2O2. More importantly, the sensing strategy could be further successfully extended to the monitoring of H2O2-produced oxidase-related reactions, such as GOx-biocatalyzed oxidation of glucose (the limit of detection: 0.06 μM) and was well applied in rat serum compared to commercial kits. This work unveiled a novel ratiometric fluorescent design, which is cost-effective, simple to prepare and easy-to-use without chemical modification or fluorescence labeling.



中文翻译:

使用Tb 3+掺杂的碳点/ DNA共轭物的自校准逻辑系统和基于氧化酶的生物传感器

以柠檬酸铵为碳源,以Tb 3+为掺杂剂,以简便的水热法制备了掺有Tb 3+的碳点(Tb 3+ @CDs)。引入15 bp的富含GT的单链DNA(ssDNA),通过天线效应使Tb 3+敏感,从而产生两个荧光信号(CDs和Tb 3+),形成Tb 3+ @ CDs / ssDNA的结合物。Tb 3+ @ CDs / ssDNA的比例荧光可以被Ag +和Cys可逆调节,其中Tb 3+的荧光峰位于546 nm可以将CD的444 nm处的荧光峰保持恒定作为内置参考,而可以将其切换为“开”或“关”作为信号指示符。Tb 3+ @ CDs / ssDNA中建议的Ag + / Cys介导的可逆荧光变化也被证明可用于自校准比例荧光逻辑系统的设计。通过与H 2 O 2和Cys之间的特异性反应整合,将Tb 3+ @ CDs / ssDNA用于H 2 O 2的比例荧光检测。更重要的是,传感策略可以进一步成功地扩展到H 2 O 2的监视产生的氧化酶相关反应,例如GOx生物催化的葡萄糖氧化(检测极限:0.06μM),与市售试剂盒相比,在大鼠血清中得到了很好的应用。这项工作揭示了一种新颖的比例荧光设计,该设计经济高效,易于制备且易于使用,无需化学修饰或荧光标记。

更新日期:2018-08-14
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