Key Laboratory of Functional Molecular Engineering of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China.
Key Laboratory of Functional Molecular Engineering of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China.
Biosens Bioelectron. 2018 Jan 15;99:274-280. doi: 10.1016/j.bios.2017.07.066. Epub 2017 Jul 29.
Luminescent gold nanoclusters (AuNCs) synthesized using non-thiolate DNA ligands were reported to show both optical and structure responses toward diethyposphorthioate (DEP) derived from the hydrolysis of chlorpyrifos (CP). After incubation of AuNCs with DEP, the non-thiolate DNA ligands were immediately replaced and the tiny AuNCs with ultrasmall size transformed gradually to plasmonic nanoparticles, which resulted in significant luminescence quenching of the AuNCs, offering a new possibility to selectively detect organophosphorothioate pesticides that could be easily hydrolyzed to form the special structures such as DEP containing two binding sites (e.g. S and O atoms). Therefore, selecting CP as a model analyte, we here developed a general strategy for the construction of a novel chemosensor for the determination of CP using the non-thiolate DNA coated AuNCs as an optical probe. Based on aggregation-induced luminescence quenching, this strategy exhibited highly sensitive and selective responses towards CP with a limit of detection (LOD) of 0.50μM, and was applied successfully to the analysis of CP in real sample. More interestingly, this facile strategy could easily distinguish CP from other thiol reagents through solution color change in spite of the existence of the coordination between Au and S atom for both of them, and the response mechanisms for them were studied in detail. In additional, it could be extended to detect the other organophosphorothioate pesticides with the similar structure as CP, which exploits a new platform for the construction of chemosensor and application.
使用非硫醇 DNA 配体合成的发光金纳米团簇 (AuNCs) 被报道对来源于毒死蜱 (CP) 水解的二乙基膦酸酯 (DEP) 表现出光学和结构响应。AuNCs 与 DEP 孵育后,非硫醇 DNA 配体立即被取代,具有超小尺寸的微小 AuNCs逐渐转变为等离子体纳米颗粒,这导致 AuNCs 的荧光猝灭显著,为选择性检测容易水解形成特殊结构(如含有两个结合位点的 DEP,例如 S 和 O 原子)的有机磷硫代酸盐农药提供了新的可能性。因此,选择 CP 作为模型分析物,我们在这里开发了一种使用非硫醇 DNA 包覆的 AuNCs 作为光学探针构建新型 CP 测定化学传感器的通用策略。基于聚集诱导的荧光猝灭,该策略对 CP 表现出高灵敏度和选择性响应,检测限 (LOD) 为 0.50μM,并成功应用于实际样品中 CP 的分析。更有趣的是,尽管 Au 和 S 原子之间存在配位,这种简单的策略仍然可以通过溶液颜色变化轻松区分 CP 与其他硫醇试剂,并且详细研究了它们的响应机制。此外,它可以扩展到检测具有与 CP 相似结构的其他有机磷硫代酸盐农药,为化学传感器的构建和应用开辟了新的平台。