Key Laboratory of Virology & Key Laboratory of Analytical Chemistry for Biology and Medicine (MOE), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, PR China.
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Province Key Laboratory of Industrial Biotechnology, Hubei Key Laboratory of Polymer Materials, Faculty of Materials Science & Engineering, Hubei University, Wuhan 430062, PR China.
J Colloid Interface Sci. 2019 Sep 1;551:101-110. doi: 10.1016/j.jcis.2019.04.088. Epub 2019 May 4.
Carbon dots (C-dots) are superior in the aspects of excellent water solubility, good biocompatibility, environmentally friendliness and non-blinking fluorescence. In this work, highly photoluminescent small-size C-dots (QY = 18.8%, quinine sulfate as standard) with narrow size distribution (1.70 ± 0.21 nm) have been synthesized by using citric acid and triethylamine through hydrothermal method. The optimal excitation and emission wavelength of C-dots are 350 nm and 437 nm, respectively. And the prepared C-dots display excitation-independent behavior due to less surface defects and uniform size. Interestingly, the fluorescence of C-dots could be rapidly and selectively quenched by Hg within 200 s at room temperature without further modification. Under optimal conditions, the limit of detection (LOD) was measured to be nanomolar level (2.8 nM) with a linear range of 0.05-7 μM, lower than the previous published reports. Furthermore, our results reveal that static quenching mechanism was dominated in the process in which Hg coordinate with the oxygen-containing groups of C-dots to form nonfluorescent complexes. And only the addition of Hg destroyed the surface defects of C-dots resulting in the fluorescent quenching. The presence of other common interfering metal ions reported in previous literature (Ag, Cu, Fe) do not affect the surface defects, which has rarely been reported before. Besides, this sensing platform has been further successfully applied to the label free detection of Hg in tap water and living cells. These conclusions demonstrate the great potential of our C-dots in selective detection of environmental and cellular Hg, which may achieve a lot of achievements in clinical diagnosis and other biological researches.
碳点 (C-dots) 在优异的水溶性、良好的生物相容性、环境友好性和非闪烁荧光等方面具有优势。在这项工作中,通过水热法使用柠檬酸和三乙胺合成了具有窄尺寸分布 (1.70 ± 0.21nm) 的高发光小尺寸 C-dots (QY = 18.8%,以硫酸奎宁为标准)。C-dots 的最佳激发和发射波长分别为 350nm 和 437nm。并且由于表面缺陷较少且尺寸均匀,所制备的 C-dots 表现出激发独立行为。有趣的是,荧光 C-dots 的荧光可以在室温下在 200s 内被 Hg 快速且选择性地猝灭,而无需进一步修饰。在最佳条件下,检测限 (LOD) 测量值为纳摩尔级 (2.8nM),线性范围为 0.05-7µM,低于先前的报道。此外,我们的结果表明,Hg 与 C-dots 含氧基团配位形成非荧光配合物的静态猝灭机制在该过程中起主导作用。并且只有添加 Hg 才会破坏 C-dots 的表面缺陷,从而导致荧光猝灭。与之前文献中报道的其他常见干扰金属离子 (Ag、Cu、Fe) 不同,它们不会影响表面缺陷,这在以前很少有报道。此外,该传感平台已进一步成功应用于自来水和活细胞中 Hg 的无标记检测。这些结论表明我们的 C-dots 在环境和细胞 Hg 的选择性检测方面具有巨大的潜力,这可能在临床诊断和其他生物研究中取得许多成果。