School of Material Science & Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.
School of Material Science & Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.
Talanta. 2019 May 1;196:563-571. doi: 10.1016/j.talanta.2019.01.001. Epub 2019 Jan 3.
Element doping is recognized as a powerful way to modify surface defect structure and further enhance the fluorescence performance of graphene quantum dots (GQDs). N-doped, S-doped and S, N co-doped GQDs were synthesized to explore the influence of element doping on fluorescence sensing of dopamine (DA) biomolecules. Two interesting works are found, one is that the N-doped GQDs with urea as N source are more effective than the S-doped and S,N co-doped GQDs, characterized by the higher quantum yield (QY) up to 78% and sensitive fluorescence quenching performance to DA. The other is that the N-doped GQDs with ethylenediamine as N source have the highest QY up to 95%, however, exhibits no quenching performance to DA. This abnormal observation is discussed based on the microstructure analysis. Under the optimal reaction condition, the N-doped GQDs exhibit a dual linear relationship of quenching intensity with DA concentration in the range of 10-3000 nM and 3000-7000 nM with detection limits of 3.3 and 611 nM, respectively. The quenching mechanism of N-doped GQDs toward DA is explored from the view of N chemical states, biomolecule structure of DA homologues and redox reaction of DA.
元素掺杂被认为是一种有效的方法,可以修饰表面缺陷结构,并进一步增强石墨烯量子点(GQDs)的荧光性能。本研究通过合成 N 掺杂、S 掺杂和 S、N 共掺杂的 GQDs,探索了元素掺杂对多巴胺(DA)生物分子荧光传感的影响。研究发现了两个有趣的现象:其一,以尿素作为 N 源的 N 掺杂 GQDs 比 S 掺杂和 S、N 共掺杂 GQDs 更有效,其量子产率(QY)高达 78%,对 DA 的荧光猝灭性能更灵敏;其二,以乙二胺作为 N 源的 N 掺杂 GQDs 的 QY 最高可达 95%,但对 DA 没有猝灭性能。基于微观结构分析对这种异常现象进行了讨论。在最佳反应条件下,N 掺杂 GQDs 对 10-3000nM 和 3000-7000nM 范围内的 DA 浓度具有双重线性关系,检测限分别为 3.3 和 611nM。从 N 化学态、DA 同系物的生物分子结构和 DA 的氧化还原反应等方面探讨了 N 掺杂 GQDs 对 DA 的猝灭机制。