Improved mercury ions (Hg2+) detection by composite silver nanoparticles (AgNPs) and nitrogen - Sulfur co-doped carbon dots (N, S-CDs)

Sriati Wahyudi , Japar Abdul Aziz , Ferry Faizal , Ayi Bahtiar
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Abstract

Heteroatom doping has been demonstrated as an efficient method to increase the fluorescence quantum yield efficiency of carbon dots. Co-doping with heteroatoms leads to additional active sites on carbon dots, both extending their use in sensing systems and improving the sensitivity of detection. In this study, the synthesis of nitrogen and sulfur co-doped carbon dots (N, S-CDs) through a single step hydrothermal process was reported, utilizing citric acid and thiourea as sources of carbon, nitrogen, respectively. This N, S-CDs was composited with silver nanoparticles (AgNPs) to detect mercury ions (Hg2+) with reabsorption principle. The fluorescence intensity of the carbon dots was vanished by AgNPs due to the reabsorption effect due to overlap between emission spectrum of N, S-CDs and absorption spectrum of AgNPs, and it is recovered by the addition of Hg2+ due to formation Ag/Hg amalgam. As a result, composite of N, S-CDs-AgNPs can be used as a fluorescence "turn-on" probe for rapid and highly sensitive detection of Hg2+. The lowest limit of detection (LOD) of Hg2+ is 10 nM with linear detection in the range of 1 nM - 1.0 μM. This LOD is improved three-order of magnitude as compared to the N, S-CDs only with detection limit in 10 μM. This result proves that the composite of N, S–CDs-AgNPs is a very sensitive fluorescence probe for mercury ions detection. This work will also provide ideas for creating and building novel fluorescence probes for similar applications.

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利用复合银纳米粒子(AgNPs)和氮-硫共掺杂碳点(N,S-CDs)改进汞离子(Hg2+)检测
杂原子掺杂已被证明是提高碳点荧光量子产率效率的有效方法。杂原子的共掺杂会在碳点上形成额外的活性位点,从而扩大碳点在传感系统中的应用并提高检测灵敏度。本研究利用柠檬酸和硫脲分别作为碳源和氮源,通过一步水热法合成了氮和硫共掺杂碳点(N, S-CDs)。这种 N、S-CDs 与银纳米粒子(AgNPs)复合,利用重吸收原理检测汞离子(Hg2+)。由于 N, S-CDs 的发射光谱与 AgNPs 的吸收光谱重叠,产生了重吸收效应,碳点的荧光强度被 AgNPs 消弱,而加入 Hg2+ 后,由于形成 Ag/Hg 汞齐,荧光强度又被恢复。因此,N、S-CDs-AgNPs 复合物可用作快速、高灵敏度检测 Hg2+ 的荧光 "开启 "探针。Hg2+ 的最低检测限(LOD)为 10 nM,线性检测范围为 1 nM - 1.0 μM。与检测限仅为 10 μM 的 N、S-CD 相比,这个检测限提高了三个数量级。这一结果证明,N, S-CDs-AgNPs 的复合体是一种非常灵敏的汞离子检测荧光探针。这项工作还将为创建和构建用于类似应用的新型荧光探针提供思路。
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