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Electrochemical synthesis of carbon dots with a Stokes shift of 309 nm for sensing of Fe3+ and ascorbic acid

机译:碳点的电化学合成,STOKES偏移309nm,用于感测Fe3 +和抗坏血酸

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摘要

Preparation of carbon dots (C dots) with strong emission at long wavelengths is an ongoing goal to their advanced applications, especially in bioanalysis. For sensing Fe3+ and ascorbic acid (AA), we prepared C dots with a large Stokes shift using o-phenylenediamine (OPD) as the carbon source through an electrochemical method. During the electrolysis, OPD undergoes polymerization, carbonization, and passivation at the platinum anode to form C dots. These C dots were characterized by UV-Vis spectroscopy, transmission electron microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and FT-IR spectroscopy. They are composed of C, N, O, H elements, having a maximum of emission at 570 nm and a supreme excitation at 261 nm, with a Stokes shift of 309 nm. A new emission at 350 nm emerged with their exposure to Fe3+ and the intensity rises upon increasing Fe3+, while the emission intensity at 570 nm decreases. Thus, dissimilar to the usual quenching strategy, a novel ratiometric fluorescent sensor based on the fluorescence intensity ratio (F-350/F-570) of the C dots at 350 nm and 570 nm has been developed for quantitation of Fe3+ with a limit of detection (LOD) of 0.16 mu M and high selectivity toward Fe3+ against K+, Cu2+, and Fe2+. With evidence of decreased C-N=C and C-O/N-O in XPS and increased content of C=O/N=O and N-H, we suggested the complexation of Fe3+ with the surface groups led to the changes in chemical bonds accounting for their optical property variation. Furthermore, AA can quench the fluorescence of C dots at 570 nm and Fe3+-treated C dots (incubated with 50 mu M Fe3+) at 350 nm by a static mechanism. Accordingly, two assays toward AA were developed with LODs of 0.12 mu M and 0.32 mu M by using C dots and Fe3+-treated C dots, respectively. Especially, both AA assays exhibited excellent selectivity under various substances including those with strong reducing ability such as pyrogallic acid, sodium citrate, tea polyphenol, and dithiothreitol. The applications of the assays were validated with the quantitation of Fe3+ in urine and AA in beverages. Electrochemical method is a significant approach to develop novel C dots even using the same carbon sources as in other methods.
机译:制备具有长波长强发射的碳点(C点)是其高级应用的持续目标,尤其是在生物分析中。为了检测Fe3+和抗坏血酸(AA),我们使用邻苯二胺(OPD)作为碳源,通过电化学方法制备了具有大斯托克斯位移的C点。在电解过程中,OPD在铂阳极上进行聚合、碳化和钝化,形成C点。通过紫外-可见光谱、透射电子显微镜、拉曼光谱、X射线光电子能谱(XPS)和FT-IR光谱对这些C点进行了表征。它们由C、N、O、H元素组成,最大发射波长为570 nm,最大激发波长为261 nm,斯托克斯位移为309 nm。随着Fe3+的暴露,在350nm处出现了一个新的发射,并且随着Fe3+的增加,发射强度增加,而在570nm处发射强度降低。因此,与通常的猝灭策略不同,基于C点在350 nm和570 nm处的荧光强度比(F-350/F-570),开发了一种新型比率荧光传感器,用于Fe3+的定量,检测限(LOD)为0.16μM,对Fe3+对K+、Cu2+和Fe2+具有高选择性。随着XPS中C-N=C和C-O/N-O的减少以及C=O/N=O和N-H含量的增加,我们认为Fe3+与表面基团的络合导致了化学键的变化,从而解释了其光学性质的变化。此外,AA可以通过静态机制在570nm处猝灭C点和Fe3+处理的C点(在350nm处与50μM Fe3+孵育)的荧光。因此,通过使用C点和经Fe3+处理的C点,分别以0.12μM和0.32μM的LOD开发了两种针对AA的检测方法。尤其是,这两种AA分析方法在各种物质下都表现出优异的选择性,包括具有强还原能力的物质,如焦性没食子酸、柠檬酸钠、茶多酚和二硫苏糖醇。通过尿液中Fe3+和饮料中AA的定量,验证了分析方法的应用。电化学方法是开发新型碳点的重要方法,即使使用与其他方法相同的碳源。

著录项

  • 来源
    《Dyes and Pigments》 |2021年第1期|共8页
  • 作者单位

    Cent South Univ Forestry &

    Technol Coll Food Sci &

    Engn Natl Engn Lab Deep Proc Rice &

    Byprod Changsha 410004 Hunan Peoples R China;

    Cent South Univ Forestry &

    Technol Coll Food Sci &

    Engn Natl Engn Lab Deep Proc Rice &

    Byprod Changsha 410004 Hunan Peoples R China;

    Hunan Edible Fungi Inst Changsha 410004 Peoples R China;

    Cent South Univ Forestry &

    Technol Coll Food Sci &

    Engn Natl Engn Lab Deep Proc Rice &

    Byprod Changsha 410004 Hunan Peoples R China;

    Cent South Univ Forestry &

    Technol Coll Sci Changsha 410004 Peoples R China;

    Cent South Univ Forestry &

    Technol Coll Food Sci &

    Engn Natl Engn Lab Deep Proc Rice &

    Byprod Changsha 410004 Hunan Peoples R China;

    Cent South Univ Forestry &

    Technol Coll Food Sci &

    Engn Natl Engn Lab Deep Proc Rice &

    Byprod Changsha 410004 Hunan Peoples R China;

    Cent South Univ Forestry &

    Technol Coll Food Sci &

    Engn Natl Engn Lab Deep Proc Rice &

    Byprod Changsha 410004 Hunan Peoples R China;

    Natl Taiwan Univ Dept Chem Roosevelt Rd Taipei 10617 Taiwan;

  • 收录信息
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 染料及中间体工业;颜料工业;
  • 关键词

    Carbon dot; Ratiometric sensing; Fe3+; Ascorbic acid; Stokes shift;

    机译:碳点;比率感测;Fe3 +;抗坏血酸;Stokes Shift;

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