Manipulating time-dependent size distribution of sulfur quantum dots and their fluorescence sensing for ascorbic acid.

Unlike the previous commonly used strong alkaline solvent sodium hydroxide, we employ an eco-friendly solvent, ethanol, as a solvent for the preparation of ultra-small-sized sulfur quantum dots (SQDs). Ethanol can disperse bulk sulfur and allow sufficient transfer of large-sized sulfur to smaller-sized SQDs through a one-pot synthesis approach. The SQDs obtained from ethanol as the solvent displays superior photoluminescence properties to those in water and sodium hydroxide. By delicately controlling the reaction conditions, including the amount of bulk sulfur, the reaction time, and the proportion of sulfur to oxidizing reagent, highly blue emissive SQDs with a photoluminescence quantum yield (PLQY) of 7.04% with ultra-high stability for several months can be successfully prepared. Furthermore, we found out that the SQDs display a dynamic photoluminescence properties and varied particle sizes as the reaction time increases, which is possibly realized via the etching-aggregation process. Morevoer, the fluorescence of SQDs-72 can be effectively quenched by CoOOH nanosheets and recovered upon addition of ascorbic acid (AA) by consuming CoOOH nanosheets through the redox reaction, leading to fluorescence recovery. Therefore, a fluorescence "off-on" nanosensor for the detection of AA with a limit of detection (LOD) of 0.85 µM was constructed.

One-step synthesis of nitrogen-doped multi-emission carbon dots and their fluorescent sensing in HClO and cellular imaging.

Tunable multicolor carbon dots (CDs) with a quantum yield reach up to 35% were generated directly from rhodamine and urea via one-step hydrothermal approach and purified through silica gel column chromatography. Transmission electron microscopy images reveal that the as-prepared CDs possess a small size distribution below 10 nm with bright blue, green, and yellow color emission, designated as b-CDs, g-CDs, and y-CDs, respectively. The in-depth investigations reveal that the multicolor emission CDs with different fraction displays fluorescence emission wavelength ranges from 398 nm (b-CDs), 525 nm (g-CDs), to 553 nm (y-CDs) which could be well modulated by controlling the amount of heteroatom nitrogen especially amino nitrogen onto their surface structures. Further experiments verify the important role of nitrogen content by using rhodamine solely or substituting urea with sulfur containing compounds as precursors to produce corresponding CDs since the performance is lower than that of urea incorporation. Theoretical calculation results also reveal that the increasing amount of amino nitrogen into their surface structures of b-CDs, g-CDs to y-CDs is responsible for reduced band gaps energy, which result in the redshifted wavelength. Benefiting from the excellent photoluminescence properties, wide pH variation range, high photo stability, and low toxicity, these CDs were employed for HClO sensing at 553 nm within the range 5 to 140 µM with a limit of detection (LOD) of 0.27 ± 0.025 µM (n = 3) and multicolor cellular imaging in HeLa cells. Tunable multicolor carbon dots (CDs) were generated directly from rhodamine and urea via one-step hydrothermal approach and purified through silica gel column chromatography. The as-prepared CDs exhibit bright blue, green, and yellow color emission which could be well modulated by controlling the increasing incorporation of heteroatom nitrogen especially amino nitrogen into their surface structures. These CDs were employed for HClO sensing and demonstrated to multicolor cellular imaging in HeLa cells.

Nitrogen-doped graphene quantum dots prepared by electrolysis of nitrogen-doped nanomesh graphene for the fluorometric determination of ferric ions.

Nitrogen-doped graphene quantum dots (N-GQDs) were synthesized by direct electrolysis of a carbon cloth electrode coated with nitrogen-doped nanomesh graphene (NG) in high yield (~ 25%). The N-GQDs emit intense blue fluorescence with a quantum yield (QY) of 10% ± 3%. Meanwhile, the N-GQDs are rich in hydroxyl, carboxyl, basic pyridinic nitrogen, and nitro groups, which are conducive to strengthen the interaction between N-GQDs and Fe3+ for highly sensitive determination of Fe3+ ions. Specifically, the determination for Fe3+ was conducted at different concentrations of N-GQD solution with a wide linear range of 10-1000 µM (150 µg·mL-1) and a low detection limit of 0.19 µM (10 µg·mL-1). Moreover, the fluorescence quenching mechanism illustrated that the functional groups generated by electrochemical oxidation enhanced the interaction of N-GQDs and Fe3+, and the narrow band gap (2.83 eV) of N-GQDs accomplished electron transfer from N-GQDs to Fe3+ easily. Graphical abstract A highly conductive carbon cloth electrode coated with nitrogen-doped nanomesh graphene (NG) was developed to prepared nitrogen-doped graphene quantum dots (N-GQDs) which was endowed with a wide linear range from 10 to 1000 µM (150 µg/mL) and a low detection limit of 0.19 µM (10 µg/mL) in the determination of Fe3+.

Bionanosensor based on N-doped graphene quantum dots coupled with CoOOH nanosheets and their application for in vivo analysis of ascorbic acid.

Herein, we employ 3D nitrogen-doped porous graphene frameworks (NPG) as raw material to prepare emissive nitrogen doped graphene quantum dots (r-NGQDs) via chemical oxidation method. The as-prepared fluorescent r-NGQDs was integrated with CoOOH nanosheets to construct a sensing platform for in vivo ascorbic acid (AA) analysis. Initially, the fluorescence emission intensity of r-NGQDs was quenched by CoOOH nanosheets based on the inner filter effect (IFE). Then the quenched intensity of r-NGQDs and CoOOH nanosheets system was enlightened by addition of AA, since AA could consume CoOOH nanosheets through redox reaction, leading to the release of r-NGQDs and fluorescence restoration. Moreover, the restored fluorescence intensity of r-NGQDs is highly dependent on the concentration of AA which endows them as a quantitative analysis of AA with a limit of detection (LOD) reach up to1.85 µM (n = 3) in aqueous solution. Finally, the as constructed bionanosensor was further employed for in vivo analysis of AA in living rat brain microdialysate with basal value up to 9.4 ± 1.4 µM (n = 3).

Emissive carbon dots derived from natural liquid fuels and its biological sensing for copper ions.

Liquid fuels rich in aliphatic and aromatic carbon compounds are utilized as the carbon precursors for the production of carbon dots (CDs) for the first time. Herein we demonstrate the preparation of liquid fuels derived CDs (d-CDs and f-CDs) via chemical oxidation approach and the subsequent application for cerebral copper ions (Cu2+) sensing in rat brain microdialysate. The as-prepared CDs exhibits different morphology and photoluminescence properties depending on the different component of precursors. The luminescence of the as-prepared d-CDs can be significantly quenched upon addition of Cu2+, in which Cu2+ are trapped by the oxygen and nitrogen functional groups surrounding the emissive d-CDs. Moreover, the fluorescence intensity of d-CDs is sensitive to the concentration of Cu2+ with a linear relationship in the range of 0-4 µM, and a detection limit was estimated to be 0.039 µM. Simultaneously, we found out that the luminescent d-CDs manifests an extraordinarily high selectivity which can clearly discriminate Cu2+ from other interference species in aqueous solution and therefore substantially endows d-CDs as a fluorescent sensing platform for Cu2+. According to this nature, we employed d-CDs for the in vivo analysis of Cu2+ in the rat brain microdialysate and the measured basal level of Cu2+ was estimated to be 2.82 ±â€¯0.16 µM (n = 3) even in the presence of other metal ions, biological substances and amino acids that commonly existing in the rat brain.

Fe3O4@C Core-Shell Carbon Hybrid Materials as Magnetically Separable Adsorbents for the Removal of Dibenzothiophene in Fuels.

Herein, we demonstrate a new class of core-shell magnetic carbon hybrid materials (Fe3O4@C) for remarkable adsorptive desulfurization of dibenzothiophene (DBT), which have been successfully prepared through hydrocarbonization of glucose on the surface of Fe3O4 and the subsequent pyrolyzation process. The as-obtained Fe3O4@C retains amorphous nature of carbon shells with a large surface area and displays an increase of iron atoms as active sites under elevated pyrolyzation temperature which is favorable in the adsorption of sulfur-containing species through physical and chemical adsorption, respectively. We investigate the adsorption capacity and efficiency of Fe3O4@C as a magnetically adsorbent for the removal of DBT in model oils under various experimental conditions including the adsorbent obtained at different temperatures, the amount of adsorbents, the DBT initial concentration, the regeneration approach, as well as the interference species. Our results demonstrated that the as-obtained Fe3O4@C at 650 °C (Fe3O4@C-650) displays a remarkable estimated adsorption performance (57.5 mg DBT/g for 200 ppmw), extraordinary high desulfurization efficiency (99% for 200 ppmw), and a high selectivity for DBT compared with its derivatives. Moreover, Fe3O4@C can be recovered in a quite easy, economical, and eco-friendly manner by an external magnet after five cycles without significant weight loss, which significantly simplifies the operation procedure and favors the recycle of Fe3O4@C. Combined with the economic and eco-friendly merits, Fe3O4@C offers a new avenue to employ the magnetic carbon materials for industrial applications and provides a promising substitute for adsorptive desulfurization in view of academic, industrial, and environmental aspects.