The doping of carbon quantum dots with nitrogen provides a promising direction to improve fluorescence performance and broaden their applications in sensing systems. Herein we report a one-pot solvothermal synthesis of N-doped carbon quantum dots (NCQDs) and the synthesis of a series of NCQDs with different nitrogen contents. The as-prepared NCQDs were compared with carbon quantum dots (CQDs); the introduction of nitrogen atoms largely increased the quantum yield of NCQDs and highest emission efficiency is up to 36.3 %. The fluorescence enhancement may originate from more polyaromatic structures induced by incorporated nitrogen atoms and protonation of nitrogen atoms on dots. It was found that NCQDs can act as a multifunctional fluorescence sensing platform because they can be used to detect pH values, Ag(I), and Fe(III) in aqueous solution. The fluorescence intensity of NCQDs is inversely proportional to pH values across a broad range from 5.0 to 13.5, which indicates that NCQDs can be devised as an effective pH indicator. Selective detection of Ag(I) and Fe(III) was achieved based on their distinctive fluorescence influence because Ag(I) can significantly enhance the fluorescence whereas Fe(III) can greatly quench the fluorescence. The quantitative determination of Ag(I) can be accomplished with NCQDs by using the linear relationship between fluorescence intensity of NCQDs and concentration of Ag(I). The sensitive detection of H2O2 was developed by taking advantage of the distinct quenching ability of Fe(III) and Fe(II) toward the fluorescence of NCQDs. Cellular toxicity test showed NCQDs still retain low toxicity to cells despite the introduction of a great deal of nitrogen atoms. Moreover, bioimaging experiments demonstrated that NCQDs have stronger resistance to photobleaching than CQDs and more excellent fluorescence labeling performance.
Heteroatom doping of carbon quantum dots not only enables great improvement of fluorescence efficiency and tunability of fluorescence emission, but also provides active sites in carbon dots to broaden their application in sensor. Silicon as a biocompatible element offers a promising direction for doping of carbon quantum dots. Si-doped carbon quantum dots (SiCQDs) were synthesized through a facile and effective approach. The as-prepared Si-doped carbon quantum dots possess visible fluorescence with high quantum yield up to 19.2%, owing to fluorescence enhancement effect of introduced silicon atoms into carbon dots. The toxicity test on human Hela cells showed that SiCQDs have lower cellular toxicity than common CQDs, and bioimaging experiments clearly demonstrated their excellent biolabelling ability and outstanding performance in resistance to photobleaching. Strong fluorescence quenching effect of Fe(III) on SiCQDs can be used for its selective detection among general metal ions. Specific electron transfer between SiCQDs and hydrogen peroxide enables SiCQDs as a sensitive fluorescence sensing platform for hydrogen peroxide. The subsequent fluorescence recovery induced by removal of hydrogen peroxide from SiCQDs due to formation of the stable adducts between hydrogen peroxide and melamine was taken advantage of to construct effective sensor for melamine.
Fluorescent B-doped carbon quantum dots (BCQDs) were prepared by a facile one-pot solvothermal route. The BCQDs can be used as a novel fluorescence sensing system for hydrogen peroxide and glucose detection.
A novel and efficient fluorescence sensing platform based on biocompatible graphene quantum dots and graphene oxide was established. It showed high selectivity and sensitivity for DNA detection.
P-doped carbon quantum dots (PCQDs) were synthesized by a solvent-thermal method using phosphorous tribromide and hydroquinone as precursors. The as-prepared PCQDs present strong visible fluorescence with quantum yield up to 25%. The toxicity and bioimaging experiments showed that PCQDs have low cell toxicity and excellent biolabeling ability.
A simple and efficient method to prepare halogenated carbon quantum dots (CQDs) through solvent-thermal reaction was reported. The halogenated CQDs were synthesized and further surface functionalization with diamines was achieved based on the halogenated CQDs as intermediates. The halogenated CQDs provide an alternative approach for surface modification of CQDs.
Dominant components of oxidized products of multi-walled carbon nanotubes were separated by column chromatography, the origin of highly visible fluorescence from carbon quantum dots was revealed, and the nature of weak near-UV-Vis fluorescence of oxidized carbon nanotubes from isolated sp 2 carbon clusters was supported among the four proposed explanations through experimental and theoretical approaches.It was found that three dominant components including carbon quantum dots, short and long oxidized carbon nanotubes were produced during the oxidation of carbon nanotubes. The highly visible fluorescence was mainly originated from carbon quantum dots, while short and long oxidized carbon nanotubes only exhibited weak near-UV-Vis fluorescence. For the nature of fluorescence of oxidized carbon nanotubes, two proposed explanations including defects mechanism and an isolated carbon cluster mechanism were compared and discussed through theoretical analysis of corresponding model compounds. It was supported that the fluorescence is dominantly originated from sp 2 carbon clusters isolated by sp 3 carbons due to oxidation depending on the comparison between experimental data and calculated values. The results also indicated that carbon nanotubes can be transformed to large graphene oxide during oxidation. This work not only clearly demonstrated the origin of highly visible fluorescence in an oxidized carbon nanotube mixture and a reasonable explanation for fluorescence of oxidized carbon nanotubes, but also provided an example to understand visible fluorescent graphene oxide and carbon quantum dots.
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