期刊
ACS NANO
卷 15, 期 4, 页码 6582-6593出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c09781
关键词
carbon dots; photoluminescence; diagnostics; alcohol nanosensors; phase transition
类别
资金
- Ministry of Education, Youth and Sports of the Czech Republic (ERDF/ESF Nano4Future) [CZ.02.1.01/0.0/0.0/16_019/0000754]
- Ministry of Education, Youth and Sports of the Czech Republic (Operational Programme Research, Development and Education) [CZ.02.1.01/0.0/0.0/15_003/0000416]
- Palacky University [IGA_PrF_2020_022, IGA_PrF_2020_011]
- Research Grant Council of Hong Kong SAR [CityU 11306619]
- Czech Science Foundation [19-27454X]
Highly fluorescent carbon nanoparticles known as carbon dots have attracted significant attention in research due to their simple synthesis process, non-toxic nature, and wide range of potential applications in fields such as optoelectronics and biomedicine. By studying the photoluminescence behavior of these carbon dots, researchers were able to develop a fluorescence turn-on alcohol sensor for analyzing exhaled breath condensate, which could potentially be used as a cost-effective and non-invasive diagnostic tool for early stage lung cancer screening.
Highly fluorescent carbon nanoparticles called carbon dots (CDs) have been the focus of intense research due to their simple chemical synthesis, nontoxic nature, and broad application potential including optoelectronics, photocatalysis, biomedicine, and energy-related technologies. Although a detailed elucidation of the mechanism of their photoluminescence (PL) remains an unmet challenge, the CDs exhibit robust, reproducible, and environment-sensitive PL signals, enabling us to monitor selected chemical phenomena including phase transitions or detection of ultralow concentrations of molecular species in solution. Herein, we report the PL turn-off/on behavior of aqueous CDs allowing the reversible monitoring of the water-ice phase transition. The bright PL attributable to molecular fluorophores present on the CD surface was quenched by changing the liquid aqueous environment to solid phase (ice). Based on light-induced electron paramagnetic resonance (LEPR) measurements and density functional theory (DFT) calculations, the proposed kinetic model assuming the presence of charge-separated trap states rationalized the observed sensitivity of PL lifetimes to the environment. Importantly, the PL quenching induced by freezing could be suppressed by adding a small amount of alcohols. This was attributed to a high tendency of alcohol to increase its concentration at the CD/solvent interface, as revealed by all-atom molecular dynamics simulations. Based on this behavior, a fluorescence turn-on alcohol sensor for exhaled breath condensate (EBC) analysis has been developed. This provided an easy method to detect alcohols among other common interferents in EBC with a low detection limit (100 ppm), which has a potential to become an inexpensive and noninvasive clinically useful diagnostic tool for early stage lung cancer screening.
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