TY - JOUR
T1 - Multicolor Phenylenediamine Carbon Dots for Metal-Ion Detection with Picomolar Sensitivity
AU - Barhum, Hani
AU - Alon, Tmiron
AU - Attrash, Mohammed
AU - Machnev, Andrey
AU - Shishkin, Ivan
AU - Ginzburg, Pavel
N1 - Publisher Copyright:
© 2021 American Chemical Society
PY - 2021/9/24
Y1 - 2021/9/24
N2 - Carbon dots keep attracting attention in multidisciplinary fields, motivating the development of new compounds. Phenylenediamine C6H4(NH2)2dots are known to exhibit colorful emission, which depends on size, composition, and the functional surface groups, forming those structures. While quite a few fabrication protocols have been developed, the quantum yield of phenylenediamine dots still does not exceed 50% owing to undesired fragment formation during carbonization. Here, we demonstrate that an ethylene glycol-based environment allows obtaining multicolor high-quantum-yield phenylenediamine carbon dots. In particular, a kinetic realization of solvothermal synthesis in acidic environments enhances carbonization reaction yield for meta phenylenediamine compounds and leads to quantum yields, exciting 60%. Reaction yield after the product’s purification approaches 90%. Furthermore, proximity of metal ions (Nd3+, Co3+, La3+) can either enhance or quench the emission, depending on the concentration. Optical monitoring of the solution allows performing an accurate detection of ions at picomolar concentrations. An atomistic model of carbon dots was developed to confirm that the functional surface group positioning within the molecular structure has a major impact on dots’ physicochemical properties. The high performance of new carbon dots paves the way toward their integration in numerous applications, including imaging, sensing, and therapeutics.
AB - Carbon dots keep attracting attention in multidisciplinary fields, motivating the development of new compounds. Phenylenediamine C6H4(NH2)2dots are known to exhibit colorful emission, which depends on size, composition, and the functional surface groups, forming those structures. While quite a few fabrication protocols have been developed, the quantum yield of phenylenediamine dots still does not exceed 50% owing to undesired fragment formation during carbonization. Here, we demonstrate that an ethylene glycol-based environment allows obtaining multicolor high-quantum-yield phenylenediamine carbon dots. In particular, a kinetic realization of solvothermal synthesis in acidic environments enhances carbonization reaction yield for meta phenylenediamine compounds and leads to quantum yields, exciting 60%. Reaction yield after the product’s purification approaches 90%. Furthermore, proximity of metal ions (Nd3+, Co3+, La3+) can either enhance or quench the emission, depending on the concentration. Optical monitoring of the solution allows performing an accurate detection of ions at picomolar concentrations. An atomistic model of carbon dots was developed to confirm that the functional surface group positioning within the molecular structure has a major impact on dots’ physicochemical properties. The high performance of new carbon dots paves the way toward their integration in numerous applications, including imaging, sensing, and therapeutics.
KW - carbonization
KW - fluorescence
KW - molecular dynamics (MD)
KW - quantum yield (QY)
KW - sensing
UR - http://www.scopus.com/inward/record.url?scp=85115764096&partnerID=8YFLogxK
U2 - 10.1021/acsanm.1c02496
DO - 10.1021/acsanm.1c02496
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C2 - 34622144
AN - SCOPUS:85115764096
SN - 2574-0970
VL - 4
SP - 9919
EP - 9931
JO - ACS Applied Nano Materials
JF - ACS Applied Nano Materials
IS - 9
ER -