Ludmerczki Robert, Malfatti Luca, Stagi Luigi, Meloni Manuela, Carbonaro Carlo Maria, Casula Maria Francesca, Bogdán Dóra, Mura Stefania, Mándity István M, Innocenzi Plinio
Department of Chemistry and Pharmacy, Laboratory of Materials Science and Nanotechnology, CR-INSTM, University of Sassari, Via Vienna 2, 07100, Sassari, Italy.
Department of Physics, University of Cagliari, sp 8, km 0.700, 09042, Monserrato, Italy.
Chemistry. 2021 Feb 1;27(7):2543-2550. doi: 10.1002/chem.202004465. Epub 2021 Jan 21.
Carbonized polymer dots (CPDs), a peculiar type of carbon dots, show extremely high quantum yields, making them very attractive nanostructures for application in optics and biophotonics. The origin of the strong photoluminescence of CPDs resides in a complicated interplay of several radiative mechanisms. To understand the correlation between CPD processing and properties, the early stage formation of carbonized polymer dots has been studied. In the synthesis, citric acid monohydrate and 2-amino-2-(hydroxymethyl)propane-1,3-diol have been thermally degraded at 180 °C. The use of an oil bath instead of a more traditional hydrothermal reactor has allowed the CPD properties to be monitored at different reactions times. Transmission electron microscopy, time-resolved photoluminescence, nuclear magnetic resonance, infrared, and Raman spectroscopy have revealed the formation of polymeric species with amide and ester bonds. Quantum chemistry calculations have been employed to investigate the origin of CPD electronic transitions. At short reaction times, amorphous C-dots with 80 % quantum yield, have been obtained.
碳化聚合物点（CPDs）是一种特殊类型的碳点，具有极高的量子产率，这使得它们成为光学和生物光子学应用中极具吸引力的纳米结构。CPDs强烈光致发光的起源在于几种辐射机制的复杂相互作用。为了理解CPD加工与性能之间的相关性，人们对碳化聚合物点的早期形成过程进行了研究。在合成过程中，一水柠檬酸和2-氨基-2-（羟甲基）丙烷-1,3-二醇在180°C下发生了热降解。使用油浴而非更传统的水热反应器，使得能够在不同反应时间监测CPD的性能。透射电子显微镜、时间分辨光致发光、核磁共振、红外和拉曼光谱揭示了具有酰胺键和酯键的聚合物物种的形成。量子化学计算被用于研究CPD电子跃迁的起源。在较短反应时间内，获得了量子产率为80%的非晶态碳点。
