From Coal to Carbon Quantum Dots by Chemical Oxidation: Effects of Synthesis Conditions and Coal Chemical Structure

The synthesis of carbon dots (CDs) from coal represents a promising strategy for advancing both the efficient, low-carbon utilization of coal resources and the cost-effective production of CDs. To enable the controlled, high-quality conversion of CDs from coal, a comprehensive understanding of the relationship between the coal chemical structure and the properties of CDs is crucial. This study prepared CDs from nine kinds of coal using a chemical oxidation method, and the correlations between properties of coal-based carbon dots and the original materials were revealed. The results show that the luminescence sites of coal-derived CDs are mostly distributed around 435 nm or 500 nm, where the former one relates to the confined sp2 domains and the latter one is associated with the defect structure. Coal with a volatile content of about 20–30% in the nine samples was found to produce higher CD yields, with a maximum mass yield of 19.96%, accompanied by stronger fluorescence intensity. During chemical oxidation processes, the unsaturated double bonds (C=C, C=O) and aliphatic chains firstly break, and then aromatic clusters are formed by dehydrocyclization between carbon crystallites, followed by the introduction of a C–O group. The growth of the C–O group in the CDs contributes to a stronger fluorescence property. Furthermore, strong correlations were found between the carbon skeleton structure of raw coal and photoluminescence characteristics of corresponding CDs, as reflected by Raman parameters AD1/AG, ID1/IG, and FWHMD. The findings offer significant insights into the precise modulation and control of coal-based carbon dot structures.