Kinetics of nitrogen-doped carbon dot formation via hydrothermal synthesis

Abstract

Carbon dots (CDs) have attracted great attention because of their unique luminescence properties, chemical inertness, thermal stability, high water solubility, low toxicity, and ease of functionalization. Here, the kinetics of nitrogen-doped CD (N-CD) formation by hydrothermal synthesis were evaluated in an attempt to realize the rapid and efficient production of N-CDs. A series of N-CDs was synthesized using various heating rates, reaction times, reaction temperatures, and precursor concentrations. Characterization of the series of N-CDs indicated that N-CD formation is a first-order reaction with a reaction rate constant of 0.634 min⁻¹. In addition, systematic investigation revealed that synthesis temperature is a more important factor to obtain highly fluorescent N-CDs than reaction time. Citric acid amides are formed by the reaction between citric acid and urea at 130 °C and N-CDs consisting of two or three citric acid amide molecules are formed through dehydration, deammoniation and dehydrogenation of citric acid at 150 °C. By adjusting the operating conditions, N-CDs with a highest quantum yield of 39.7% could be produced at a production rate of 50 g h⁻¹ with a reaction time of 16 min. The N-CDs were then embedded in polyvinyl alcohol (PVA) nanofibers. The luminescence intensity of the N-CD–PVA composite nanofibers was more than twice that of the N-CDs in solution.