Deep insights to explain the mechanism of carbon dot formation at various reaction times using the hydrothermal technique: FT-IR, 13C-NMR, 1H-NMR, and UV-visible spectroscopic approaches

Sewara J Mohammed; Khalid M Omer; Farouq E Hawaiz

doi:10.1039/d3ra01646c

Deep insights to explain the mechanism of carbon dot formation at various reaction times using the hydrothermal technique: FT-IR, ¹³C-NMR, ¹H-NMR, and UV-visible spectroscopic approaches

RSC Adv. 2023 May 10;13(21):14340-14349. doi: 10.1039/d3ra01646c. eCollection 2023 May 9.

Authors

Sewara J Mohammed^{1

2}, Khalid M Omer¹, Farouq E Hawaiz³

Affiliations

¹ Department of Chemistry, College of Science, University of Sulaimani Qlyasan Street Sulaimani 46002 Kurdistan Regional Government Iraq Sewara.mohammed@univsul.edu.iq.
² Anesthesia Department, College of Health Sciences, Cihan University Sulaimaniya Sulaimaniya 46001 Kurdistan Region Iraq.
³ Department of Chemistry, College of Education, Salahaddin University - Hawler Erbil Kurdistan Iraq.

Abstract

A well-explained mechanism for synthesizing carbon dots (CDs) is not yet explored and is still a subject of great debate and challenge. This study used a one-step hydrothermal method to prepare highly efficient, gram-scale, excellent water solubility, and blue fluorescent nitrogen-doped carbon dots (NCDs) with the particle size average distribution of around 5 nm from 4-aminoantipyrine. The effects of varying synthesis reaction times on the structure and mechanism formation of NCDs were investigated using spectroscopic methods, namely FT-IR, ¹³C-NMR, ¹H-NMR, and UV-visible spectroscopies. The spectroscopic results indicated that increasing the reaction time affects the structure of the NCDs. As the hydrothermal synthesis reaction time is extended, the intensity of the peaks in the aromatic region decreases, and new peaks in the aliphatic and carbonyl group regions are generated, which display enhanced intensity. In addition, the photoluminescent quantum yield increases as the reaction time increases. The presence of a benzene ring in 4-aminoantipyrine is thought to contribute to the observed structural changes in NCDs. This is due to the increased noncovalent π-π stacking interactions of the aromatic ring during the carbon dot core formation. Moreover, the hydrolysis of the pyrazole ring in 4-aminoantipyrine results in polar functional groups attached to aliphatic carbons. As the reaction time prolongs, these functional groups progressively cover a larger portion of the surface of the NCDs. After 21 h of the synthesis process, the XRD spectrum of the produced NCDs illustrates a broad peak at 21.1°, indicating an amorphous turbostratic carbon phase. The d-spacing measured from the HR-TEM image is about 0.26 nm, which agrees with the (100) plane lattice of graphite carbon and confirms the purity of the NCD product with a surface covered by polar functional groups. This investigation will lead to a greater understanding of the effect of hydrothermal reaction time on the mechanism and structure of carbon dot synthesis. Moreover, it offers a simple, low-cost, and gram-scale method for creating high-quality NCDs crucial for various applications.