Synthesis of fluorescent carbon quantum dots from aqua mesophase pitch and their photocatalytic degradation activity of organic dyes

doi:10.1016/j.jmst.2019.03.039

Abstract

Abstract:

A synthesis strategy of fluorescent carbon quantum dots (CQDs) with high quantum yield (QY) using aqua mesophase pitch (AMP) as the carbon source has been developed via the hydrothermal method in this study. The hydrothermal temperature and soaking time have important effects on the morphology and QY of CQDs. As-prepared CQDs at 120 °C holding for 24 h (CQDs-120-24) have the uniform size of about 2.8 nm, and the QY can reach 27.6%. The obtained CQDs are successfully modified with ammonia and thionyl chloride, respectively, and they exhibit an excellent photocatalytic performance on degrading rhodamine B (Rh B), methyl blue (MB) and indigo carmine (IC). Importantly, the degradation percentage of N-CQDs on Rh B under natural light for 4 h reaches 97% with the degradation rate constant of 0.02463 min^-1 and it can maintain 93% after repetitively used 5 times. The results indicate that these as-prepared CQDs have the potential application in degrading organic dyes.

Key words: Carbon quantum dots, Aqua mesophase pitch, Photocatalytic performance, Degradation rate

Youliang Cheng, Mengsha Bai, Jian Su, Changqing Fang, Hang Li, Jing Chen, Jieming Jiao. Synthesis of fluorescent carbon quantum dots from aqua mesophase pitch and their photocatalytic degradation activity of organic dyes[J]. J. Mater. Sci. Technol., 2019, 35(8): 1515-1522.

Figures/Tables 11

Fig. 1. Synthesis of CQDs and the degradation process of the of organic dyes.

Fig. 2. TEM images and the size distribution graphics of (a) CQDs-120-24, (b) CQDs-150-48, (c) CQDs-180-48, (d) N-CQDs, (e) Cl-CQDs and (f) HRTEM image of CQDs-120-24.

Table 1 Representative synthesis, particle size and yield of CQDs in the previous reports.

Precursor	Synthetic method	Size in diameter (nm)	Yield	Refs
Dopamine	Hydrothermal at 180 °C	3.8	12%	[39]
Grass Saccharide and PEG	Hydrothermal at 180 °C Microwave (500 W)	2-22 2.75 ± 0.45	2.5%-6.2% 6.3%	[40] [41]
Glucose	Alkali or acid assisted ultrasonic	<5	7%	[42]

Fig. 3. FTIR spectra of CQDs-120-24, N-CQDs and Cl-CQDs.

Fig. 4. (a), (b), and (c) the full binding energy spectra of CQDs-120-24, N-CQDs and Cl-CQDs, respectively; (d), (e) and (f) the high resolution of the C1s spectrum for CQDs-120-24, N-CQDs and Cl-CQDs, respectively.

Fig. 5. (a) UV-vis and (c) PL spectra of CQDs derived from AMP under different conditions, (b) UV-vis and (d) PL spectra of CQDs-120-24, N-CQDs and Cl-CQDs.

Fig. 6. (a), (b) and (c) the UV-vis spectra of Rh B, MB, and IC when CQDs-120-24, N-CQDs and Cl-CQDs are added, respectively under natural light for 4 h. (a) contains the UV-vis spectra of Rh B when only hydrogen peroxide was added.

Fig. 7. (a) Time dependent UV-vis spectra of Rh B in the presence of N-CQDs, (b) the corresponding plot of ln(Ct/C0) vs. time of Rh B in the presence of N-CQDs.

Fig. 8. Photodegradation profiles of Rh B for repetitvely using 5 times as a function of reaction time using N-CQDs as the catalysts under natural light for 4 h.

Fig. 9. Schematic illustration for the catalytic degradation mechanism of CQDs on organic dyes.

Table 2 Degradation efficiency of different photocatalysts on organic dyes.

Composite	Organic dyes	Light region	Degradation efficiency	Reference
N-CQDs	Rh B	Visible Light	97%/240 min	This work
TiO₂/C	Rh B	Visible light	84%/360 min	[60]
CdS- G	Alcohol	Visible light	80%/300 min	[61]
G-ZnO	MB	UV light	80%/240 min	[62]
G-TiO₂	MB	UV light	75%/180 min	[63]

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