Uniform assembly of gold nanoparticles on S-doped g-C3N4 nanocomposite for effective conversion of 4-nitrophenol by catalytic reduction

doi:10.1016/j.jmst.2019.08.031

Abstract

Abstract:

In this work, a simple synthesis of sulfur doped graphitic carbon nitride (S-g-C₃N₄) act as a support cum stabilizers for gold nanoparticles (Au) and its was characterized by UV-vis and XRD to measure the absorbance and crystallinity, respectively. The functional group and morphology of the samples were identified using FT-IR and TEM. Finally, the Au@S-g-C₃N₄ nanocatalyst exhibits good catalytic performance and stability in the reduction of hazardous 4-nitrophenol (NP) compared to S-g-C₃N₄ using NaBH₄. Moreover, the Au@S-g-C₃N₄ nanocomposite holds a good catalytic efficiency (near 100%) achieved by within 5 min. The highest catalytic reduction of NP is due to the synergistic effect of Au nanoparticles decorated on S-g-C₃N₄. The fast electron transfer reduction mechanism was elucidated and discussed. Excellent reusability and stability of the developed nanocomposites were also observed in consecutive reduction experiments. The filtering and catalyzing device was used for the direct conversion of NP polluted water. This method can open a new avenue for the metal nanoparticles based carbon materials heterogeneous catalyst and its reduction of toxic contaminants.

Key words: Gold nanoparticles, S-doped g-C₃N₄, Catalytic reduction, 4-nitrophenol

Vellaichamy Balakumar, Hyungjoo Kim, Ji Won Ryu, Ramalingam Manivannan, Young-A Son. Uniform assembly of gold nanoparticles on S-doped g-C₃N₄ nanocomposite for effective conversion of 4-nitrophenol by catalytic reduction[J]. J. Mater. Sci. Technol., 2020, 40: 176-184.

Figures/Tables 16

Scheme 1. Schematic illustration of the synthetic procedure of Au@S-g-C3N4 nanocomposite.

Fig. 1. XRD patterns of S-g-C3N4 (black line) and Au@S-g-C3N4 nanocomposite (red line).

Fig. 2. FT-IR spectra of S-g-C3N4 (black line) and Au@S-g-C3N4 nanocomposite (red line).

Fig. 3. XPS spectra of Au@S-g-C3N4 nanocomposite: (A) the survey spectra; (B) C 1s; (C) N 1s; (D) S 2p; (E) Au 4f.

Fig. 4. UV-vis spectra of S-g-C3N4 (black line) and Au@S-g-C3N4 nanocomposite (red line).

Fig. 5. TEM images of S-g-C3N4 (A), Au@S-g-C3N4 nanocomposite (B, C) and SAED pattern of Au@S-g-C3N4 nanocomposite (D).

Fig. 6. EDS spectrum of Au@S-g-C3N4 nanocomposite and the quantitative elemental composition of the nanocomposite (the inset).

Fig. 7. (A) SEM mapping analysis of Au@S-g-C3N4 nanocomposite and corresponding elements (B) C, (C) N, (D) S and (E) Au.

Table 1 Reduction efficiency and their rate constant at various condition in 5 min with different NP concentarion.

NP concentration (mM)	Reduction (%)	Rate constant (min^-1)	Correlation co-efficient, R²
0.5	99.2	0.796	0.9938
1.0	98.6	0.751	0.9977
1.5	90.1	0.493	0.9876

Table 2 Reduction efficiency and their rate constant at various condition in 5 min with different catalyst weight.

Catalyst weight (mg)	Reduction (%)	Rate constant (min^-1)	Correlation co-efficient, R²
0.1	68.2	0.047	0.9862
0.5	98.6	0.751	0.9977
1.0	99.0	0.772	0.9984

Fig. 8. UV-vis spectra of NP (curve a) and after addition of NABH4 in NP (curve b).

Fig. 9. Photographic image of 4-nitrophenolate ions with Au@S-g-C3N4 nanocomposite at different time intervals (a) and UV-vis spectra of 4-nitrophenolate ions with Au@S-g-C3N4 nanocomposite at different time intervals (b).

Fig. 10. The plot of reduction vs. reaction time (A) and ln(C/C0) against the reaction time for reduction kinetics of NP (B).

Fig. 11. Reusability of NP catalytic reduction by Au@S-g-C3N4 nanocomposite (A) and XRD patterns of Au@S-g-C3N4 nanocomposite before and after being used for 5 cycles (B).

Scheme 2. Mechanism for the fast electron transfers reduction mechanism for the reduction of NP in the presence of Au@S-g-C3N4 nanocomposite.

Fig. 12. Digital photographs of the device of NP containing water purification (A) and UV-vis spectra of 0 min (B), 3 min (C) and 5 min (D). The insets correspond to their photographs.

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Uniform assembly of gold nanoparticles on S-doped g-C₃N₄ nanocomposite for effective conversion of 4-nitrophenol by catalytic reduction

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