Solvothermal fabrication of Bi2MoO6 nanocrystals with tunable oxygen vacancies and excellent photocatalytic oxidation performance in quinoline production and antibiotics degradation

doi:10.1016/S1872-2067(21)63876-7

Abstract

Abstract:

Novel Bi₂MoO₆ nanocrystals with tunable oxygen vacancies have been developed via a facile low-cost approach with the assistance of a glyoxal reductant under solvothermal conditions. With the introduction of oxygen vacancies, the optical absorption of Bi₂MoO₆ is extended and its bandgap narrowed. Oxygen vacancies not only lead to the appearance of a defect band level in the forbidden band but can also result in a minor up-shift of the valence band maximum, promoting the mobility of photogenerated holes. Moreover, oxygen vacancies can act as electron acceptors, temporarily capturing electrons excited by light and reducing the recombination of electrons and holes. At the same time, oxygen vacancies help to capture oxygen, which reacts with the captured photogenerated electrons to generate more superoxide radicals (•O₂ ^-) to participate in the reaction, thereby significantly promoting the redox performance of the photocatalyst. From Bi₂MoO₆ containing these oxygen vacancies (OVBMO), excellent photocatalytic performance has been obtained for the oxidation of 1,2,3,4-tetrahydroquinoline to produce quinoline and cause antibiotic degradation. The reaction mechanism of the oxidation of 1,2,3,4-tetrahydroquinoline to quinoline over the OVBMO materials is elucidated in terms of heterogeneous Catal. via a radical pathway.

Key words: Bi₂MoO₆ nanocrystals, Oxygen vacancies, Photocatalytic oxidation performance, Quinoline production, Antibiotics degradation

Zhen Liu, Jian Tian, Changlin Yu, Qizhe Fan, Xingqiang Liu. Solvothermal fabrication of Bi₂MoO₆ nanocrystals with tunable oxygen vacancies and excellent photocatalytic oxidation performance in quinoline production and antibiotics degradation[J]. Chinese Journal of Catalysis, 2022, 43(2): 472-484.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63876-7

https://www.cjcatal.com/EN/Y2022/V43/I2/472

Figures/Tables 15

Fig. 1. XRD patterns of the prepared samples. (a) Survey patterns of BMO and OVBMO; (b) Magnified patterns of diffraction by the (131) crystal planes of the samples.

Fig. 2. SEM images of BMO (a), 1.5-OVBMO (b), 2-OVBMO (c), and 2.5-OVBMO (d); TEM (e) and HRTEM (f) images of 2-OVBMO.

Fig. 3. FT-IR spectra of the samples. (a) Full-spectrum; (b) Enlargement of the absorption bands from 500 to 1160 cm-1; (c) Raman spectra of BMO and 2-OVBMO (inset, magnification of the spectra in the range of 720-900 cm-1).

Fig. 4. UV-vis diffuse reflectance spectra and bandgap energies (inset) of catalysts.

Table 1 Bandgap energies of samples.

Sample	Bandgap energy E_g(eV)
BMO	2.66
0.5-OVBMO	2.62
1-OVBMO	2.61
1.5-OVBMO	2.49
2-OVBMO	2.36
2.5-OVBMO	2.25

Fig. 5. XPS profiles of BMO and 2-OVBMO samples. (a) Survey spectrum; (b) Bi 4f; (c) Mo 3d; (d) O 1s.

Table 2 Specific surface areas, pore volumes, and pore diameters of the samples.

Sample	Specific surface area (m²/g)	Pore volume (cm³/g)	Average pore size (nm)
BMO	2.64	0.0181	27.43
0.5-OVBMO	12.67	0.1074	24.68
1-OVBMO	15.46	0.1031	25.16
1.5-OVBMO	16.05	0.1301	26.77
2-OVBMO	20.90	0.1519	23.71
2.5-OVBMO	20.05	0.1422	23.14

Fig. 6. Electrical tests on catalyst samples. (a) Variation in transient photocurrent densities with irradiation time; (b) Nyquist impedance plots.

Fig. 7. Mott-Schottky (MS) plots (a) and VB-XPS curves (b) of BMO and 2-OVBMO; (c) The corresponding band position of the catalysts.

Fig. 8 PL spectra (a) and curves fitted to the fluorescence decay times (b) of the BMO and 2-OVBMO samples.

Table 3 Lifetimes (τ1, τ2, τ3, and τ) obtained by fitting the time-resolved fluorescence decay spectra.

Sample	τ₁/ns	τ₂/ns	τ₃/ns	τ/ns
BMO	2.37	2.37	11.90	7.86
2-OVBMO	1.11	3.76	27.39	21.87

Fig. 9. Photocatalytic performance of BMO and OVBMO in the degradation of CPFX: (a) Adsorption performance; (b) Adsorption-photocatalytic degradation process; (c) Removal rate; (d) Recycle test on 2-OVBMO. Photocatalytic degradation of 20 ppm OTTCH (e) and 20 ppm TC (f) over BMO and OVBMO samples.

Table 4 Optimization of the reaction conditions.

Entry	Catalyst	Addition	Base	Solvent	Yield ^a,b(%)
1	2-OVBMO	TEMPO	K₂CO₃(1.0 eq)	i-PrOH	18
2	2-OVBMO	TEMPO	K₂CO₃(0.5 eq)	i-PrOH	35
3	2-OVBMO	TEMPO	none	i-PrOH	5
4	2-OVBMO	TEMPO	t-BuOK(0.5 eq)	i-PrOH	21
5	2-OVBMO	TEMPO	K₂CO₃(0.5 eq)	MeCN	n.d
6	2-OVBMO	None	K₂CO₃(0.5 eq)	i-PrOH	trace
7	2-OVBMO	TEMPO	K₂CO₃(0.5 eq)	i-PrOH	n.d ^c
8	BMO	TEMPO	K₂CO₃(0.5 eq)	i-PrOH	trace
9	none	TEMPO	K₂CO₃(0.5 eq)	i-PrOH	n.d
10	2-OVBMO	TEMPO	K₂CO₃(0.5 eq)	i-PrOH	n.d ^d

Fig. 10. ESR spectra of DMPO-•O2- (a) and DMPO-•OH (b) in water for BMO and OVBMO; (c) ESR signal at 77 K.

Fig. 11. Plausible mechanism for the dehydrogenation of 1,2,3,4-THQ to quinolone.

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Solvothermal fabrication of Bi₂MoO₆ nanocrystals with tunable oxygen vacancies and excellent photocatalytic oxidation performance in quinoline production and antibiotics degradation

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