Chloridion-induced dual tunable fabrication of oxygen-deficient Bi2WO6 atomic layers for deep oxidation of NO

doi:10.1016/S1872-2067(20)63708-1

Abstract

Abstract:

Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion. Herein, oxygen-deficient Bi₂WO₆ atomic layers without organic residues were successfully fabricated via a facile solvothermal strategy by the multifunctional regulatory mechanism of introduced chloridion. Both DFT calculations and speciation determination revealed that chloridion displayed a more pronounced effect in the controllable synthesis of oxygen-deficient Bi₂WO₆ atomic layers without organic residues: ultrathinning and defect-engineering. This built-in multi-cooperative interface endowed Bi₂WO₆ with intriguing photoelectrochemical properties, O₂ activation ability, and ultrahigh activity in visible-light powered deep oxidation of NO. A reasonable photocatalytic mechanism was proposed based on in situ infrared spectroscopy analysis and theoretical calculations. We believe that this multi-cooperative interface engineering of oxygen-deficient Bi₂WO₆ atomic layers without organic residues could provide new insights into the design of two-dimensional (2D) layered materials with efficient active sites and pave the way for efficient NO photooxidation systems.

Key words: Oxygen vacancy, Bi₂WO₆ atomic layers, Chloridion, Photocatalysis, NO oxidation

Xianglong Yang, Shengyao Wang, Ting Chen, Nan Yang, Kai Jiang, Pei Wang, Shu Li, Xing Ding, Hao Chen. Chloridion-induced dual tunable fabrication of oxygen-deficient Bi₂WO₆ atomic layers for deep oxidation of NO[J]. Chinese Journal of Catalysis, 2021, 42(6): 1013-1023.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63708-1

https://www.cjcatal.com/EN/Y2021/V42/I6/1013

Figures/Tables 6

Fig. 1. (a) The calculated surface free energy (γ) and formation energy (ΔE) of OVs with the existence of different halogens; (b) The energy expenditure of OVs formation on Bi2WO6 {001} facet with the assistance of Cl-; (c) Schematic illustration of bottom-up solvothermal strategy to synthesis defective Bi2WO6 atomic layers with the assistance of halogens.

Fig. 2. TEM images of BWO-Cl (a) and BWO-Br (c); AFM images and the corresponding height profile of BWO-Cl (b) and BWO-Br (d); (e) ESR spectra of the samples; (f) The spin concentration and AFM-height of BWO-Cl with different dosages of KCl.

Fig. 3. Atomic-resolution HAADF-STEM images of the BWO-Cl nanosheets, the top-view (a) and the side-view (b); (c) EDS mapping of the representative BWO-Cl nanosheets; XPS spectra O 1s of BWO-H2O, BWO-None, BWO-Cl, and BWO-Br (d), Cl 2p of BWO-Cl and Br 3d of BWO-Br (e).

Table 1 The determination of Cl-, Br-, and Bi3+ in the samples after washing and digestion.

Samples		Cl (mg·g^-1)	Br (mg·g^-1)	Bi (mg·g^-1)
Washing with 1M HNO₃	BWO-H₂O	0.00	0.00	14.56
	BWO-None	0.00	0.00	14.96
	BWO-Cl	1.31	0.00	67.20
	BWO-Br	0.00	3.66	90.00
Digestion with HNO₃and H₂O₂	BWO-H₂O	0.00	0.00	530.00
	BWO-None	0.00	0.00	516.00
	BWO-Cl	12.12	0.00	352.00
	BWO-Br	0.00	19.96	384.00

Fig. 4. (a) Diffuse reflectance ultraviolet-visible spectra, (the inset is the plots of (αhν)1/2 versus photon energy (hν)); (b) schematic band diagrams of the samples; (c) Photocurrent response spectra; (d) Photocatalytic NO removal over the BWO-H2O, BWO-None, BWO-Cl, and BWO-Br; (e) Cyclic NO removal tests and (f) corresponding NO2 concentration.

Fig. 5. In situ DRIFTS spectra of NO and O2 interaction with BWO-H2O (a) and BWO-Cl (b) under visible-light irradiation; (c) Calculated reaction pathways for NO photoconversion over BWO and BWO-OVs, “*” represents adsorption on the substrate. d) Illustration of the solar-driven deep oxidation of NO.

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Chloridion-induced dual tunable fabrication of oxygen-deficient Bi₂WO₆ atomic layers for deep oxidation of NO

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