Construction of oxygen vacancy on Bi12O17Cl2 nanosheets by heat-treatment in H2O vapor for photocatalytic NO oxidation

doi:10.1016/j.jmst.2022.02.018

Abstract

Abstract:

Oxygen-vacancies (OVs) play significant roles in semiconductor-based photocatalysis, such as elevating light absorption property, photogenerated carries separation efficiency, molecular activation, and photocatalytic activity. However, heat-treatment of semiconductors in dangerous H₂ atmosphere is usually indispensable for OVs formation. In this work, C-doped Bi₁₂O₁₇C_l2 nanosheets were facially heat-treated in H₂O vapor (∼2.3 vol%) mixed with Ar at 300 °C to in-situ introduce OVs by the proposed reactions of C(s) + H₂O(g) → CO(g) + H₂(g) and H₂(g) + O_Lattice → H₂O(g) + OV. The formation of OVs, which was confirmed by electron paramagnetic resonance (EPR), can narrow the band gap, and enhance the photogenerated e^-/h⁺ separation efficiency on Bi₁₂O₁₇C_l2. Moreover, OVs-rich Bi₁₂O₁₇C_l2 nanosheets can facilitate molecular O₂ activation and produce more reactive oxygen species (ROS), especially ¹O₂, which greatly improve the NO to NO₃^- conversion efficiency with NO removal rate of ∼63% and NO₃^- production selectivity of ∼92.6 %. The present work will bring new insights into the construction and roles of OVs in semiconductor-based photocatalysis.

Key words: Oxygen-vacancies, H₂O vapor, Photocatalytic, NO oxidation, ¹O₂

Yi Yang, Yi Zeng, Tongxin Jin, Xiaohu Zhang, Huailong Teng, Shengyao Wang, Hao Chen. Construction of oxygen vacancy on Bi₁₂O₁₇C_l2 nanosheets by heat-treatment in H₂O vapor for photocatalytic NO oxidation[J]. J. Mater. Sci. Technol., 2022, 123: 234-242.

Figures/Tables 11

Scheme 1. Illustration of procedure of Bi12O17Cl2- H2O nanosheets preparation.

Fig. 1. Wide angle XRD patterns (a) and high-resolution XRD peaks around 30 degree region (b) of C-Bi12O17Cl2 and Bi12O17Cl2-H2O.

Fig. 2. TEM images of (a) C-Bi12O17Cl2 and (b) Bi12O17Cl2-H2O; AFM images of (c) C-Bi12O17Cl2 and (d) Bi12O17Cl2-H2O; (e) HRTEM of Bi12O17Cl2-H2O; (f) element mapping of Bi12O17Cl2-H2O.

Fig. 3. (a) EPR spectra of oxygen vacancies; (b) survey XPS spectra; high-resolution XPS spectra of (c) C 1s, (d) O 1s, (d) Bi 4f and (e) Cl 2p for C-Bi12O17Cl2 and Bi12O17Cl2-H2O.

Fig. 4. Comparison of NO removal ratio (a) and residual amount of NO2 (b) during photocatalysis experiments for BiOCl-control, C-Bi12O17Cl2, Bi12O17Cl2-Ar and Bi12O17Cl2-H2O.

Fig. 5. Long-term performance of Bi12O17Cl2-H2O for photocatalytic NO oxidation.

Fig. 6. Diffuse reflectance ultraviolet-visible spectra with the inset of (αhν)1/2 versus photon energy (hν) (a), photocurrent tests (b), EIS (c) and steady state photoluminescence (PL) spectra (d) of C-Bi12O17Cl2 and Bi12O17Cl2-H2O.

Fig. 7. Influence of series of scavengers on the photocatalytic NO removal ratio (a) NO2 residual amount (b) and NO2 residual ratio calculated according to Eq. (1) (c) of Bi12O17Cl2-H2O.

Fig. 8. EPR signal of DMPO-·O2- (a) and TEP-1O2 (b) for C-Bi12O17Cl2 and Bi12O17Cl2-H2O. Influence of SOD on TMP-1O2 (c) for both catalysts.

Fig. 9. In situ DRIFTS spectra of NO and O2 interaction with Bi12O17Cl2-H2O under dark (a) and light irradiation (b).

Fig. 10. The supposed steps of photocatalytic NO removal on Bi12O17Cl2-H2O.

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Construction of oxygen vacancy on Bi₁₂O₁₇C_l2 nanosheets by heat-treatment in H₂O vapor for photocatalytic NO oxidation

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