Rationally designed Ta3N5/BiOCl S-scheme heterojunction with oxygen vacancies for elimination of tetracycline antibiotic and Cr(VI): Performance, toxicity evaluation and mechanism insight

doi:10.1016/j.jmst.2022.02.012

Abstract

Abstract:

S-scheme heterojunction photocatalysts have been the “stars” in the field of photocatalysis. Herein, a novel S-scheme heterojunction of Ta₃N₅/BiOCl with oxygen vacancies (OVs) was fabricated via a facile method. The charge separation and transport mechanism of this Ta₃N₅/BiOCl S-scheme heterojunction was verified by the analyses of band energy structures, active species, photoelectric behaviors and DFT theoretical calculation. Compared with Ta₃N₅ and BiOCl, the Ta₃N₅/BiOCl unveils substantially upgraded photocatalytic property under visible light, and the photocatalytic efficiency for removal of tetracycline (TC) and hexavalent chromium (Cr(VI)) reaches 89.6% and 91.6%, respectively. The substantial enhancement of the photocatalytic activity is attributed to the synergistic effect of the S-scheme hetero-structure and oxygen vacancies, which improves the visible-light absorption, while promoting the spatial separation of charge carriers with the optimum redox capacity, thereby boosting the production of active species for catalytic reactions. The TC degradation pathway is deduced and the toxicity evolution of TC is appraised using the QSAR method. In a nutshell, this work gives a deep understanding of the photocatalytic mechanism based on Ta₃N₅/BiOCl as well as presents a newfangled thought for developing highly efficient S-scheme heterojunction photocatalysts for water decontamination.

Key words: Ta₃N₅/BiOCl, S-scheme heterojunction, Oxygen vacancy, Visible-light photocatalysis, Antibiotic degradation, Cr(VI) reduction

Shijie Li, Mingjie Cai, Chunchun Wang, Yanping Liu, Neng Li, Peng Zhang, Xin Li. Rationally designed Ta₃N₅/BiOCl S-scheme heterojunction with oxygen vacancies for elimination of tetracycline antibiotic and Cr(VI): Performance, toxicity evaluation and mechanism insight[J]. J. Mater. Sci. Technol., 2022, 123: 177-190.

Figures/Tables 13

Fig. 1. Schematic illustration for the construction of Ta3N5/BiOCl with oxygen vacancies (TN/BOC) S-scheme heterojunctions.

Fig. 2. XRD patterns of BOC, TN, and TN/BOC (TN/BOC-1, 2, 3) heterojunctions.

Fig. 3. SEM images of BOC (a, b); SEM images (c, d), TEM image (e, f), HRTEM image (g), and the corresponding EDS elemental maps (h) of TN/BOC-2.

Fig. 4. XPS spectra of BiOCl, Ta3N5, and TN/BOC-2: (a) survey, (b) Ta 4f, (c) N 1 s, (d) Bi 4f, (e) Cl 2p, (f) O 1 s.

Fig. 5. EPR spectra of BOC and TN/BOC-2.

Fig. 6. (a) Photocatalytic removal curves of TC and (b) the corresponding reaction kinetic constants over various catalysts under visible light; Effects of catalyst dose (c), co-existing ions (C = 0.05 M) (d), HA concentrations (e), and water matrix (f) on the TC removal by TN/BOC-2; (g) TOC removal performances by BOC and TN/BOC-2; (h) The cycle tests of TN/BOC-2; (i) TC removal performance under different scavengers.

Fig. 7. (a) Possible degradation routes of TC over TN/BOC-2, (b) Fathead minnow LC50 (96 h), (c) developmental toxicity, and (d) mutagenicity of TC and the decomposition intermediates.

Fig. 8. (a) Photocatalytic removal curves of Cr(VI) and (b) the corresponding kinetic data over various catalysts under visible light; (c) The cycle experiments of TN/BOC-2 for Cr(VI) removal; (d) Cr(VI) removal performance under different scavengers.

Fig. 9. N2 adsorption-desorption isotherms of as-prepared BOC and TN/BOC heterojunctions.

Fig. 10. (a) Transient photo-current responses (TPR), and (b) electrochemical impedance spectroscopy (EIS) Nyquist plots of BOC, TN, and TN/BOC heterojunctions; (c) Steady-state PL emission spectra of BOC and TN/BOC heterojunctions; (d) Time-resolved PL (TRPL) spectra of BOC and TN/BOC-2.

Fig. 11. (a) UV?Vis DRS of BOC, TN, TN/BOC-1, TN/BOC-2, and TN/BOC-3; Tauc curves (b, c) and Mott-Schottky plots (d, e) of BOC and TN; (f) The possible band alignment of BOC and TN.

Fig. 12. The electrostatic potentials of BOC (a), and TN (b); ESR spectra of BOC, TN, and TN/BOC-2 under visible-light irradiation for 5 min: (c) DMPO-•O2- and (d) DMPO-•OH.

Fig. 13. Proposed mechanism and interfacial charge transfer for the photocatalytic removal of TC and Cr(VI) over the TN/BOC S-scheme heterojunction under visible light.

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Rationally designed Ta₃N₅/BiOCl S-scheme heterojunction with oxygen vacancies for elimination of tetracycline antibiotic and Cr(VI): Performance, toxicity evaluation and mechanism insight

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