1D/0D heterostructured ZnIn2S4@ZnO S-scheme photocatalysts for improved H2O2 preparation

doi:10.1016/S1872-2067(23)64514-0

Abstract

Abstract:

Solar photocatalysis is a promising, green, and sustainable technique for the synthesis of H₂O₂. In this study, low-dimensional ZnO/ZnIn₂S₄ S-scheme heterojunction photocatalysts are fabricated using electrostatic spinning and chemical bath deposition methods for the efficient photocatalytic production of H₂O₂. ZnO nanofibers loaded with 20 wt% ZnIn₂S₄ exhibit a superior H₂O₂ production rate of 928 μmol g^-1 h^-1, which is more than four times higher than that seen in pristine hexagonal phase ZnO and ZnIn₂S₄. First-principles calculations and in-situ X-ray photoelectron spectroscopy reveal the charge separation and transfer mechanisms in the S-scheme heterojunction. The construction of the S-scheme heterojunction facilitates the spatial separation of charge carriers, and electrons and holes with higher redox abilities are retained. Photoelectrochemical and photoluminescence tests further show that the formation of an S-scheme heterojunction is beneficial for the separation of photoinduced charge carriers. Electrochemical tests and electron paramagnetic resonance measurements indicate that H₂O₂ production is primarily via a two-step single-electron O₂ reduction path. This study provides a new approach for the construction of S-scheme heterojunction materials that can efficiently produce H₂O₂ under solar irradiation.

Key words: S-scheme heterojunction, Hydrogen peroxide production, Low-dimensional heterostructure, In-situ spectroscopy, Nanofiber

You Wu, Yi Yang, Miaoli Gu, Chuanbiao Bie, Haiyan Tan, Bei Cheng, Jingsan Xu. 1D/0D heterostructured ZnIn₂S₄@ZnO S-scheme photocatalysts for improved H₂O₂ preparation[J]. Chinese Journal of Catalysis, 2023, 53: 123-133.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64514-0

https://www.cjcatal.com/EN/Y2023/V53/I10/123

Figures/Tables 11

Fig. 1. Schematic diagram for the synthesis of ZnO/ZnIn2S4 heterostructures.

Fig. 2. XRD patterns of ZnO, ZnIn2S4, and heterostructures with different ratios of ZnO/ZnIn2S4.

Fig. 3. SEM images of ZnO (a) and ZZS-20 (b) nanofibers. (c) TEM images of ZZS-20. (d) HRTEM images of ZZS-20. (e) HAADF image and EDX elemental mappings of Zn, O, In, and S elements in ZZS-20.

Fig. 4. (a) The UV-vis spectra of catalysts. (b,c) Mott-Schottky plots of ZnIn2S4 and ZnO. (d) Band structures of ZnO and ZnIn2S4.

Fig. 5. ISIXPS of the survey (a), In 3d (b), O 1s (c), and S 2p (d) for ZnO, ZnIn2S4, and ZZS-20 in dark condition and under light condition.

Fig. 6. Calculated electrostatic potentials of ZnO (a) and ZnIn2S4 (b). (c) Charge density difference of ZnO/ZnIn2S4 (the yellow region signifies the accumulation layer of electrons and the cyan region is the electron depletion layer).

Fig. 7. (a) Electron transfer mechanism of ZnO/ZnIn2S4 S-scheme heterojunction. (b) Photocatalytic H2O2 evolution performance of different photocatalysts. (c) Stability cycle test of H2O2 production by ZZS-20.

Fig. 8. PL (a) and TRPL (b) spectra of ZnO, ZnIn2S4, and ZZS-20. Transient photocurrent response (c) and EIS analysis (d) of photocatalysts.

Fig. 9. LSV of ZnO (a), ZnIn2S4 (b), and ZZS-20 (c). (d) K-L curves of samples.

Fig. 10. (a) EPR spectra for ?O2? of ZnO, ZnIn2S4, and ZZS-20 in methanol. (b) EPR spectra for ?OH of ZnO, ZnIn2S4, and ZZS-20 in water.

Fig. 11. In-situ DRFTIS spectra of ZZS-20 adsorption process (a) and illumination process (λ = 365 nm) (b).

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1D/0D heterostructured ZnIn₂S₄@ZnO S-scheme photocatalysts for improved H₂O₂ preparation

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