ZnWO4-ZnIn2S4 S-scheme heterojunction for enhanced photocatalytic H2 evolution

doi:10.1016/j.jmst.2022.02.014

Abstract

Abstract:

The recombination of photogenerated electrons and holes is a crucial factor limiting photocatalytic H₂ evolution. The S-scheme ZnWO₄-ZnIn₂S₄ heterojunction with 2D coupling interfaces was successfully synthesized using a simple solvothermal method. An effective S-scheme interfacial charge migration route at the S-scheme heterogeneous interface was determined by energy band structure analyses (such as UPS, Mott-Schottky and XPS plots), which facilitates the separation of photoexcited carriers. It is worth noting that the optimal ZnWO₄-ZnIn₂S₄ composite has an H₂ evolution activity of 4925.3 μmol g^-1 h^-1 with favourable photostability and stability. Meanwhile, the ZnWO₄-ZnIn₂S₄ heterojunction exhibits the maximum optical response value (2.8 mA cm^-2) in the initial stage, effectively promoting the separation and migration of photogenerated carriers. The establishment of the built-in electric field direction at the interface can effectively promote the space charge separation between the ZnWO₄ and ZnIn₂S₄ nanosheets, which is favorable to the photocatalytic H₂ evolution. This work provides valuable guidance for designing S-scheme heterojunction photocatalysts composed of two n-type semiconductors for energy and environmental applications.

Key words: Photocatalysts, H₂ evolution, S-scheme heterojunction, Internal electric field, ZnWO₄- ZnIn₂S₄ nanosheets

Meng Dai, Zuoli He, Peng Zhang, Xin Li, Shuguang Wang. ZnWO₄-ZnIn₂S₄ S-scheme heterojunction for enhanced photocatalytic H₂ evolution[J]. J. Mater. Sci. Technol., 2022, 122: 231-242.

Figures/Tables 11

Fig. 1. XRD patterns of the as-prepared pure ZW, ZIS and ZW-ZIS photocatalysts.

Fig. 2. SEM images of (a) ZW, (b) ZIS, (c) low and (d) high magnification ZW-ZIS-40.

Fig. 3. (a) Low- and (b) high-magnification TEM images of the ZW-ZIS-40 heterojunction. (c) and (d) HRTEM images. (e) HAADF-STEM image of the ZW-ZIS-40 heterojunction with the corresponding mapping images of Zn, In, S, W and O elements. (f) and (g) SAED patterns of ZW-ZIS-40.

Fig. 4. XPS spectra of the samples: (a) survey spectra, (b) Zn 2p, (c) In 3d, (d) S 2p, (e) W 4f and (f) W 4f magnified high-resolution spectra of ZW-ZIS-40.

Fig. 5. (a) UV-vis diffuse reflectance spectra of different photocatalysts. (b) Plots of (αhv)1/2 vs (hv) of ZW, ZIS, and ZW-ZIS-40 photocatalysts.

Fig. 6. (a) and (b) Amount and rate of H2 evolution for different catalysts. (c) and (d) Cyclic stability of H2 evolution activity over ZW-ZIS-40.

Fig. 7. (a) and (b) Amount and rate of H2 evolution for different catalysts. (c) and (d) Amount and rate of H2 evolution for different molar ratios of W to Zn.

Fig. 8. (a) EIS spectra and (b) photocurrent responses of ZW, ZIS and ZW-ZIS-40.

Fig. 9. (a) and (b) DMPO spin-trapping EPR spectra of ZW, ZIS and ZW-ZIS-40 (in aqueous solutions for DMPO-·OH and methanol solution for DMPO-·O2-). (c) EPR spectra of DMPO-·OH and (d) DMPO-·O2- over ZW, ZIS, and ZW-ZIS-40 in the dark.

Fig. 10. UPS spectra of (a) ZW and (c) ZIS, binding energy of the secondary cut-off edges of (b) ZW and (d) ZI©(e) band structures of ZW and ZIS from UPS spectra.

Fig. 11. Schematic of the energy band (a) before contact, (b) after contact, and (c) specific charge transfer and the separation process between the S-scheme heterojunction of ZW-ZIS for the H2 evolution reaction.

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ZnWO₄-ZnIn₂S₄ S-scheme heterojunction for enhanced photocatalytic H₂ evolution

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