Vacancy engineering mediated hollow structured ZnO/ZnS S-scheme heterojunction for highly efficient photocatalytic H2 production

doi:10.1016/S1872-2067(24)60099-9

Abstract

Abstract:

Designing a step-scheme (S-scheme) heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H₂ production activity. Herein, a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies (V_{O, Zn}-ZnO/ZnS) is rationally constructed via ion-exchange and calcination treatments. In such a photocatalytic system, the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption. Moreover, the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes, respectively, which are beneficial for promoting the photo-induced carrier separation. Meanwhile, the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity. As expected, the optimized V_{O, Zn}-ZnO/ZnS heterojunction exhibits a superior photocatalytic H₂ production rate of 160.91 mmol g^-1 h^-1, approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS, respectively. Simultaneously, the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S‐scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier. This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar‐to‐fuel energy conversion.

Key words: Hollow structure, ZnO/ZnS, S-scheme heterojunction, Vacancy engineering, Photocatalytic H₂ production

Fangxuan Liu, Bin Sun, Ziyan Liu, Yingqin Wei, Tingting Gao, Guowei Zhou. Vacancy engineering mediated hollow structured ZnO/ZnS S-scheme heterojunction for highly efficient photocatalytic H₂ production[J]. Chinese Journal of Catalysis, 2024, 64: 152-165.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60099-9

https://www.cjcatal.com/EN/Y2024/V64/I9/152

Figures/Tables 14

Scheme 1. Schematic illustration of preparation process of hollow structured VO, Zn-ZnO/ZnS.

Fig. 1. FESEM and TEM images of solid ZnO (a-c), thick-shell ZnO (d-f), and thin-shell ZnO (g-i).

Fig. 2. FSEM image (a), TEM image (b), HRTEM image (c), fast Fourier transform patterns (d), and elemental mappings (e?h) of O, S, Zn of VO, Zn-ZOS-2.

Fig. 3. XRD patterns of ZnO, ZnS, and VO, Zn-ZnO/ZnS (a), enlarged XRD patterns in 25°?31° (b), enlarged XRD patterns in 30°?38° (c). Raman spectra (d) of ZnO, ZnS and VO, Zn-ZOS-2. EPR spectra (e) of ZnO and VO, Zn-ZnO/ZnS. N2 adsorption-desorption isotherms (f) and pore size distribution curves (g) of ZnO and VO, Zn-ZnO/ZnS.

Fig. 4. XPS survey spectra of ZnO, ZnS, and VO, Zn-ZOS-2 (a). High-resolution XPS spectra of Zn 2p (b), O 1s (c), and S 2p (d) of ZnO, ZnS, and VO, Zn-ZOS-2 with and without light irradiation.

Fig. 5. UV‐vis diffuse reflectance spectra (a), Tauc plots (b), Mott-Schottky plots (c,d), VB-XPS spectra (e), and UPS (f) of as-prepared samples. The inset shows the optical images of as-prepared samples in (a).

Fig. 6. Transient photocurrent spectra (a), EIS Nyquist plots (b), SPV spectra (c), PL spectra (d), TRPL spectra (e), and LSV curves (f) of as-prepared samples.

Fig. 7. Photocatalytic H2 production (a) and photocatalytic H2 production rate (b) of as-prepared samples. (c) Comparison of the photocatalytic H2 production rate of VO, Zn-ZnO/ZnS heterojunction with other reported representative photocatalysts. AQY and UV‐vis absorption spectra (d), recycling H2 evolution tests (e), and XRD patterns (f) of VO, Zn-ZOS-2 before and after photocatalytic reaction.

Fig. 8. Schematic illustration (a) of preparation process of VO, Zn-ZOS-2 hydrogel. Photocatalytic H2 production (b) of pure hydrogel and VO, Zn-ZOS-2 hydrogel. Recycling H2 production tests (c) of VO, Zn-ZOS-2 hydrogel.

Fig. 9. The relation between photocatalytic H2 production rate and temperature of ZnO, ZnS, and VO, Zn-ZOS-2 (a) and comparison of the apparent activation energy (b).

Fig. 10. The structure models (a-c), density of states (d-f), and energy band structures (g-i) of ZnO, ZnS, and VO, Zn-ZnO/ZnS.

Fig. 11. DFT calculated electrostatic potentials of ZnO (a) and ZnS (b). Side view and top view of the charge density difference (c-e) and planar-averaged charge density difference (f) of VO, Zn-ZnO/ZnS. The yellow area and blue area represent the electrons accumulation and depletion, respectively.

Fig. 12. ESR spectra of DMPO-?OH (a) and DMPO-?O2- (b) of ZnO, ZnS, and VO, Zn-ZOS-2 under light illumination. Schematic illustration of S-scheme charge transfer mechanism of VO, Zn-ZnO/ZnS heterojunction: before contact (c), after contact (d), and light irradiation (e).

Scheme 2. Proposed photocatalytic H2 production mechanism of VO, Zn-ZnO/ZnS S-scheme heterojunction under simulated sunlight irradiation.

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Vacancy engineering mediated hollow structured ZnO/ZnS S-scheme heterojunction for highly efficient photocatalytic H₂ production

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