Hot-electron-assisted S-scheme heterojunction of tungsten oxide/graphitic carbon nitride for broad-spectrum photocatalytic H2 generation

doi:10.1016/S1872-2067(20)63753-6

Abstract

Abstract:

Extended light absorption and dynamic charge separation are vital factors that determine the effectiveness of photocatalysts. In this study, a nonmetallic plasmonic S-scheme photocatalyst was fabricated by loading 1D plasmonic W₁₈O₄₉ nanowires onto 2D g-C₃N₄ nanosheets. W₁₈O₄₉ nanowires play the dual role of a light absorption antenna—that extends light adsorption—and a hot electron donor—that assists the water reduction reaction in a wider light spectrum range. Moreover, S-scheme charge transfer resulting from the matching bandgaps of W₁₈O₄₉ and g-C₃N₄ can lead to strong redox capability and high migration speed of the photoinduced charges. Consequently, in this study, W₁₈O₄₉/g-C₃N₄ hybrids exhibited higher photocatalytic H₂ generation than that of pristine g-C₃N₄ under light irradiation of 420-550 nm. Furthermore, the H₂ production rate of the best-performing W₁₈O₄₉/g-C₃N₄ hybrid was 41.5 μmol·g^-1·h^-1 upon exposure to monochromatic light at 550 nm, whereas pure g-C₃N₄ showed negligible activity. This study promotes novel and environmentally friendly hot-electron-assisted S-scheme photocatalysts for the broad-spectrum utilization of solar light.

Key words: Graphite carbon nitride, W₁₈O₄₉, S-scheme, Photocatalytic H₂ generation, Wide spectrum

Qinqin Liu, Xudong He, Jinjun Peng, Xiaohui Yu, Hua Tang, Jun Zhang. Hot-electron-assisted S-scheme heterojunction of tungsten oxide/graphitic carbon nitride for broad-spectrum photocatalytic H₂ generation[J]. Chinese Journal of Catalysis, 2021, 42(9): 1478-1487.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63753-6

https://www.cjcatal.com/EN/Y2021/V42/I9/1478

Figures/Tables 12

Fig. 1. FT-IR spectra (a), enlarged spectra in the range of 780-840 cm-1 (b), XRD patterns (c) and enlarged XRD patterns (d) of HCN, W18O49, and W18O49/HCN composites.

Fig. 2. High-resolution XPS spectra of C 1s (a), N 1s (b), W 4f (c) and O 1s (d) of HCN, W18O49 and WOCN-3.

Fig. 3. Work functions of HCN (001) surface (b) and W18O49 (001) surface (b); the band-alignments of the HCN and W18O49 before (c) and after (d) contact.

Fig. 4. SEM and TEM images of HCN (a,d), W18O49 (b,e) and WOCN-3 (c, f); HRTEM image (g) and EDX elemental mapping (h) of WOCN-3.

Fig. 5. N2 sorption isotherm (a) and pore size distribution (b) over HCN and WOCN-3.

Fig. 6. Photocatalytic H2-production activities (a) and H2-production rates (b) of HCN, W18O49, and W18O49/HCN samples.

Fig. 7. Cycle stability experiments of WOCN-3.

Fig. 8. (a) Wavelength-dependent AQY of WOCN-3; (b) H2-production performances of HCN, W18O49, and WOCN-3 under 550 nm monochromic light irradiation.

Fig. 9. UV-vis spectra of HCN, W18O49 and the W18O49/HCN composites.

Fig. 10. Transient photocurrent responses (a) and EIS plots (b) of HCN, W18O49 and WOCN-3; PL (c) and TRPL (d) of HCN and WOCN-3.

Fig. 11. Band gaps (a), Mott-Schottky plots (b,c) and band alignments (d) over HCN and W18O49; comparison of ESR spectra of DMPO-?OH (e) and TEMPO -e- (f) over HCN, W18O49 and WOCN-3 samples.

Fig. 12. Hot electron assisted S-scheme over W18O49/HCN hybrid for photocatalytic H2-production.

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Hot-electron-assisted S-scheme heterojunction of tungsten oxide/graphitic carbon nitride for broad-spectrum photocatalytic H₂ generation

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