Hollow dodecahedron K3PW12O40/CdS core-shell S-scheme heterojunction for photocatalytic synergistic H2 evolution and benzyl alcohol oxidation

doi:10.1016/S1872-2067(23)64507-3

Abstract

Abstract:

Simultaneous generation of clean energy, H₂, and organic products holds immense potential in the realm of photocatalysis. The S-scheme heterojunction stands out for these dual-function applications due to its robust redox capacity, facilitating both the water reduction reaction and organic oxidation reactions. In this study, a Keggin-type polymetallic oxide, H₃PW₁₂O₄₀ hollow dodecahedron (KPW), was synthesized using a hydrothermal approach. Subsequently, cadmium sulfide (CdS) nanoparticles averaging 15 nm in size were integrated in situ onto the KPW shell, resulting in the creation of a core-shell KPW@CdS S-scheme heterojunction. This optimized composite showcased a hydrogen evolution rate of 18.7 mmol g^-1 h^-1, alongside a value-added product, benzaldehyde, with a yield of 17.5 mmol g^-1 h^-1 substantially surpassing the performance of standalone CdS. This S-scheme junction, featuring a pronounced internal electronic field, emerges between the KPW and CdS. It significantly enhances the segregation of photogenerated carriers while preserving formidable redox capability. Furthermore, the hollow structure augments light absorption and utility, and the core-shell architecture delivers dual reduction and oxidation sites. As a result, the interplay between the hollow core-shell configuration and the S-scheme mode intensifies the photocatalytic activity. This research provides an innovative approach to crafting hollow S-scheme heterojunctions, aiming to optimize photocatalytic redox reactions for effective solar energy utilization.

Key words: S-scheme heterojunction, Internal electric field, Hollow core-shell structure, Polyoxometalate, Benzyl alcohol oxidation

Lijuan Sun, Xiaohui Yu, Liyong Tang, Weikang Wang, Qinqin Liu. Hollow dodecahedron K₃PW₁₂O₄₀/CdS core-shell S-scheme heterojunction for photocatalytic synergistic H₂ evolution and benzyl alcohol oxidation[J]. Chinese Journal of Catalysis, 2023, 52: 164-175.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64507-3

https://www.cjcatal.com/EN/Y2023/V52/I9/164

Figures/Tables 9

Scheme 1. Schematic of the S-scheme heterojunction for photocatalytic synergistic HER and BA oxidation reaction under ambient conditions.

Fig. 1. (a) Schematic of CSK heterojunctions preparation process. TEM images of CdS (b), KPW (c), and CSK-3 (d). HRTEM images (e) and elemental mapping (f) of CSK-3.

Fig. 2. XRD patterns (a) and FT-IR spectra (b) of CdS, KPW, and CSK-x heterojunctions. (c) XPS full spectra of different samples. XPS high-resolution spectra of Cd 3d (d), S 2p (e), K 2p (f), P 2p (g), W 4f (h), and O 1s (i) of different samples.

Fig. 3. (a) Time-caused photocatalytic H2 production activity. H2 and BAD production rates of different samples (b) and under different light wavelengths (c-f). Long-term light irradiation experiments (g) and comparison of photocatalytic HER coupled with BA oxidation reaction activity over various photocatalysts (h).

Fig. 4. Photocurrent density with and without addition of H2O2 for CdS (a), CSK-3 (b), and KPW (c). Surface charge densities (d), SPV spectra (e) and IEF intensities (f) of CdS, CSK-3, and KPW.

Fig. 5. Photocurrent (a), photocurrent decay (b), EIS curves (c), PL spectra (d), TR-PL spectra (e), and TPV spectra (f) of CdS, CSK-3, and KPW samples.

Fig. 6. DRS (a) and colors (b) of different samples. (c) Tauc plots of KPW and CdS. (d-f) VB-XPS spectra of CdS, CSK-3, and KPW samples. (g) Possible band structure over CSK-3.

Fig. 7. (a,b) In-situ XPS spectra of Cd 3d and W 4f of different samples. DMPO-·O2- (c) and DMPO-·OH (d) of different samples.

Fig. 8. Possible mechanism of the CSK-3 S-scheme heterojunction for photocatalytic synergistic H2 evolution and BA oxidation.

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Hollow dodecahedron K₃PW₁₂O₄₀/CdS core-shell S-scheme heterojunction for photocatalytic synergistic H₂ evolution and benzyl alcohol oxidation

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