Photocatalytic selective oxidation of aromatic alcohols coupled with hydrogen evolution over CdS/WO3 composites

doi:10.1016/S1872-2067(21)63989-X

Abstract

Abstract:

Simultaneously utilizing photogenerated electrons and holes to convert renewable biomass and its derivatives into corresponding value-added products and hydrogen (H₂) is a promising strategy to deal with the energy and environmental crisis. Herein, we report a facile hydrothermal method to construct a direct Z-scheme CdS/WO₃ binary composite for photocatalytic coupling redox reaction, simultaneously producing H₂ and selectively converting aromatic alcohols into aromatic aldehydes in one pot. Compared with bare CdS and WO₃, the CdS/WO₃ binary composite exhibits significantly enhanced performance for this photocatalytic coupled redox reaction, which is ascribed to the extended light harvesting range, efficient charge carrier separation rate and optimized redox capability of CdS/WO₃ composite. Furthermore, the feasibility of converting various aromatic alcohols to corresponding aldehydes coupled with H₂ evolution on the CdS/WO₃ photocatalyst is proved and a reasonable reaction mechanism is proposed. It is hoped that this work can provide a new insight into the construction of direct Z-scheme photocatalysts to effectively utilize the photogenerated electrons and holes for photocatalytic coupled redox reaction.

Key words: Photocatalyst, Aromatic alcohols, Z-scheme, Composite photocatalyst, Hydrogen evolution

Yu-Lan Wu, Ming-Yu Qi, Chang-Long Tan, Zi-Rong Tang, Yi-Jun Xu. Photocatalytic selective oxidation of aromatic alcohols coupled with hydrogen evolution over CdS/WO₃ composites[J]. Chinese Journal of Catalysis, 2022, 43(7): 1851-1859.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63989-X

https://www.cjcatal.com/EN/Y2022/V43/I7/1851

Figures/Tables 6

Fig. 1. (a) Schematic diagram of the preparation process of CdS/WO3 composites. FESEM (b) and HRTEM (c) images of CdS/WO3-20 composite. (d) The magnification image of the selected area in the red circle of panel c. EDS spectrum (e) and Element mapping (f) of Cd, S, W, and O of CdS/WO3-20 composite.

Fig. 2. (a) XRD patterns of WO3, CdS and CdS/WO3; XPS spectra of Cd 3d (b), S 2p (c), W 4f (d) and O 1s (e) of the pure CdS (bottom), the pure WO3 (bottom) and CdS/WO3-20 composite(top). (f) DRS spectra of the WO3, CdS and CdS/WO3-x composites.

Fig. 3. (a) The results of photocatalytic performance tests of H2 evolution integrated with selective BA oxidation into BAD over bare WO3, bare CdS and CdS/WO3-x composites. (b) Photocatalytic cyclic tests over CdS/WO3-20 composite. Reaction conditions: 5 mg catalysts, 100 μmol BA, 10 mL H2O, full spectrum, irradiation for 2 h.

Table 1 Photocatalytic H2 evolution integrated with a series of biomass-derived alcohols oxidation.

Entry	Alcohol substrate	Yield of oxidation product (μmol)		Yield of H₂(μmol)
1	1-phenylethanol	Acetophenone	79.9	103.1
2	p-methoxybenzyl alcohol	Anisaldehyde	76.3	102.3
3	p-methylbenzyl alcohol	p-methyl benzaldehyde	67.9	95.2
4	p-fluorobenzyl alcohol	p-fluorobenzaldehyde	60.6	91.6
5	Furfuryl alcohol	Furfural	78.0	82.3
6	p-chlorobenzyl alcohol	p-chlorobenzaldehyde	43.5	87.2

Fig. 4. (a) Polarization curves of bare CdS, bare WO3 and CdS/WO3-20 composite. (b) Photocurrent density under full spectrum. (c) The EIS Nyquist plots of bare CdS, bare WO3 and CdS/WO3-20 composite. EPR spectra of DMPO-•O2- (d), DMPO-•OH (e) and EPR spectra (f) of DMPO-CH(OH)Ph over bare CdS, bare WO3 and CdS/WO3-20 composite with light irradiation.

Fig. 5. The schematic diagram of the charge transfers in CdS/WO3-20 heterojunction (left) and proposed reaction mechanism for photocatalytic BA oxidation integrated with H2 evolution over CdS/WO3 composite (right).

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Photocatalytic selective oxidation of aromatic alcohols coupled with hydrogen evolution over CdS/WO₃ composites

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