Noble-metal-free plasmonic MoO3‒x-based S-scheme heterojunction for photocatalytic dehydrogenation of benzyl alcohol to storable H2 fuel and benzaldehyde

doi:10.1016/S1872-2067(22)64124-X

Abstract

Abstract:

Simultaneous generation of H₂ fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy. Herein, for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol (BA) into benzaldehydes (BAD) and H₂, a novel localized surface plasmon resonance (LSPR) enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO_3-_x as oxidation semiconductor and Zn_0.1Cd_0.9S as reduction semiconductor. The photoredox system of Zn_0.1Cd_0.9S/MoO_3-_x displayed an unconventional reaction model, in which the BA served as both electron donor and acceptor. The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically. Moreover, due to the LSPR effect of MoO_3‒_x nanosheets, Zn_0.1Cd_0.9S/MoO_3‒_x photocatalysts exhibited strong absorption in the region of full solar spectrum. Therefore, the Zn_0.1Cd_0.9S/MoO_3‒_x composite generated H₂ and BAD simultaneously via selective oxidation of BA with high production (34.38 and 33.83 mmol•g^-1 for H₂ and BAD, respectively) upon full solar illumination. Even under NIR light irradiation, the H₂ production rate could up to 94.5 mmol•g^-1•h^-1. In addition, the Zn_0.1Cd_0.9S/MoO_3-_x composite displayed effective photocatalytic H₂ evolution rate up to 149.2 mmol•g^-1•h^-1 from water, which was approximate 6 times that of pure Zn_0.1Cd_0.9S. This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.

Key words: Zn_0.1Cd_0.9S/MoO_3?x S-scheme heterojunction, Localized surface plasmon resonance, Benzyl alcohol oxidation, Hydrogen generation, Full-spectrum light response

Yingcong Wei, Qiqi Zhang, Ying Zhou, Xiongfeng Ma, Lele Wang, Yanjie Wang, Rongjian Sa, Jinlin Long, Xianzhi Fu, Rusheng Yuan. Noble-metal-free plasmonic MoO_3‒_x-based S-scheme heterojunction for photocatalytic dehydrogenation of benzyl alcohol to storable H₂ fuel and benzaldehyde[J]. Chinese Journal of Catalysis, 2022, 43(10): 2665-2677.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64124-X

https://www.cjcatal.com/EN/Y2022/V43/I10/2665

Figures/Tables 13

Scheme 1. (a) Conventional reaction modes. (b) Reaction modes in this work.

Scheme 2. Schematic illustration of the synthesis for the Zn0.1Cd0.9S/MoO3?x composites.

Fig. 1. XRD patterns (a) and photocatalytic H2-production (from water) performance (b) of CdS and ZnxCd1-xS samples with visible light excitation.

Fig. 2. (a) XRD patterns of Zn0.1Cd0.9S, MoO3-x and Zn0.1Cd0.9S/MoO3?x composites. (b) XRD patterns of MoO3-x, Zn0.1Cd0.9S and 25% MO-ZnCdS samples.

Fig. 3. SEM and TEM images of MoO3-x (a,b), Zn0.1Cd0.9S (c,d), and 25% MO-ZnCdS (e,f). (g,h) TEM and HRTEM images of 25% MO-ZnCdS.

Fig. 4. XPS survey spectra (a), high-resolution XPS spectra of Zn 2p (b), Cd 3d (c) and S 2p (d) of Zn0.1Cd0.9S and 25% MO-ZnCdS samples; Mo 3d (e), O 1s (f) of MoO3-x and 25% MO-ZnCdS samples.

Fig. 5. Photocatalytic H2-generation (from water) performance (a) and production rates (b) of Zn0.1Cd0.9S and Zn0.1Cd0.9S/MoO3?x samples. (c) Cycle stability experiments of 25% MO-ZnCdS. (d) XRD of 25% MO-ZnCdS before and after cycle reaction. (e) Wavelength-dependent AQY of 25% MO-ZnCdS sample.

Fig. 6. (a) Photocatalytic dehydrogenation of BA over different catalysts. Reaction conditions: 15 mL CH3CN, 0.4 mmol benzyl alcohol, 0.2 mmol Na2CO3, 32 h reaction time. (b) BA conversion and BAD selectivity over 25% MO-ZnCdS sample. (c) Photocatalytic coproduction of H2 and BAD under different reaction time. (d) Wavelength-dependent BAD and H2 production of 25% MO-ZnCdS.

Fig. 7. Photocurrent responses (a), EIS Nyquist plots (b), LSV curves (c), steady-state PL spectra (d), and TRPL spectra (e) of Zn0.1Cd0.9S, MoO3-x and 25% MO-ZnCdS samples. The fs-TA spectra of Zn0.1Cd0.9S (f) and 25% MO-ZnCdS (g). The experimental decay kinetics for Zn0.1Cd0.9S (h) and 25% MO-ZnCdS (i).

Fig. 8. (a) UV-vis DRS of MoO3-x, Zn0.1Cd0.9S and Zn0.1Cd0.9S/MoO3?x composites. (b) Band gaps of MoO3-x and Zn0.1Cd0.9S. (c) Mott-Schottky plots a of MoO3-x and Zn0.1Cd0.9S. Calculated electrostatic potentials for MoO3-x (d) and Zn0.1Cd0.9S (e). (f) Band alignments over Zn0.1Cd0.9S-MoO3-x heterojunction.

Fig. 9. ESR spectra of TEMPO-e- (a) and DMPO-•OH (b) for 25% MO-ZnCdS. ESR spectra of TEMPO-e- (c) and DMPO-•OH (d) over Zn0.1Cd0.9S and 25% MO-ZnCdS samples.

Fig. 10. Free-energy diagrams for the dehydrogenation of benzyl alcohol into benzaldehyde and H2.

Fig. 11. (a) Type-II transfer mechanism. (b) S-scheme transfer mechanism of photocatalytic H2 production by H2O splitting under UV-visible light irradiation. Photocatalytic dehydrogenation of BA over Zn0.1Cd0.9S/MoO3?x heterojunction under UV-visible (c) and NIR (d) light irradiation.

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Noble-metal-free plasmonic MoO_3‒_x-based S-scheme heterojunction for photocatalytic dehydrogenation of benzyl alcohol to storable H₂ fuel and benzaldehyde

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