Unveiling product selectivity in S-scheme heterojunctions: Harnessing charge separation for tailored photocatalytic oxidation

doi:10.1016/S1872-2067(23)64610-8

Abstract

Abstract:

The utilization of semiconductor-based photocatalytic technology holds immense promise for harnessing solar energy. However, the inherent issue of strong Coulombic attraction between photo-generated electrons and holes within a single photocatalyst often leads to rapid recombination, limiting efficiency. Addressing this challenge, the development of S-scheme heterojunction photocatalysts has emerged as an effective strategy. Nevertheless, the impact of this spatial separation on the photocatalytic reaction has remained largely unexplored. This study reveals that the recombination of useless charge carriers significantly influences the oxidation product. In the pristine ZnIn₂S₄ system, the spatially unseparated holes interact with the H₂O₂ generated on the surface of ZnIn₂S₄, all of which are converted to •OH with higher oxidation ability, causing excessive oxidation of 5-hydroxymethylfurfural (HMF). Conversely, the BiOBr/ZnIn₂S₄ system, effective separation of electrons and holes in space, selectively oxidizes HMF into valuable 2,5-dimethylfuran (DFF) while efficiently generating H₂O₂ (1.15 mmol∙L^-1, 5 h). This outcome, elucidated through in-situ Fourier-transform infrared spectroscopy, density functional theory calculation, and femtosecond transient absorption spectroscopy, underscores the role of spatially separated charge carriers in influencing product selectivity within S-scheme heterojunctions. This work sheds new light on selective oxidation phenomena and underscores the significance of charge separation in S-scheme heterojunctions.

Key words: BiOBr/ZnIn₂S₄, S-scheme heterojunction, H₂O₂ production, 5-Hydroxymethylfurfural conversion, Transformation mechanism

Miaoli Gu, Yi Yang, Bei Cheng, Liuyang Zhang, Peng Xiao, Tao Chen. Unveiling product selectivity in S-scheme heterojunctions: Harnessing charge separation for tailored photocatalytic oxidation[J]. Chinese Journal of Catalysis, 2024, 59: 185-194.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64610-8

https://www.cjcatal.com/EN/Y2024/V59/I4/185

Figures/Tables 6

Fig. 1. (a) The XRD patterns of BOB, BOB/ZIS-2, and ZIS. SEM images of BiOBr (b) and BOB/ZIS-2 hybrids (c). (d) EDS mapping images of BOB/ZIS-2. (e) HRTEM images of BOB/ZIS-2.

Fig. 2. ISIXPS spectra of survey (a), Bi 4f and S 2p (b), Br 3d (c), and O 1s (d) for BOB, ZIS, and BOB/ZIS-2 (light means ultraviolet light, and dark means dark-state).

Fig. 3. 2D mapping femtosecond fs-TAS of BOB/ZIS-2 (a) and ZIS nanocrystals (b) under 330 nm laser excitation, and fs-TAS spectra signals ofBOB/ZIS-2 (c) and ZIS (d) on the fs-ns timescales. (e) Normalized decay kinetic curves of the GBS at 395 nm for as-obtained samples. (f) Schematic diagram of photogenerated carrier transfer.

Fig. 4. (a) Production of H2O2 in an O2-saturated aqueous solution of HMF under LED lamp-illumination in 5 h. (b) Photocatalytic oxidation of HMF to DFF and FDCA over as-obtained photocatalysts. Error bars for photocatalytic H2O2 performance of different batches of BOB/ZIS-2 (c) and ZIS (d).

Fig. 5. DMPO spin-trapping ESR spectra for ?O2- in methanol (a) and ?OH in water (b).

Fig. 6. In-situ DRIFTS spectra of (a,c) ZIS and (b,d) BOB/ZIS-2 adsorb HMF under the dark state and light irradiation (λ = 420 nm).

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