Hierarchical S-scheme heterojunctions of ZnIn2S4-decorated TiO2 for enhancing photocatalytic H2 evolution

doi:10.1016/S1872-2067(23)64633-9

Abstract

Abstract:

Photocatalytic water splitting to produce H₂ using semiconductor photocatalysts is a reliable approach to alleviating energy shortages and environmental pollution. However, the inadequate light-harvesting ability, rapid photogenerated carrier recombination, and inferior redox capacity of the individual photocatalysts restrict their photocatalytic activity. To address these limitations, a hierarchical S-scheme heterojunction of ZnIn₂S₄-nanosheet-decorated flower-like TiO₂ microspheres for enhancing photocatalytic H₂ evolution, purposely constructed through in situ chemical bath deposition, has been reported. The as-synthesized TiO₂/ZnIn₂S₄ heterojunctions exhibited ZnIn₂S₄-content-dependent photocatalytic activity for solar-driven H₂ evolution. As a result, the optimized TiO₂/ZnIn₂S₄ heterojunction exhibited a superior photocatalytic H₂ evolution rate of 6.85 mmol g^-1 h^-1, approximately 171.2- and 3.9-fold with respect to that obtained on pure TiO₂ and ZnIn₂S₄, respectively, mainly attributed to the unique hierarchical structure, extended light-harvesting ability, enhanced redox capacity, and improved separation and transfer efficiencies of the photogenerated carriers induced by the S-scheme heterojunctions. Simultaneously, a detailed analysis of the S-scheme electron transfer pathway in the TiO₂/ZnIn₂S₄ heterojunction was performed using in situ irradiated X-ray photoelectron spectroscopy and electron paramagnetic resonance spectroscopy. This study provides insights into the design of highly active heterojunction photocatalysts for sustainable solar-to-fuel energy conversion.

Key words: TiO₂, Hierarchical structure, ZnIn₂S₄, S-scheme heterojunction, Photocatalysis, H₂ evolution

Baolong Zhang, Fangxuan Liu, Bin Sun, Tingting Gao, Guowei Zhou. Hierarchical S-scheme heterojunctions of ZnIn₂S₄-decorated TiO₂ for enhancing photocatalytic H₂ evolution[J]. Chinese Journal of Catalysis, 2024, 59: 334-345.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64633-9

https://www.cjcatal.com/EN/Y2024/V59/I4/334

Figures/Tables 10

Fig. 1. Schematic diagram of synthesis process of TiO2/ZnIn2S4 (a), Zeta potentials (b) of TiO2 and ZnIn2S4, XRD patterns (c) of TiO2, ZnIn2S4, and heterojunctions with different ZnIn2S4 content, N2 adsorption-desorption isotherms (d) and pore size distribution curves (e) of TiO2, ZnIn2S4, and TZ-2.

Fig. 2. FESEM images of TiO2 (a,b) and TZ-2 (c,d). TEM images of TiO2 (e) and TZ-2 (f,g). HRTEM image (h) and elemental mappings (i-n) of Ti, O, Zn, In, and S of TZ-2. The inset shows the fast Fourier transform patterns in (h).

Fig. 3. (a) XPS survey spectra of TiO2, ZnIn2S4, and TZ-2. High-resolution XPS spectra of Ti 2p (b), O 1s (c), Zn 2p (d), In 3d (e), and S 2p (f) of TiO2, ZnIn2S4, and TZ-2 with and without light irradiation.

Fig. 4. UV-vis diffuse reflectance spectra (a), Tauc plots (b), Mott-Schottky plots (c), VB-XPS spectra (d), UPS (e), and band structure diagram (f) of as-prepared samples.

Fig. 5. Photocatalytic H2 evolution (a) and photocatalytic H2 evolution rate (b) of as-obtained samples. Photocatalytic H2 evolution rate (c) of TZ-2 with and without sacrificial agents. AQY and UV-vis absorption spectra (d) of TZ-2. Recycling H2 evolution tests (e) of TZ-2. XRD patterns (d) of TZ-2 before and after photocatalytic reaction.

Table 1 Comparison of the photocatalytic H2 evolution rate of as-prepared TiO2/ZnIn2S4 heterojunction with other reported representative photocatalysts.

Photocatalyst	Sacrificial agent	H₂evolution rate (mmol g^-1 h^-1)	Enhancement factor vs. TiO₂	Ref.
ZnIn₂S₄/TiO_2-_x	MeOH	0.84	20.0	[65]
TiO₂@NC-A/ZnIn₂S₄	TEOA	2.80	—	[66]
TiO₂@ZnIn₂S₄	Lactic acid	1.24	24.2	[67]
rGO/TiO₂/ZnIn₂S₄	Na₂S/Na₂SO₃	0.46	71.1	[68]
g-C₃N₄/TiO₂/ZnIn₂S₄ (3 wt% Pt)	MeOH	6.53	6.9	[69]
TiO₂/ZnIn₂S₄	TEOA	6.03	3.7	[42]
Ti₃C₂@TiO₂/ZnIn₂S₄	Na₂S/Na₂SO₃	1.19	—	[70]
TiO₂/ZnIn₂S₄	TEOA	6.85	171.2	This work

Fig. 6. Transient photocurrent spectra (a), EIS Nyquist plots (b), SPV spectra (c), PL spectra (d), TRPL spectra (e), and LSV curves (f) of as-prepared samples.

Fig. 7. Linear relation between photocatalytic H2 evolution rate and temperature of TiO2 (a), ZnIn2S4 (b), and TZ-2 (c). (d) Corresponding comparison of apparent activation energy.

Fig. 8. EPR spectra of DMPO-?OH (a) and DMPO-?O2- (b) over TiO2, ZnIn2S4, and TZ-2 under light illumination. Schematic diagram of S-scheme mechanism over TiO2/ZnIn2S4 heterojunction: before contact (c), after contact (d), and light irradiation (e).

Fig. 9. Proposed photocatalytic H2 evolution mechanism of TiO2/ZnIn2S4 S-scheme heterojunction under simulated sunlight irradiation.

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Hierarchical S-scheme heterojunctions of ZnIn₂S₄-decorated TiO₂ for enhancing photocatalytic H₂ evolution

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