g-C3N4/CoTiO3 S-scheme heterojunction for enhanced visible light hydrogen production through photocatalytic pure water splitting

doi:10.1016/S1872-2067(22)64111-1

Abstract

Abstract:

Photocatalytic hydrogen (H₂) production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy. However, the realization of a photocatalytic pure water splitting system with desirable efficiency is still a huge challenge. Herein, visible light photocatalytic H₂ production from pure water splitting was successfully achieved using a g-C₃N₄/CoTiO₃ S-scheme heterojunction photocatalyst in the absence of sacrificial agents. An optimum hydrogen evolution rate of 118 μmol∙h^-1∙g^-1 was reached with the addition of 1.5 wt% CoTiO₃. The remarkably promoted hydrogen evolution rate was attributed to the intensified light absorption coupled with the synergistic effect of visible light responsive CoTiO₃, the promoted efficiency in charge separation, and the reserved strong redox capacity induced by the S-scheme charge transfer mechanism. This work provides an alternative to visible light-responding oxidation photocatalysts for the construction of S-scheme heterojunctions and high-efficiency photocatalytic systems for pure water splitting.

Key words: CoTiO₃, g-C₃N₄, Photocatalytic hydrogen evolution, Pure water splitting, S-scheme heterojunction

Aiyun Meng, Shuang Zhou, Da Wen, Peigang Han, Yaorong Su. g-C₃N₄/CoTiO₃ S-scheme heterojunction for enhanced visible light hydrogen production through photocatalytic pure water splitting[J]. Chinese Journal of Catalysis, 2022, 43(10): 2548-2557.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64111-1

https://www.cjcatal.com/EN/Y2022/V43/I10/2548

Figures/Tables 10

Fig. 1. XRD patterns of the CN, CoTiO3 (a) and CCT-x (x = 0.5, 1.5, 2, 3) (b) samples.

Fig. 2. FESEM images of CN (a), CoTiO3 (b), and CCT-1.5 (c). TEM image (d) and high-resolution transmission electron microscopy (HRTEM) image (e) of CCT-1.5; FESEM image (f) and corresponding EDS mapping images (g-k) of CCT-1.5. Scale bar of (g-k) is 10 μm.

Fig. 3. UV-Vis diffuse reflectance spectroscopy of the CN, CoTiO3, and CCT-x (x = 0.5, 1.5, 2, 3) samples.

Fig. 4. Survey (a) and high-resolution XPS spectra of C 1s (b), N 1s (c), and O 1s (d) for CN, CoTiO3, CCT-1.5, and CCT-1.5-light (CCT-1.5 under light irradiation). High-resolution XPS spectra of Ti 2p (e) and Co 2p (f) for CCT-15 and CCT-15-light.

Fig. 5. Electrostatic potentials of C3N4 (a) and CoTiO3 (110) planes (b). The blue, gray, red, light gray, and purple spheres represent N, C, O, Ti, and Co atoms, respectively. The red and blue dashed lines represent the Fermi potential and vacuum energy potential, respectively.

Fig. 6. (a) Photocatalytic H2 production rates over the CN, CoTiO3, and CCT-x (x = 0.5, 1.5, 2, 3) samples under visible light illumination (λ > 400 nm). (b) Time-dependent H2 production yields on the CN, CoTiO3, and CCT-x samples under visible light illumination (λ > 400 nm). (c) Photocatalytic H2 production rates of CCT-1.5 under different light sources (λ = 365, 400, and 475 nm, visible light with λ > 400 nm, UV-Vis light without filter). (d) Absorption intensity of H2O2 over CN, CoTiO3, and CCT-1.5 suspensions after 3 h of pure water splitting. The amount of H2O2 was measured using iodometry via UV-Vis absorption spectroscopy. Detailed measurements are shown in experimental part.

Fig. 7. (a,b) M-S curves of CN, CoTiO3, and CCT-1.5. (c) Band structure illustrations for CN and CoTiO3.

Fig. 8. EPR spectra of DMPO-•O2- in methanol (a) and DMPO-•OH in the aqueous dispersion (b) in the presence of CN, CoTiO3, and CCT-1.5.

Fig. 9. PL spectra (a) and transient photocurrent response curves (b) of the samples under visible light irradiation (λ > 400 nm).

Fig. 10. Schematic of the energy levels of CN and CoTiO3 without contact (a), with contact (b), and under irradiation (c) and the photocatalytic S-scheme reaction mechanism of CCT-1.5 under irradiation.

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g-C₃N₄/CoTiO₃ S-scheme heterojunction for enhanced visible light hydrogen production through photocatalytic pure water splitting

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