S-scheme CoTiO3/Cd9.51Zn0.49S10 heterostructures for visible-light driven photocatalytic CO2 reduction

doi:10.1016/j.jmst.2022.01.030

Abstract

Abstract:

Cd_1-_xZn_xS solid solutions with strong light absorption are promising materials for solar-driven CO₂ reduction; however, their relatively weak redox ability and intrinsic photo-corrosion limit their further development as a photocatalyst. The addition of a second photocatalyst with a suitable band structure to construct a S-scheme photocatalytic system can solve both problems simultaneously. Here, we report a S-scheme photocatalyst based on the heterostructure of CoTiO₃/Cd_9.51Zn_0.49S₁₀ (abbreviated as CoTiO₃/CdZnS) that enables the efficient photocatalytic reduction of CO₂. Detailed physicochemical characterization resolves the S-scheme charge transfer mechanism in this composite photocatalyst. With the well-designed structure of particles and desirable band offsets, this hybrid system offers visible light absorption in a broad spectral region, large surface area, strong redox ability, and fast carrier separation and transportation. Under visible-light illumination, the CoTiO₃/CdZnS hybrid system displays a CO formation rate of about 11 mmol h^-1 g^-1 combined with a long-term operational stability. Besides, a high apparent quantum efficiency (AQE) of 7.27% is realized for the CO₂-to-CO reduction reaction by the optimized CoTiO₃/CdZnS hybrid under 420 nm monochromatic light irradiation.

Key words: Photocatalysis, CO₂ reduction, S-scheme, Metal sulfides, Heterostructure

Bo Su, Haowei Huang, Zhengxin Ding, Maarten B.J. Roeffaers, Sibo Wang, Jinlin Long. S-scheme CoTiO₃/Cd_9.51Zn_0.49S₁₀ heterostructures for visible-light driven photocatalytic CO₂ reduction[J]. J. Mater. Sci. Technol., 2022, 124: 164-170.

Figures/Tables 5

Fig. 1. (a) Schematic illustration of the synthetic process of all CoTiO3/Cd9.51Zn0.49S10 (CoTiO3/CdZnS) heterostructures. (b, c) FESEM images, (d) TEM image, and (e) HRTEM image of CoTiO3 microprisms. (f, g) FESEM images, (h, i) TEM images, and (j) HRTEM image of heterostructures.

Fig. 2. UPS spectra of (a) CoTiO3 and (b) CdZnS. (c) DRS spectra of CoTiO3, CdZnS and 20%-CoTiO3/CdZnS and (d) Tauc plots of CoTiO3 and CdZnS. (e) Schematic illustration of the band structures for CoTiO3 and CdZnS before and after contact. (f) ESR signal intensity of DMPO-·O2- adducts of CdZnS, CoTiO3, and 20%-CoTiO3/CdZnS. Schematic illustration of the charge transfer pathway followed the S-scheme mechanism in the hybrids (inset).

Fig. 3. (a) Photocatalytic CO2 reduction activity of the different samples. (b) CO2 photoreduction performance of the system under varied conditions. (c) Wavelength-dependence of the CO2 reduction reaction. (d) Stability tests of 20%-CoTiO3/CdZnS.

Fig. 4. (a) The steady-state PL spectra, (b) TRPL decay curve fitted with multiexponential parameters and probed at 550 nm with 376 nm excitation, (c) Transient photocurrent spectra recorded by alternating dark and illumination, and (d) EIS spectra of 20%-CoTiO3/CdZnS and CdZnS.

Scheme 1. The possible reaction mechanism of photocatalytic CO2 reduction over the S-scheme CoTiO3/CdZnS heterostructure.

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S-scheme CoTiO₃/Cd_9.51Zn_0.49S₁₀ heterostructures for visible-light driven photocatalytic CO₂ reduction

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