Organic amine surface modified one-dimensional CdSe0.8S0.2-diethylenetriamine/two-dimensional SnNb2O6 S-scheme heterojunction with promoted visible-light-driven photocatalytic CO2 reduction

doi:10.1016/S1872-2067(20)63784-6

Abstract

Abstract:

Achieving a strong redox ability and high visible-light absorption ability in a single semiconductor material is difficult. Designing a heterojunction between two semiconductor materials is a feasible method. The new step (S-scheme) heterojunction can effectively promote the separation and transfer of photogenerated electron-hole pairs and retain strong redox ability. We designed and prepared a CdSe_0.8S_0.2-diethylenetriamine (DETA)/SnNb₂O₆ heterostructure material via the solvothermal method. When CdSe_0.8S_0.2-DETA and SnNb₂O₆ form an S-scheme heterojunction, 30%CdSe_0.8S_0.2-DETA/SnNb₂O₆ exhibits the highest CO production rate (17.31 μmol·g ^-1·h ^-1), which is factors of 2.8 and 4.8 higher than that of traditional solvothermal SnNb₂O₆(6.2 μmol·g ^-1·h ^-1) and CdSe_0.8S_0.2-DETA (3.6 μmol·g ^-1·h ^-1), respectively. X-ray photoelectron spectroscopy characterization data provided evidence that the transfer pathway of space charge in the CO₂ reduction process was in accordance with the S-scheme. This research provides a simple strategy through which one can optimize the band structure to promote the separation of photogenerated carriers and achieve a high efficiency of CO₂ reduction.

Key words: Photocatalysis, CdSe_xS_1-x-DETA, SnNb₂O₆, Step-scheme, CO₂ reduction

Hui Yang, Jin feng Zhang, Kai Dai. Organic amine surface modified one-dimensional CdSe_0.8S_0.2-diethylenetriamine/two-dimensional SnNb₂O₆ S-scheme heterojunction with promoted visible-light-driven photocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2022, 43(2): 255-264.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63784-6

https://www.cjcatal.com/EN/Y2022/V43/I2/255

Figures/Tables 8

Fig. 1. Schematic of the synthesis of CdSe0.8S0.2-DETA/SnNb2O6 nanocomposite.

Fig. 2. XRD patterns of SnNb2O6 and CdSe0.8S0.2-DETA/SnNb2O6 photocatalysts.

Fig. 3. (a-c) Field emission scanning electron microscopy images of SnNb2O6, CdSe0.8S0.2-DETA, and 30%CdSe0.8S0.2-DETA/SnNb2O6; (d,e) HRTEM images of 30%CdSe0.8S0.2-DETA/SnNb2O6. (f-n) EDS elemental mapping of 30%CdSe0.8S0.2-DETA/SnNb2O6.

Fig. 4. XPS spectra of pure CdSe0.8S0.2-DETA, SnNb2O6, and 30%CdSe0.8S0.2-DETA/SnNb2O6 nanocomposite: (a) Survey spectrum; (b) O 1s; (c) Nb 3d; (d) Sn 3d; (e) Se 3d; (f) S 2p; (g) Cd 3d and N 1s.

Fig. 5. (a) UV-visible diffuse reflectance spectra of different photocatalysts. (b) Plots of (αhν)2 vs. photon energies (hν) for CdSe0.8S0.2-DETA and plots of (αhν)1/2 vs. photon energies (hν) for SnNb2O6. (c,d) Valence-band spectra of CdSe0.8S0.2-DETA and SnNb2O6.

Fig. 6. Transient photocurrent responses (a) and Nyquist plot of electrochemical impedance spectra (b) of SnNb2O6, CdSe0.8S0.2-DETA and 30%CdSe0.8S0.2-DETA/SnNb2O6 nanocomposite.

Fig. 7. (a) Photocatalytic CO2 reduction activities of different samples. (b) Stability tests of CdSe0.8S0.2-DETA, SnNb2O6, and 30%CdSe0.8S0.2-DETA/SnNb2O6 for four consecutive cycles. (c) CO2 photoreduction performance of the system under varied conditions. (d) XRD patterns of 30%CdSe0.8S0.2-DETA/SnNb2O6 before and after testing.

Fig. 8. Schematic of the charge transfer pathway of 30%CdSe0.8S0.2-DETA/SnNb2O6.

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Organic amine surface modified one-dimensional CdSe_0.8S_0.2-diethylenetriamine/two-dimensional SnNb₂O₆ S-scheme heterojunction with promoted visible-light-driven photocatalytic CO₂ reduction

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