Photocatalytic CO2 conversion of W18O49/CdSe-Diethylenetriamine with high charge transfer efficiency: Synergistic effect of LSPR effect and S-scheme heterojunction

doi:10.1016/S1872-2067(21)64024-X

Abstract

Abstract:

Non-stoichiometric W₁₈O₄₉ (WO) prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies. This has great potential in the field of using sunlight to convert carbon dioxide into organic fuels. In addition, through the amination of CdSe, the one-dimensional/two-dimensional step-scheme (S-scheme) WO/CdSe-diethylenetriamine (WO/CdSe-D) photocatalyst with electron transmission channels driven by visible light to NIR light is constructed by microwave solvothermal method. The LSPR of WO and the synergistic effect of coupling semiconductors to construct S-scheme heterojunctions can improve light utilization and achieve efficient charge carrier transfer efficiency. The optimized photocatalyst of 35%WO/CdSe-D has the best CO₂ reduction performance compared to WO and CdSe-D, and the yield is 25.37 µmol h^-1 g^-1. X-ray photoelectron spectroscopy was used to verify the charge transfer path of the S-scheme WO/CdSe-D heterojunction. This work provides a possibility for the application of non-stoichiometric oxides rich in oxygen vacancies in the field of photocatalytic CO₂ reduction.

Key words: S-Scheme, Photocatalytic CO₂ reduction, W₁₈O₄₉, Localized surface plasmon resonance, Diethylenetriamine

Yue Huang, Kai Dai, Jinfeng Zhang, Graham Dawson. Photocatalytic CO₂ conversion of W₁₈O₄₉/CdSe-Diethylenetriamine with high charge transfer efficiency: Synergistic effect of LSPR effect and S-scheme heterojunction[J]. Chinese Journal of Catalysis, 2022, 43(10): 2539-2547.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64024-X

https://www.cjcatal.com/EN/Y2022/V43/I10/2539

Figures/Tables 11

Fig. 1. Schematic diagram of WO/CdSe-D compounding process.

Fig. 2. (a) XRD patterns of WO, and WO/CdSe-D. (b) XRD comparison patterns of CdSe-D and CdSe.

Fig. 3. TEM images of WO (a), CdSe-D (b) and 35%WO/CdSe-D (c). (d) HRTEM images of 35%WO/CdSe-D. SEM images of WO (e) and CdSe-D (f); TEM images of 35%WO/CdSe-D (g) and element mapping of Cd (h), O (i), Se (j) and W (k).

Fig. 4. (a) XPS full spectra of WO, CdSe-D and 35%WO/CdSe-D. High-resolution XPS of Cd 3d (b), Se 3d (c), W 4f (d) and O 1s (e).

Fig. 5. N2 adsorption-desorption isotherm curves (a) and SBET (b) of WO, CdSe-D and 35%WO/CdSe-D.

Fig. 6. (a) UV-Vis DRS of WO, CdSe-D and WO/CdSe-D. (b) plots of the (αhν)2 vs photon energy (hν) for WO and plots of the (αhν)1/2 vs. photon energy (hν) for CdSe-D; Mott-Schottky plots of (c) CdSe-D and (d) WO measured at the frequency of 2 and 3 kHz.

Fig. 7. PL spectra of WO, 35%WO/CdSe-D and CdSe-D.

Fig. 8. Transient photocurrent responses (a) and EIS (b) of CdSe-D, WO and 35%WO/CdSe-D.

Fig. 9. (a) PCR rate of CdSe-D, WO, WO/CdSe-D,WO+CdSe-D and 35% WO/CdSe; (b) Cyclic experiment results of CdSe-D, WO and WO/CdSe-D.

Fig. 10. Optimized structures of WO (100) (a) and CdSe (100) (b). Calculated Fermi energy levels and work functions of WO (100) (c) and CdSe (100) (d).

Fig. 11. Schematic diagram of the photocatalytic mechanism of the composite.

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Photocatalytic CO₂ conversion of W₁₈O₄₉/CdSe-Diethylenetriamine with high charge transfer efficiency: Synergistic effect of LSPR effect and S-scheme heterojunction

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