Investigating S-scheme charge transfer pathways in NiS@Ta2O5 hybrid nanofibers for photocatalytic CO2 conversion

doi:10.1016/S1872-2067(23)64478-X

Abstract

Abstract:

Investigating the charge-transfer behavior of photocatalysts is important to promote the photoreduction of CO₂ into solar fuels. Therefore, in this study, hybrid Ta₂O₅ nanofibers were produced through the in situ growth of freestanding NiS nanosheets. The charge separation and CO₂ photoreduction mechanisms of these nanofibers were investigated using in situ X-ray photoelectron spectroscopy and density functional theory calculations. The results suggested that the NiS@Ta₂O₅ nanohybrids formed an S-scheme heterojunction, which promoted the efficient separation of electron-hole pairs and enhanced CO₂ photoreduction. Compared to the pristine Ta₂O₅ nanofibers, the hybrid nanofibers exhibited a significantly higher CO₂-reduction rate (43.27 μmol g^-1 h^-1 for CO; 6.56 μmol g^-1 h^-1 for CH₄). In situ diffuse reflectance infrared Fourier-transform spectroscopy results confirmed the process of CO₂ hydrogenation and S-scheme charge transfer pathways in NiS@Ta₂O₅ nanohybrids.

Key words: Ta₂O₅ nanofiber, Heterojunction, CO₂ photoreduction, Charge separation, S-Scheme mechanism

Xiuli Shao, Ke Li, Jingping Li, Qiang Cheng, Guohong Wang, Kai Wang. Investigating S-scheme charge transfer pathways in NiS@Ta₂O₅ hybrid nanofibers for photocatalytic CO₂ conversion[J]. Chinese Journal of Catalysis, 2023, 51: 193-203.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64478-X

https://www.cjcatal.com/EN/Y2023/V51/I8/193

Figures/Tables 9

Fig. 1. (a) Schematic for the preparation of NiS@Ta2O5 hybrid nanofibers. TEM image of (b) Ta2O5, (c) Ni(OH)2@Ta2O5 and (d) NiS@Ta2O5 hybrid nanofibers. (e) HRTEM and (f) HAADF-STEM images of 20NSTO composites and EDX mapping images of Ta, O, Ni, and S elements.

Fig. 2. PXRD patterns (a), Raman spectra (b), N2 adsorption-desorption isotherms (c), and CO2 adsorption isotherms (d) of as-prepared samples.

Fig. 3. XPS spectra of Ta 4f (a) and O 1s (b) of Ta2O5 and 20NSTO. XPS spectra of Ni 2p (c) and S 2p (d) of NiS and 20NSTO.

Fig. 4. (a) UV-vis diffuse reflectance spectra of Ta2O5, NiS, 10NSTO, 20NSTO, and 50NSTO. Tauc plots (b), VB-XPS spectra (c) and band structure (d) of Ta2O5 nanofibers and NiS nanosheets.

Fig. 5. PL (a), TRPL(b) spectra, Transient photocurrent (c), EIS Nyquist plots (d), SPV spectra (e) and LSV curves (f) of as-prepared samples.

Fig. 6. Time-dependent CH4 (a) and CO (b) production rate over as-prepared samples. Control experiments (c) and the photocatalytic cycle performance (d) of 20NSTO.

Fig. 7. CO2-TPD (a) and CO-TPD (b) profiles of Ta2O5, NiS and 20NSTO. In situ DRIFTS measurements of Ta2O5 (c) and 20NSTO (d) under full spectrum light irradiation in pure CO2.

Fig. 8. Calculated electrostatic potentials of Ta2O5 (a) and NiS (b). Planar-averaged electron density difference ρ(z) (c) and 2D charge density difference (d) for NiS@Ta2O5 heterojunction.

Fig. 9. ESR signals of Ta2O5, NiS, and 20NSTO for (a) DMPO-superoxide radical and (b) DMPO-hydroxyl radical under irradiation for 10 min, respectively. (c) Schematic illustration of NiS@Ta2O5 heterojunction.

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Investigating S-scheme charge transfer pathways in NiS@Ta₂O₅ hybrid nanofibers for photocatalytic CO₂ conversion

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