WO3/PHI S-scheme heterojunction with photoinduced dual defects for highly selective photocatalytic CO2-to-CO conversion

doi:10.1016/S1872-2067(26)65232-1

Abstract

Abstract:

Photocatalytic CO₂ reduction, which converts solar energy into chemical energy, represents a highly promising strategy. However, conversion efficiency is often constrained by the poor adsorption and activation of CO₂ and H₂O molecules. Here, we report an oxygen and nitrogen-vacancy-enriched WO₃/poly(heptazine imide) (PHI) S-scheme heterojunction for efficient and selective CO₂ photoreduction. The optimized WO₃/PHI heterojunction delivers a CO evolution rate of 129.2 μmol g^-1 h^-1 with 96.1% selectivity, corresponding to 7.9- and 6.5-fold enhancements over pristine WO₃ and PHI, respectively. Experiments and theoretical calculations demonstrate that the in-situ formed and photoinduced dual vacancies facilitate adsorption of CO₂ and H₂O, thereby improving the efficiency of photocatalytic CO₂ reduction. The interfacial W-N bonds serve as critical channels to accelerate interfacial charge transfer across the WO₃/PHI heterojunction. The S-scheme charge-transfer pathway, in concert with a dual-defect interfacial architecture, promotes charge transport, substantially boosting CO₂ reduction performance. This work provides mechanistic insight into defect-assisted S-scheme photocatalysis and offers a rational strategy for designing efficient photocatalysts for solar fuel production.

Key words: S-scheme heterojunction, WO₃/poly(heptazine imide), Dual defect, Synergistic effect, Photocatalytic mechanism

Mengxuan Liu, Rongxin Zhang, Xin Zhang, Yanfeng Zhang. WO₃/PHI S-scheme heterojunction with photoinduced dual defects for highly selective photocatalytic CO₂-to-CO conversion[J]. Chinese Journal of Catalysis, 2027, 92: 219-236.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65232-1

https://www.cjcatal.com/EN/Y2027/V92/I1/219

Figures/Tables 14

Fig. 1. (a) Schematic illustration for synthesis of WO3/PHI. SEM micrographs of WO3 (b), PHI (c), and WO3/PHI (d). (e) HRTEM image of WO3/PHI. lattice spacing of WO3 (f) and PHI (g). EDS images of C (h), N (i), W (j), and O (k) in WO3/PHI.

Fig. 2. XRD patterns (a) and FTIR spectra (b) of WO3, PHI, and WO3/PHI. Polarized Raman mapping images of WO3 (c) and WO3/PHI (d).

Fig. 3. High-resolution XPS spectra of C 1s (a), N 1s (b), W 4f (c), and O 1s (d) for WO3, PHI and WO3/PHI under dark and illuminated conditions.

Fig. 4. W L3-edge XANES (a) and corresponding k2-weight W-L3 edge FT-EXAFS (b) of W Foil, WO3 and WO3/PHI. (c) k space of EXAFS for W Foil, WO3 and WO3/PHI. W L3-edge WT-EXAFS for W Foil (d), WO3 (e), and WO3/PHI (f). All EXAFS data are k2-weighted and not phase-corrected.

Fig. 5. Pseudocolor mapping (a-c) and relevant two-dimensional ultrafast spectral signal (d-f) of fs-TA for WO3, PHI, and WO3/PHI. Corresponding kinetic decay curves within 2000 ps of WO3 (g), PHI (h), WO3/PHI (i). The decay pathways of photogenerated carriers in WO3 (j) and WO3/PHI heterojunction (k).

Fig. 6. (a) Yield of CO and CH4 with different photocatalysts. (b) Yield of CO and CH4 in catalysts prepared by different methods. (c) Yield of CO and CH4 under different experimental conditions. (d) Yield of CO and CH4 in WP-3 with different water volume. (e) Cycle experiments of WP-3 for photocatalytic CO2 RR. (d) CO2 RR experiments via WP-3 under different illumination time. (f) Performance of different catalysts for yield of CO in photocatalytic CO2 RR.

Fig. 7. (a) UV-vis DRS of pristine WO3, PHI, and WO3/PHI. (b) Bandgap plots of pristine WO3 and PHI. (c) Mott-Schottky plots of pristine WO3 and PHI. (d) VB-XPS spectra of pristine WO3 and PHI. (e) Schematic band structures of pristine WO3 and PHI.

Fig. 8. Nyquist plots (a), instantaneous photocurrent density (b), PL spectra (c) and TRPL curves (d) of pristine WO3, PHI and WO3/PHI.

Fig. 9. N2 adsorption-desorption isotherms (a) and pore-size distribution profiles (b) of WO3, PHI and WO3/PHI. (c) EPR spectra of WO3, PHI and WO3/PHI recorded under dark and illuminated conditions in air and CO2 atmospheres.

Fig. 10. Band structures of pristine WO3 (a) and PHI (b). DOS of pristine WO3 (c) and PHI (d). Work functions of pristine WO3 (e) and PHI (f).

Fig. 11. (a) Schematic illustration of the S-scheme charge-transfer pathway in WO3/PHI. EPR spectra of DMPO-trapped •OH (b) and •O2- (c) radicals for pristine WO3, PHI and WO3/PHI.

Fig. 12. In-situ FTIR spectra of photocatalytic CO2 reduction via WO3/PHI under dark (a,b), and three-dimensional colour-mapped image of photocatalytic CO2 reduction via WO3/PHI under dark (c,d).

Fig. 13. In-situ FTIR spectra of photocatalytic CO2 reduction via WO3/PHI under illumination (a,b), and three-dimensional colour-mapped image of photocatalytic CO2 reduction via WO3/PHI under illumination (c,d).

Fig. 14. Proposed mechanism of WO3/PHI for photoreduction CO2.

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WO₃/PHI S-scheme heterojunction with photoinduced dual defects for highly selective photocatalytic CO₂-to-CO conversion

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