Ultrafast electron transfer in 2D/2D g-C3N4/WO3 S-scheme heterojunctions for enhanced H2O2 production

doi:10.1016/S1872-2067(26)64949-2

Abstract

Abstract:

The increasing demand for sustainable and environmentally friendly hydrogen peroxide (H₂O₂) production has necessitated the development of efficient photocatalytic strategies. A two-dimensional (2D)/2D graphitic carbon nitride (g-C₃N₄)/WO₃ S-scheme heterojunction was synthesized in this study via in situ growth, yielding an atomically intimate interface that promotes ultrafast interfacial charge transfer. Comprehensive spectroscopy, photoelectrochemistry, Kelvin probe force microscopy, and density functional theory investigations confirmed the S-scheme charge-transfer mechanism. This system, driven by an internal electric field, promotes the spatial separation of photoexcited charge carriers and maintains robust redox abilities. Femtosecond transient absorption spectroscopy revealed ultrafast interfacial charge transfer from WO₃ to g-C₃N₄. The optimized heterostructure exhibited considerably photocatalytic activity, achieving a 2571.6 μmol g⁻¹ h⁻¹ H₂O₂ production rate, representing 2.8- and 63.5-fold improvements over g-C₃N₄ and WO₃, respectively. Electron paramagnetic resonance and in situ diffuse reflectance infrared Fourier-transform spectroscopy were used to elucidate the oxygen reduction reaction mechanism, indicating that ethanol undergoes sequential oxidation, whereas photogenerated electrons reduce O₂ to produce H₂O₂ through a sequential single-electron process. This study offers significant mechanistic insights into the carrier dynamics within 2D S-scheme heterojunctions and presents a scalable and efficient route for green H₂O₂ synthesis.

Key words: g-C₃N₄, WO₃, S-scheme heterojunction, H₂O₂ production, Oxygen reduction reaction

Ping Li, Liang Wei, Wei Xia, Chengcheng Yuan, Chenbin Ai, Meng Li. Ultrafast electron transfer in 2D/2D g-C₃N₄/WO₃ S-scheme heterojunctions for enhanced H₂O₂ production[J]. Chinese Journal of Catalysis, 2026, 85: 333-345.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)64949-2

https://www.cjcatal.com/EN/Y2026/V85/I6/333

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Fig. 1. (a) Schematic diagram illustrating the synthesis of the 2D/2D g-C3N4/WO3 heterostructures. XRD patterns (b) and FTIR spectra (c) of pure g-C3N4, WO3, and their composites.

Fig. 2. FESEM images of g-C3N4 (a), WO3 nanosheets (b), and CW15 (c). TEM (d) and HRTEM (e) images of CW15. HAADF image (f) and corresponding EDX elemental maps (g-j) of CW15, confirming the homogeneous distribution of C, N, W, and O.

Fig. 3. (a) UV-vis DRS spectra of pure g-C3N4, WO3, and their composites. Tauc plot analysis (b), Mott-Schottky electrochemical plots (c), and schematic diagram illustrating the electronic band structure (d) for g-C3N4 and WO3.

Fig. 4. PL spectra (a), TRPL decay profiles (b), transient photocurrent densities (c), and EIS Nyquist plots (d) of g-C3N4, WO3, and their composites.

Fig. 5. High-resolution XPS spectra for the C 1s (a), N 1s (b), W 4f (c), and O 1s (d) regions of g-C3N4, WO3, and CW15 under dark and light irradiation.

Fig. 6. EPR spectra for DMPO-·O2- (a) and DMPO-·OH (b) for g-C3N4, WO3 and CW15.

Fig. 7. KPFM images of CW15 in the dark (a) and under light illumination (b). Corresponding VCPD (c) and SPV (d) of CW15 along the marked line.

Fig. 8. Calculated electrostatic potentials of the g-C3N4 (001) (a) and WO3 (001) (b) slabs. (c) Charge density difference of the g-C3N4/WO3 heterojunction interface; cyan and yellow isosurfaces represent electron depletion and accumulation regions, respectively. (d) Schematic diagram illustrating the interfacial electron transfer pathways and IEF formation in the S-scheme heterojunction.

Fig. 9. Two-dimensional pseudocolor fs-TA spectral maps for g-C3N4 (a), WO3 (b) and CW15 (c). Normalized temporal decay profiles of the GSB signals for g-C3N4 and CW15 probed at 430 nm (d) and WO3 probed at 420 nm within 6000 ps (e). (f) Schematic diagram illustrating the mechanistic pathways for photogenerated carrier relaxation and the charge transfer dynamics within the g-C3N4/WO3 S-scheme heterojunction.

Fig. 10. (a) Time-dependent photocatalytic H2O2 production over the as-prepared samples using ethanol as a sacrificial agent. (b) Comparison of the H2O2 production rates for the as-prepared samples. (c) Photocatalytic decomposition kinetics of 1 mmol L-1 H2O2 under light irradiation for 60 min. (d) Kinetic constants for H2O2 formation and decomposition derived from the data in (a) and (c).

Fig. 11. (a) Photocatalytic H2O2 production by CW15 in an N2 atmosphere, pure water, and various trapping agents. (b) Pseudocolor map depicting the temporal spectral intensity evolution on CW15 during dark adsorption and subsequent light irradiation with a H2O, O2, and ethanol mixed gas flow, followed by light irradiation. (c) Representative in-situ DRIFTS spectra of CW15.

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Ultrafast electron transfer in 2D/2D g-C₃N₄/WO₃ S-scheme heterojunctions for enhanced H₂O₂ production

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