Boosting sequential single-electron O2 reduction reaction on S-scheme SbVO4/PCN heterojunction for efficient artificial photosynthesis of H2O2 under ambient condition

doi:10.1016/S1872-2067(26)65203-5

Abstract

Abstract:

Non-sacrificial artificial photosynthesis of H₂O₂ offers a charming process for onsite H₂O₂ generation with unique merits of sustainability and environmental friendliness. However, the low conversion efficiency of sequential single-electron oxygen reduction reaction (SSORR) greatly limits the H₂O₂ production rate. Herein, we develop a step-scheme (S-scheme) SbVO₄/PCN system for artificial photosynthesis of H₂O₂, which displays greatly boosted photocatalytic SSORR. The H₂O₂ yield can reach as high as 94.7 μmol·g-catalyst^-1·h^-1 under visible light illumination (λ > 420 nm), about 41 times higher than that of the pristine PCN. The S-scheme charge transfer pathway is systematically demonstrated by photo-irradiated Kelvin probe force microscopy, in-situ X-ray photoelectron spectroscopy and surface photovoltage measurements. Theoretical calculations further indicate that the SbVO₄/PCN is favorable to transfer electrons from its hybrid p orbitals to the 1π and 2π* orbitals of O₂ and the evolution from *O₂ to *OOH consumes no energy, therefore greatly promoting the formation of PCN-*OOH even without electron donor. The onsite generated O₂ via water oxidation reaction on SbVO₄ can replenish its consumption on PCN, leading to boosted reaction kinetics.

Key words: Artificial photosynthesis, Sequential single-electron oxygen reduction reaction, H₂O₂, S-scheme, SbVO₄/PCN

Zhuangzhuang Wang, Yuan Li, Qiang Cheng, Xiaotian Wang, Bin Liu, Gaoke Zhang. Boosting sequential single-electron O₂ reduction reaction on S-scheme SbVO₄/PCN heterojunction for efficient artificial photosynthesis of H₂O₂ under ambient condition[J]. Chinese Journal of Catalysis, 2026, 91: 241-251.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65203-5

https://www.cjcatal.com/EN/Y2026/V91/I12/241

Figures/Tables 5

Fig. 1. (a) Schematic illustration showing the synthetic process of 10-SbV/PCN nanocomposites. (b,c) TEM images of 10-SbV/PCN nanocomposites. (d) HRTEM image of 10-SbV/PCN nanocomposites. (e) EDS elemental mapping images of 10-SbV/PCN nanocomposites.

Fig. 2. (a) Long-term photocatalytic H2O2 production catalyzed by pristine PCN (pink color) and 10-SbV/PCN (yellow color) under different irradiation wavelength. (b) Solar-to-chemical conversion efficiency of 10-SbV/PCN under 365 and 420 nm light irradiation in pure water and open air. (c) Apparent quantum yield of 10-SbV/PCN under 365 and 420 nm light irradiation in pure water and open air. (d) In-situ DRIFTS spectra recorded over 10-SbV/PCN. Photocatalytic O2 (e) and H2 (f) evolution over PCN and 10-SbV/PCN.

Fig. 3. (a) In-situ and ex-situ survey XPS spectra of different catalysts. In-situ and ex-situ high-resolution XPS spectra of C 1s (b), N 1s (c), V 3d (d), Sb 3d (e), and O 1s (f). In-situ XPS spectra were collected under the irradiation of 365 nm light.

Fig. 4. Surface potential distribution of 10-SbV/PCN in dark (a) and under 365 nm light irradiation (b). (c) The line-scanning surface potential from A1 to B1 in dark and A2 to B2 under 365 nm light irradiation, respectively. (d) Surface photovoltage spectra of pristine PCN and 10-SbV/PCN. (e) Surface photocurrent spectra of PCN and 10-SbV/PCN. (f) TRPL spectra of PCN and 10-SbV/PCN.

Fig. 5. The calculated electrostatic potential of (111) plane of SbV (a) and its corresponding structural model along the [111] direction (b). The calculated electrostatic potential of (001) plane of PCN (c) and its corresponding structural model along the [001] direction (d). The planar-averaged electron density difference Δρ (e) and the side-view of the charge density difference (f) over the SbV/PCN heterojunction. Inset shows the electronic location function of SbV/PCN (the red and green colors represent electron accumulation and depletion, respectively). (g) The interaction of px+py orbitals of SbV/PCN and O2 orbitals after O2 adsorption on SbV/PCN. (h) Free energy of sequential single-electron ORR. (i) Proposed photocatalytic mechanism of SbV/PCN heterojunction for robust production of H2O2.

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Boosting sequential single-electron O₂ reduction reaction on S-scheme SbVO₄/PCN heterojunction for efficient artificial photosynthesis of H₂O₂ under ambient condition

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