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<p>Photocatalytic oxidation of toluene to valuable benzaldehyde offers a promising pathway for sustainable production of fine chemicals and pharmaceuticals. In this process, photogenerated holes play a crucial role in C(sp<sup>3</sup>)-H bond dissociation. However, the photocatalytic performance of current photocatalysts is often hindered by the low separation and transfer efficiency of photogenerated charges. In this work, we presented a perovskite-based heterostructure via in situ growth of defective WO<sub>3-<i>x</i></sub> nanosheets on Cs<sub>2</sub>AgBiBr<sub>6</sub> nanoparticles for photocatalytic toluene transformation. In situ Fourier transform infrared spectroscopy tests proved the introduction of oxygen-deficient WO<sub>3-<i>x</i></sub> component enhanced the chemisorption of molecular oxygen. The in situ electron paramagnetic resonance and 4-chloro-7-nitro-1,2,3-benzoxadiazole fluorescence measurements further confirmed the presence of oxygen vacancies, and the formation of heterostructure synergistically accelerated the formation of the superoxide radicals and the transfer of photogenerated charge carriers. Under visible light irradiation, Cs<sub>2</sub>AgBiBr<sub>6</sub>/WO<sub>3-<i>x</i></sub> photocatalyst could effectively oxidize toluene toward benzaldehyde with a conversion rate of 9020&#xa0;μmol&#xa0;g<sup>−1</sup>&#xa0;h<sup>−1</sup>, which was a 3.5-fold increase over that of the unmodified Cs<sub>2</sub>AgBiBr<sub>6</sub>. </p> Graphical abstract <p></p>

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Oxygen vacancy in lead-free perovskite Cs2AgBiBr6/WO3-X for enhanced photocatalytic C(sp3)-H bond oxidation

  • 期刊论文

  • 发表日期：

    2025年6月30日

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  • Taoran Chen,
  • Tian Qin,
  • Hongli Sun,
  • Chenliang Su

摘要

Photocatalytic oxidation of toluene to valuable benzaldehyde offers a promising pathway for sustainable production of fine chemicals and pharmaceuticals. In this process, photogenerated holes play a crucial role in C(sp3)-H bond dissociation. However, the photocatalytic performance of current photocatalysts is often hindered by the low separation and transfer efficiency of photogenerated charges. In this work, we presented a perovskite-based heterostructure via in situ growth of defective WO3-x nanosheets on Cs2AgBiBr6 nanoparticles for photocatalytic toluene transformation. In situ Fourier transform infrared spectroscopy tests proved the introduction of oxygen-deficient WO3-x component enhanced the chemisorption of molecular oxygen. The in situ electron paramagnetic resonance and 4-chloro-7-nitro-1,2,3-benzoxadiazole fluorescence measurements further confirmed the presence of oxygen vacancies, and the formation of heterostructure synergistically accelerated the formation of the superoxide radicals and the transfer of photogenerated charge carriers. Under visible light irradiation, Cs2AgBiBr6/WO3-x photocatalyst could effectively oxidize toluene toward benzaldehyde with a conversion rate of 9020 μmol g−1 h−1, which was a 3.5-fold increase over that of the unmodified Cs2AgBiBr6.

Graphical abstract