<p>Photocatalytic oxygen reduction reaction (ORR) represents a green and cost-effective means to produce the high-value industrial compound H<sub>2</sub>O<sub>2</sub>. However, the efficient H<sub>2</sub>O<sub>2</sub> synthesis awaits in-depth knowledge of the ORR mechanisms for the design of highly active photocatalysts. In this work, surface indium vacancies (denote hereafter as V<sub>In</sub>) have been introduced into In<sub>2</sub>S<sub>3</sub>, which significantly boosts the photocatalytic activity for H<sub>2</sub>O<sub>2</sub> production, with an optimal H<sub>2</sub>O<sub>2</sub> generation rate of 4.77 ± 0.05 mmol·h<sup>−1</sup>·g<sub>cat.</sub><sup>−1</sup> under visible light illumination (λ ≥ 420 nm) and an apparent quantum efficiency (AQE) of 7.49 ± 0.01% at 420 ± 20 nm. Mechanistic analysis reveals the multifunctionality of V<sub>In</sub>, such as enlarging the chemisorption capacity of O<sub>2</sub>, enriching photo-generated electrons for ORR, endorsing high reducing power to photo-generated electrons, and promoting H<sub>2</sub>O<sub>2</sub> desorption. These findings justify that surface cation vacancies open up new possibilities for H<sub>2</sub>O<sub>2</sub> photosynthesis by leveraging their reaction dimensions in ORR.</p>

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Surface indium vacancies promote photocatalytic H2O2 production over In2S3

  • Qiong Zhu,
  • Jingjing Su,
  • Guoan Lin,
  • Guisheng Li,
  • Zhiwen Zhuo,
  • Weiyi Wang,
  • Jialin Li,
  • Xiaoxiang Xu

摘要

Photocatalytic oxygen reduction reaction (ORR) represents a green and cost-effective means to produce the high-value industrial compound H2O2. However, the efficient H2O2 synthesis awaits in-depth knowledge of the ORR mechanisms for the design of highly active photocatalysts. In this work, surface indium vacancies (denote hereafter as VIn) have been introduced into In2S3, which significantly boosts the photocatalytic activity for H2O2 production, with an optimal H2O2 generation rate of 4.77 ± 0.05 mmol·h−1·gcat.−1 under visible light illumination (λ ≥ 420 nm) and an apparent quantum efficiency (AQE) of 7.49 ± 0.01% at 420 ± 20 nm. Mechanistic analysis reveals the multifunctionality of VIn, such as enlarging the chemisorption capacity of O2, enriching photo-generated electrons for ORR, endorsing high reducing power to photo-generated electrons, and promoting H2O2 desorption. These findings justify that surface cation vacancies open up new possibilities for H2O2 photosynthesis by leveraging their reaction dimensions in ORR.