<p>Photocatalytic oxidation of methyl mercaptan (CH<sub>3</sub>SH) often suffers from inefficient degradation and the generation of odorous byproducts such as dimethyl disulfide (DMDS), leading to secondary pollution and catalyst deactivation. In this study, we engineer a Sr-doped polymeric carbon nitride (CN) catalyst featuring spatially separated redox centers constructed via Sr–N coordination and nitrogen vacancies (N<sub>V</sub>). The optimized Sr-CN-N<sub>V</sub> material achieves stable &gt; 99% CH<sub>3</sub>SH removal over 50 h of continuous operation while completely suppressing DMDS formation. Mechanistic studies indicate that the spatially segregated charge carriers enhance reactive oxygen species (ROS) generation and promote the deep oxidation of adsorbed intermediates. This work provides a spatial-site engineering strategy for designing robust and selective photocatalysts toward efficient and sustainable air purification.</p>

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Engineering selective pathways for photocatalytic methyl mercaptan oxidation via spatially separated redox centers in Sr-modified carbon nitride

  • Shanrong Li,
  • Jiali Wang,
  • Shuangqing Liu,
  • Fanghua Zeng,
  • Zhiqi Wen,
  • Rui Xiong,
  • Can Yang

摘要

Photocatalytic oxidation of methyl mercaptan (CH3SH) often suffers from inefficient degradation and the generation of odorous byproducts such as dimethyl disulfide (DMDS), leading to secondary pollution and catalyst deactivation. In this study, we engineer a Sr-doped polymeric carbon nitride (CN) catalyst featuring spatially separated redox centers constructed via Sr–N coordination and nitrogen vacancies (NV). The optimized Sr-CN-NV material achieves stable > 99% CH3SH removal over 50 h of continuous operation while completely suppressing DMDS formation. Mechanistic studies indicate that the spatially segregated charge carriers enhance reactive oxygen species (ROS) generation and promote the deep oxidation of adsorbed intermediates. This work provides a spatial-site engineering strategy for designing robust and selective photocatalysts toward efficient and sustainable air purification.