1. Benzothiadiazole-functionalized Zr-MOF nanosheets enable visible-light mediated photocatalytic oxidation of sulfides in water.
- Author
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Chong, Yu-Liang, Zhao, Dong-Dong, Yan, Mi, Zhou, Xing-Yu, Zhang, Jun-Jie, Wang, Bing, Chen, Zhuo, and Zhuang, Jin-Liang
- Subjects
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SULFOXIDES , *PHOTOCATALYTIC oxidation , *OXIDATION of water , *NANOSTRUCTURED materials , *REACTIVE oxygen species , *PHOTOCATALYSTS , *VISIBLE spectra - Abstract
Water stable Zr-BTDB ultrathin nanosheets incorporated with benzothiadiazole moieties enable efficient aerobic oxidation of a wide range of sulfides to sulfoxides under visible light irradiation in water at room temperature. [Display omitted] • Ultrathin, water stable and photoactive Zr-MOF nanosheets were synthesized. • Zr-MOF nanosheets exhibit superior photocatalytic activity for aerobic oxidation of sulfides. • Singlet oxygen and superoxide radical are reactive oxygen species for the oxidation of sulfides. Ultrathin metal-organic frameworks (MOFs) nanosheets incorporating photochromic units are highly efficient heterogeneous photocatalysts, thanks to their highly exposed catalytic sites, short diffusion pathways, and efficient separation of photo-generated carriers. Herein, we report on the solvothermal synthesis of photoactive benzothiadiazole (BTz) functionalized Zr-MOF nanosheets (Zr-BTDB-NS), which are constructed from Zr 12 nodes linked by nine BTDB2− (BTDB = 4,4′-(benzo[c][1,2,5]thiadiazole-4,7-diyl)dibenzoate) ligands. The Zr-BTDB-NS exhibited superior photocatalytic activity towards the aerobic oxidation of a broad range of sulfides to their corresponding sulfoxides under visible light irradiation in water at room temperature, even in a gram-scale. The Zr-BTDB-NS can be efficiently recycled and reused for seven cycles without a decrease in conversion or selectivity. Detailed mechanism studies revealed that the Zr-BTDB-NS generates singlet oxygen (1O 2) and superoxide radical (O 2 –) reactive oxygen species under visible light irradiation, which are responsible for the oxidation of sulfides into their corresponding sulfoxides. The simplicity of the synthetic approach as well as the diversity of photoactive organic units hold great promise for designing ultrathin, water-stable, and photoactive Zr-MOF nanosheets. This work will also be of added value for selective photooxidation of sulfides under green and mild conditions. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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