One-pot synthesis of mesoporous silicas supported Cu single-atom and CuO nanoparticles for peroxymonosulfate-activated degradation of tetracycline over a wide pH range

作者：Liu, Ying; Qiu, Lijun; Nan, Qingwei; Wang, Jie; Zhao, Joe R.; Li, Tingzhen; Hu, Chuanbo; Hu, Lei; Tang, Jianting^*; Liu, Xiao^*

来源：Microporous and Mesoporous Materials, 2022, 333: 111729.

DOI：10.1016/j.micromeso.2022.111729

• Cu single-atom
• CuO nanoparticles
• Fenton-like
• Peroxymonosulfate
• Tetracycline

Peroxymonosulfate activated heterogeneous Fenton-like catalytic reactions are promising in degradation of recalcitrant pollutants. Mesoporous silicas supported high-dispersion Cu species, as a kind of conventional heterogeneous catalysts for extensive applications, are rarely studied for their degradation efficiency in peroxymonosulfate-triggered reactions. In this work, one-pot incorporation method was employed to generate simultaneously Cu single-atom, Cu nanoparticles in mesoporous silicas (like the sample of Cu/Si-3 with 0.68 wt% of Cu) using sodium copper chlorophyllin as Cu source by calcining directly in air atmosphere. Several char-acterizations confirm the coexistence of Cu single-atom, Cu nanoparticles and mesopore with uniform size dis-tribution. Activated by peroxymonosulfate, Cu/Si-3 was found to be efficient in degradation of tetracycline throughout a wide pH range of 2-11. The radicals of SO4g-, center dot OH and O-1(2) played their role in the degradation reaction. The underlying catalytic mechanism of the Fenton-like reaction was speculated on the basis of analysis of reactive oxygen species. This work has important implication in reasonable design and fabrication of catalysts with high-dispersion metal and controllable synthesis of functional mesoporous materials, as well as in proper disposal of recalcitrant pollutants including tetracycline.

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