Novel Fenton-like Catalyst HKUST-1(Cu)/MoS2-3-C with Non-Equilibrium-State Surface for Selective Degradation of Phenolic Contaminants: Synergistic Effects of -Cu-Ligand and Mo-OOSO3- Complex

Xiaoze Yin,Huaqin Yin, Renjie Wang,Jinnan Wang,Aimin Li

Water(2024)

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摘要
Novel Fenton-like catalyst HKUST-1(Cu)/MoS2-3-C with a non-equilibrium-state surface was constructed for selective degradation of phenolic contaminants. Electron-polarized distribution facilitated the formation of sigma-Cu-ligand between electron-poor Cu centre and phenolic compounds, which not only enhanced radicals generation but also accelerated the Cu(I)/Cu(II) redox. Meanwhile, equivalent to Mo-OOSO3- complexes formed by the electron-rich Mo centre and peroxymonosulfate (PMS), could directly oxidize phenolic contaminants with the generation of SO4 center dot-. The radical quenching experiments and EPR tests indicated that both SO4 center dot- and center dotOH played a dominant role in the reaction. Additionally, O-2 could be reduced to O-2(center dot-) by OVs and subsequently converted into O-1(2) over the Mo centre. DFT calculation, FT-IR, and in situ Raman spectra analysis results demonstrated that phenolic compounds and PMS were respectively adsorbed by electron-poor Cu centre and electron-rich Mo centre, favouring the electrons transfer from phenolic contaminants to Mo centre for PMS activation. With synergistic effects of sigma-Cu-ligand and equivalent to Mo-OOSO3- complexes, HKUST-1(Cu)/MoS2-3-C achieved a high degradation rate of phenolic contaminants and utilization efficiency of PMS.
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关键词
fenton-like catalyst,non-equilibrium-state surface,sigma-Cu-ligand,equivalent to Mo-OOSO3- complex,phenolic contaminants degradation
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