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Fabricating an oxygen-vacancy-rich urchin-like Co3O4 nanocatalyst to boost peroxymonosulfate activation to degrade high-concentration crystal violet

Journal 2022 · IF 5.532 · 发表于 2022 年 6 月 3 日
作者: Bo Li,Huan-Yan Xu,Yu-Long Liu,Li-Min Dong,Sridhar Komarneni
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摘要

Due to the in-situ generation of reactive oxygen species (ROS), sulfate radical-based advanced oxidation processes (SR-AOPs) have emerged for the oxidative degradation of organic contaminants. Developing highly efficient heterogeneous catalysts is of great importance for SR-AOPs. In this work, an urchin-like Co 3 O 4 nanocatalyst with oxygen vacancies (V O ) was elaborately fabricated and employed for enhanced peroxymonosulfate (PMS) activation to degrade the high-concentration active dye crystal violet (CV). The obtained sample was characterized by field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and N 2 adsorption/desorption isotherms. Characterization results indicated that this unique V O -rich urchin-like Co 3 O 4 nanocatalyst was endowed with a larger surface area and abundant reactive sites for PMS adsorption and activation. The experimental results of CV degradation showed that nearly complete removal of 100 mg L −1  CV could be realized within 30 min of reaction time under neutral conditions at room temperature, and the degradation process followed retarded-first-order kinetics. Electron paramagnetic resonance (EPR) spectra accompanied by quenching experiments of radicals demonstrated that the contribution of ROS to CV degradation followed this sequence: 1 O 2  > ▪OH > SO 4 ▪-  > O 2 ▪- . The degradation pathways of CV were proposed by a combination of density functional theory (DFT) calculations along with frontier orbit theory while the toxicity of intermediate products was evaluated by quantitative structure-activity relationship (QSAR) prediction.

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