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Polyoxometalates/TiO2 Fenton-like photocatalysts with rearranged oxygen vacancies for enhanced synergetic degradation
摘要： Oxygen vacancy modulation has emerged as a prevalent strategy to improve the performance of heterogeneous catalysts. By far, the impact of oxygen vacancy rearrangement on the efficiency of Fenton-like reaction remains largely unknown. In this paper, Fe-containing polyoxometalates were coupled with defect-rearranged TiO2 to construct defective Fenton-like photocatalysts. Experimental characterizations revealed that defect rearrangement facilitated the interfacial transfer of electrons from TiO2 to polyoxometalate molecules. Fenton-like photocatalysts with rearranged defects exhibited 5 and 3.5 times higher activity for the synergetic degradation of toxic dye and 5-Sulfosalicylic acid than pristine TiO2. This enhancement was ascribed to the beneficial role of oxygen vacancy modulation for activating oxygen and H2O2 molecules into ?O2- and ?OH radicals. Our work provides new opportunities for exploring efficient Fenton-like photocatalysts for environmental remediation.
关键词： Photocatalytic reaction,Polyoxometalates,Fenton-like reaction,Titanium Dioxide,Oxygen vacancy rearrangement
更新于2025-09-10 09:29:36
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Transformation pathway and degradation mechanism of methylene blue through β-FeOOH@GO catalyzed photo-Fenton-like system
摘要： To enhance the catalytic and separation properties of akaganéite nanoparticles, rice spike-like akaganéite impregnated graphene oxide (β-FeOOH@GO) nanocomposite was fabricated through facile hydrolysis. The apparent first-order decolorization rate of methylene blue (MB) in β-FeOOH@GO catalyzed photo Fenton-like system was 0.6322 min-1 about 3 folds that of prinstine β-FeOOH nanoparticles. The degradation intermediates of MB adsorbed on the solid surface of β-FeOOH@GO were comprehensively identified with time of flight-secondary ion mass spectroscopy (TOF-SIMS) for the first time. Newly identified sulfoxide intermediates, sulphone intermediates and desulfurization intermediates and N-demethylaton or dedimethamine intermediates were reported for the first time. The proposed degradation pathway of MB predominantly proceeded with the rupture of phenothiazine rings oxided with ?OH, HO?? and singlet oxygen (1O2) radicals, which fully extending the reaction pathways proposed in previous work in literature. The enhanced catalytic activity of β-FeOOH@GO was ascribed to the formation of heterojunctions confirmed by the presence of Fe-O-C chemical bonds through X-ray photoelectron spectroscopy (XPS). The complete elimination of MB and its acute toxicity to Luminous bacteria showed that β-FeOOH@GO would be served as a highly efficient Fenton-like catalyst for treatment of high concentration refractory organic contaminant.
关键词： Degradation mechanism,Graphene oxide,Methylene blue,β-FeOOH,Photo-Fenton-like reaction
更新于2025-09-10 09:29:36