期刊
CHEMICAL ENGINEERING JOURNAL
卷 369, 期 -, 页码 745-757出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.03.108
关键词
Advanced oxidation processes (AOPs); Tetracycline hydrochloride (TC-HCl); Photocatalyst; MIL-88A; Degradation pathway
资金
- National Natural Science Foundation of China [21277108, 21476179]
- one hundred talents project of Guangzhou University
- Wuhan Yellow Crane Talents (Science) Program
In this work, a Fe-based metal organic frameworks (MIL-88A) has been synthesized through a hydrothermal method and adopted as a high-efficiency catalyst for photocatalysis (PC) coupled with sulfate radical-based advanced oxidation processes (SR-AOPs) to degrade tetracycline hydrochloride (TC-HC1) under visible light irradiation. The effects of MIL-88A/persulfate (PS) molar ratio, initial solution pH and catalyst dosage were studied. The results indicated that the combining of the photocatalysis and SR-AOPs could remarkably enhance TC degradation and 200mg/L 100mL TC could be degraded completely at 0.25 g/L MIL-88A, unadjusted pH value and 4 mM PS in 80 mins. The results of scavenging experiments and ESR analysis demonstrated that SO4-center dot and O-center dot(2-) radicals were the predominant radicals for the TC degradation. The significant improvement of degradation rate in MIL-88A/PS/Vis process is attributed to the following two factors: (1) as a photocatalyst, MIL88A could be excited by visible light, therefore photogenerated electrons (e(-)) on the conduction band (CB) of MIL-88A could be trapped by PS to generate SO(4)(-center dot)radicals. In this process, PS acted as an electron acceptor and the electron/hole recombination was suppressed leading to the enhanced photocatalyst efficiency; (2) The PS can be activated not only by photoelectrons but also Fe (III) in MIL-88A leads to the generation of SO4-center dot radicals more rapidly and easily. A possible mechanism and degradation pathway for TC was proposed based on the trapping/ESR experiments and liquid chromatography-mass spectrometry (LC-MS) analysis. This work proposed a new idea and method in combining two oxidation processes in degradation of organic pollutants thus could be potentially used in environmental purification.
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