Coupling of heterogeneous advanced oxidation processes and photocatalysis in efficient degradation of tetracycline hydrochloride by Fe-based MOFs: Synergistic effect and degradation pathway

•Heterogeneous AOP and photocatalysis were coupled for efficient degradation of TC.•The introduction of PS effectively suppressed the recombination of charge carries.•Photogenerated electron can activate PS to generate SO4−• radicals.•The degradation pathways for TC are investigated through LC-MS te...

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Published in:	Chemical engineering journal (Lausanne, Switzerland : 1996) Vol. 369; pp. 745 - 757
Main Authors:	Zhang, Ying, Zhou, Jiabin, Chen, Xin, Wang, Luo, Cai, Weiquan
Format:	Journal Article
Language:	English
Published:	Elsevier B.V 01.08.2019
Subjects:	Advanced oxidation processes (AOPs) Degradation pathway MIL-88A Photocatalyst Tetracycline hydrochloride (TC-HCl) MIL-88A Tetracycline hydrochloride (TC-HCl) Advanced oxidation processes (AOPs) Photocatalyst Degradation pathway
ISSN:	1385-8947, 1873-3212
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Abstract	•Heterogeneous AOP and photocatalysis were coupled for efficient degradation of TC.•The introduction of PS effectively suppressed the recombination of charge carries.•Photogenerated electron can activate PS to generate SO4−• radicals.•The degradation pathways for TC are investigated through LC-MS technique. 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-HCl) 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 200 mg/L 100 mL 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−• and •O2– 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, MIL-88A 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 SO4−• 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−• 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.
AbstractList	•Heterogeneous AOP and photocatalysis were coupled for efficient degradation of TC.•The introduction of PS effectively suppressed the recombination of charge carries.•Photogenerated electron can activate PS to generate SO4−• radicals.•The degradation pathways for TC are investigated through LC-MS technique. 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-HCl) 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 200 mg/L 100 mL 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−• and •O2– 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, MIL-88A 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 SO4−• 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−• 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.
Author	Zhang, Ying Chen, Xin Zhou, Jiabin Wang, Luo Cai, Weiquan
Author_xml	– sequence: 1 givenname: Ying surname: Zhang fullname: Zhang, Ying organization: School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China – sequence: 2 givenname: Jiabin surname: Zhou fullname: Zhou, Jiabin email: jbzhou@swpu.edu.cn organization: School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China – sequence: 3 givenname: Xin surname: Chen fullname: Chen, Xin organization: School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, China – sequence: 4 givenname: Luo surname: Wang fullname: Wang, Luo organization: School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, China – sequence: 5 givenname: Weiquan surname: Cai fullname: Cai, Weiquan email: cccaiwq@gzhu.edu.cn organization: School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, PR China
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Snippet	•Heterogeneous AOP and photocatalysis were coupled for efficient degradation of TC.•The introduction of PS effectively suppressed the recombination of charge...
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SubjectTerms	Advanced oxidation processes (AOPs) Degradation pathway MIL-88A Photocatalyst Tetracycline hydrochloride (TC-HCl)
Title	Coupling of heterogeneous advanced oxidation processes and photocatalysis in efficient degradation of tetracycline hydrochloride by Fe-based MOFs: Synergistic effect and degradation pathway
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