Rapid degradation of tetracycline hydrochloride by heterogeneous photocatalysis coupling persulfate oxidation with MIL-53(Fe) under visible light irradiation

被引:190
作者
Zhang, Ying [1 ,2 ]
Zhou, Jiabin [1 ]
Chen, Junhui [3 ]
Feng, Xiaoqiong [3 ]
Cai, Weiquan [4 ]
机构
[1] Southwest Petr Univ, Sch Chem & Chem Engn, Chengdu 610500, Peoples R China
[2] Wuhan Univ Technol, Sch Resources & Environm Engn, Wuhan 430070, Peoples R China
[3] Sichuan Acad Environm Sci, Chengdu 610041, Peoples R China
[4] Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou Higher Educ Mega Ctr, 230 Wai Huan Xi Rd, Guangzhou 510006, Peoples R China
基金
中国国家自然科学基金;
关键词
MIL-53(Fe); Advanced oxidation processes; Photocatalyst; Sulfate radical; Degradation pathway; METAL-ORGANIC FRAMEWORKS; HYDROGEN-PEROXIDE; RHODAMINE-B; ACTIVATION; PHOTODEGRADATION; PERFORMANCE; ADSORPTION; PATHWAY; FABRICATION; COMPOSITES;
D O I
10.1016/j.jhazmat.2020.122315
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This work demonstrates a facile route to assemble MIL-53(Fe) by solvothermal method. Sulfate radical-based advanced oxidation processes (SR-AOPs) coupling with photocatalysis based on MIL-53(Fe) were investigated under visible light. The catalytic effect of MIL-53(Fe) for the degradation of tetracycline hydrochloride (TC-HCl) was systematically studied, as well as the reusability of the catalyst and the effect of operating parameters. The results indicated that 99.7 % of TC (300 mg/L) could be degraded within 80 min in the SR-AOPs coupling with photocatalysis processes, as compared to 71.4 % for the SR-AOPs and only 17.1 % for the photocatalysis. The trapping experiments and electron spin-resonance spectroscopy (ESR) showed the photogenerated electrons of MIL-53(Fe) under visible light irritation were trapped by persulfate to generated sulfate radicals which effectively suppressed the recombination of photogenerated carriers. And also, the SO4-center dot could be formed by the conversion between Fe (III) and Fe (II) in MIL-53(Fe). Moreover, (OH)-O-center dot and O-center dot(2)- generated by the reaction increased significantly due to the increase of SO4-center dot which generated more 'OH and reduced photogenerated carrier recombination respectively. Thus, the degradation efficiency of TC-HCl was improved. Furthermore, the degradation pathway for TC-HCl was proposed using the theoretical calculations and liquid chromatography coupled with mass spectrometry.
引用
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页数:11
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