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

• Published in: Journal of hazardous materials Vol. 392; p. 122315
• Main Authors: Zhang, Ying, Zhou, Jiabin, Chen, Junhui, Feng, Xiaoqiong, Cai, Weiquan
• Format: Journal Article
• Language: English
• Published: Netherlands Elsevier B.V 15.06.2020
• Subjects: Advanced oxidation processes; Anti-Bacterial Agents - chemistry; Catalysis; catalysts; Degradation pathway; electron paramagnetic resonance spectroscopy; electrons; free radicals; iron; Iron - chemistry; Iron - radiation effects; irradiation; Light; liquid chromatography; mass spectrometry; Metal-Organic Frameworks - chemistry; Metal-Organic Frameworks - radiation effects; MIL-53(Fe); oxidation; Oxidation-Reduction; photocatalysis; Photocatalyst; Photochemical Processes; Sodium Compounds - chemistry; Sodium Compounds - radiation effects; Sulfate radical; sulfates; Sulfates - chemistry; Sulfates - radiation effects; superoxide anion; tetracycline; Tetracycline - chemistry; Water Pollutants, Chemical - chemistry; Advanced oxidation processes; MIL-53(Fe); Sulfate radical; Photocatalyst; Degradation pathway
• ISSN: 0304-3894; 1873-3336; 1873-3336
• DOI: 10.1016/j.jhazmat.2020.122315

[Display omitted] •Heterogeneous AOP and photocatalysis were coupled for degradation of TC.•The introduction of PS effectively suppressed the recombination of charge carries.•Photogenerated electron of MIL-53(Fe) can activate PS to generate SO4− radicals.•The degradation pathway of TC is proposed by theoretical calculations and LC–MS. 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− could be formed by the conversion between Fe (Ⅲ) and Fe (Ⅱ) in MIL-53(Fe). Moreover, OH and O2− generated by the reaction increased significantly due to the increase of SO4− 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.