One-step synthesis of Mn-doped MIL-53(Fe) for synergistically enhanced generation of sulfate radicals towards tetracycline degradation

Jun Yu; Jiao Cao; Zhaohui Yang; Weiping Xiong; Zhengyong Xu; Peipei Song; Meiying Jia; Saiwu Sun; Yanru Zhang; Juan Zhu

doi:10.1016/j.jcis.2020.07.045

One-step synthesis of Mn-doped MIL-53(Fe) for synergistically enhanced generation of sulfate radicals towards tetracycline degradation

J Colloid Interface Sci. 2020 Nov 15:580:470-479. doi: 10.1016/j.jcis.2020.07.045. Epub 2020 Jul 15.

Authors

Jun Yu¹, Jiao Cao¹, Zhaohui Yang², Weiping Xiong³, Zhengyong Xu⁴, Peipei Song⁵, Meiying Jia¹, Saiwu Sun¹, Yanru Zhang¹, Juan Zhu⁶

Affiliations

¹ College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.
² College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China. Electronic address: yzh@hnu.edu.cn.
³ College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China. Electronic address: xiongweiping@hnu.edu.cn.
⁴ Science and Technology Service Center of Hunan Province, Changsha 410128, PR China.
⁵ College of Resources and Environment, Key Laboratory of Agricultural Environment, Shandong Agricultural University, Tai'an 271000, PR China.
⁶ Hunan Xinheng Environmental Technology Co Ltd, Changsha 410005, PR China.

PMID: 32711198
DOI: 10.1016/j.jcis.2020.07.045

Abstract

Herein, Mn-doped MIL-53(Fe) were fabricated via one-pot solvothermal method and used for peroxymonosulfate (PMS) activation towards tetracycline (TC) degradation from aqueous solution. The characterizations of SEM, FTIR and XRD were utilized to reveal the morphology and structure of the materials. The results showed that Mn-MIL-53(Fe)-0.3 displayed the optimal catalytic performance, the removal efficiency of TC could reach 93.2%. Moreover, the catalytic activity of Mn-MIL-53(Fe) towards TC under different initial pH values, co-existing anions (Cl^-,CO₃^2- and SO₄^2-) and humic acid (HA) were investigated. The results of thermodynamic experiment suggested that the catalytic process was endothermic. In addition, integrated with capture experiments results and the characterization results of electron paramagnetic resonance (EPR), which revealed that SO₄^·- and HO^- were the reactive radicals involving in the reaction. More importantly, the possible activation mechanism was discussed in detail based on the X-ray photoelectron spectroscopy results. The active species were generated by the active sites of Fe(II) and Mn(II) on Mn-MIL-53(Fe) effectively activated PMS. Furthermore, the degradation intermediates and possible degradation pathway were investigated by LC-MS. Finally, the catalyst also showed good performance in actual wastewater and demonstrated good recyclability. The Mn-MIL-53(Fe)/PMS system exhibited a promising application prospect for antibiotic-containing waste water treatment.

Keywords: MIL-53(Fe); Mn-doped; One-step solvothermal synthesis; Peroxymonosulfate activation; Tetracycline.

MeSH terms

Anti-Bacterial Agents
Sulfates*
Tetracycline*

Substances

Anti-Bacterial Agents
sulfate radical
Sulfates
Tetracycline