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In-situ fabrication of MOF-derived MnO-C modified graphite felt for electro-activation of peroxymonosulfate toward degradation of tetracycline: Performance, mechanism and degradation pathway

SEPARATION AND PURIFICATION TECHNOLOGY [2024]
Rong Su, Zeyi Wang, Feng Xiao, Luyao Zhang, Qihang He, Lei Wang, Yu Jiang, Lichuan Chen, Lu Yang, Ping He
ABSTRACT

Peroxymonosulfate (PMS) activation by synergy of electrochemistry and catalyst has emerged as a promising technique for the degradation of organic contaminants. Herein, manganese oxide-carbon modified graphite felt (MnO-C/GF) electrodes are successfully synthesized by pyrolyzing Mn-MOF/GF composite. MnO-C/GF is employed as an anode to remove tetracycline (TC) in a process of PMS activation with the assistance of electrochemistry (EC). Under optimal conditions (50 mg/L TC, 10 mA·cm −2 , pH 7, 0.80 mM PMS,0.05 M Na 2 SO 4 , 25 °C), MnO-C 800 /GF electrode (pyrolysis at 800 °C) achieves remarkable degradation efficiency of 90.48 % for TC after 60 min in EC-PMS system. The reaction rate constant ( k ) of MnO-C 800 /GF increases by 4.54 and 2.38 times compared to bare GF and MnO/GF in EC-PMS system, respectively. In addition, quenching test and electron paramagnetic resonance test reveal that ·OH, SO 4 − , O 2 − and 1 O 2 are involved in the degradation process at MnO-C 800 /GF-EC-PMS system. According to the results of density functional theory and liquid chromatography-mass spectrometry, the degradation of TC mainly includes hydrogenation, demethylation, deamidation, dehydroxylation and ring-opening reactions. This work demonstrates that the combination of electrochemistry and metal oxide-activated PMS is a highly efficient approach for the degradation of antibiotic contaminant.

MATERIALS

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