Effect of surface properties of activated carbon fiber cathode on mineralization of antibiotic cefalexin by electro-Fenton and photoelectro-Fenton treatments: Mineralization, kinetics and oxidation products

摘要

Solutions of 200 mg L-1 cefalexin (CLX), an antibiotic with high usage frequency and biodegradation resistance, have been comparatively degraded by electro-Fenton (EF) and photoelectro-Fenton (PEF) processes using two kinds of activated carbon fiber (ACF) cathodes with different physical properties. These two ACFs shared similar pore volumes and pore diameters but varied BET surface areas, which were confirmed to be 0.5210 cm(3) g(-1), 2.26 nm and 921 m(2) g(-1) for ACF1, while 0.6508 cm(3) g(-1), 2.16 nm and 1206 m(2) g(-1) for ACF2, respectively. Their oxidation abilities were comparatively assessed in terms of degradation kinetics and mineralization rates, which increased in the order: ACF1-EF ACF2-EF ACF1-PEF ACF2-PEF. These results confirmed the superiority of ACF with higher surface area, which was correlated to faster H2O2 and (OH)-O-center dot accumulation in more reaction sites provided. After 120 min electrolysis, ACF1 exhibited 1510 mu M H2O2 and 37 mu M (OH)-O-center dot accumulation, while ACF2 generated 1934 mu M H2O2 and 85 mu M (OH)-O-center dot. Moreover, ACF cathode with more developed pore structure also revealed faster formation of degradation by-products like inorganic ions (NH4+ and NO3- ions) and short-chain carboxylic acids (acetic, formic, oxamic and oxalic acids), as well as enhanced removal for partial acids. In order to gain a deeper understanding of degradation mechanisms for ACF2-PEF system, evolutions of six aromatic by-products generated from sulfoxidation, hydroxylation and decarboxylation were confirmed by UPLC-QTOF-MS/MS determination. Based on the above identifications of the degradation intermediates, a plausible reaction pathway for CLX removal was proposed. (C) 2019 Published by Elsevier Ltd.