Degradation of methylparaben by sonocatalysis using a Co–Fe magnetic carbon xerogel

• Published in: Ultrasonics sonochemistry Vol. 64; p. 105045
• Main Authors: Zanias, Athanasios, Frontistis, Zacharias, Vakros, John, Arvaniti, Olga S., Ribeiro, Rui S., Silva, Adrián M.T., Faria, Joaquim L., Gomes, Helder T., Mantzavinos, Dionissios
• Format: Journal Article
• Language: English
• Published: Netherlands Elsevier B.V 01-06-2020
• Subjects: Advanced oxidation; Cavitation; Low frequency ultrasound; Micropollutants; Sonodegradation; Water quality; Low frequency ultrasound; Micropollutants; Advanced oxidation; Sonodegradation; Cavitation; Water quality
• DOI: 10.1016/j.ultsonch.2020.105045
• EISSN: 1873-2828
• ISSN: 1350-4177

•Methylparaben (MP) can be degraded by low frequency ultrasound.•Adding the CX/CoFe catalyst enhances degradation of MP in a synergistic way.•H2O2 formed through water sonolysis is decomposed to hydroxyl radicals.•Water matrix effects are detrimental to methylparaben degradation.•Main oxidation pathways involve hydroxyl radicals and other oxygen species.
The degradation of methylparaben (MP) through 20 kHz ultrasound coupled with a bimetallic Co-Fe carbon xerogel (CX/CoFe) was investigated in this work. Experiments were performed at actual power densities of 25 and 52 W/L, catalyst loadings of 12.5 and 25 mg/L, MP concentrations between 1 and 4.2 mg/L and initial pH values between 3 and 10 in ultrapure water (UPW). Matrix effects were studied in bottled water (BW) and secondary treated wastewater (WW), as well as in UPW spiked with bicarbonate, chloride or humic acid. The pseudo–first order kinetics of MP degradation increase with power and catalyst loading and decrease with MP concentration and matrix complexity; moreover, the reaction is also favored at near–neutral conditions and in the presence of dissolved oxygen. The contribution of the catalyst is synergistic to the sonochemical degradation of MP and the extent of synergy is quantified to be >45%. This effect was ascribed to the ability of CX/CoFe to catalyze the dissociation of hydrogen peroxide, formed through water sonolysis, to hydroxyl radicals. Experiments in UPW spiked with an excess of tert-butanol (radical scavenger), sodium dodecyl sulfate or sodium acetate (surfactants) led to substantially decreased rates (i.e. by about 8 times), thus implying that the liquid bulk and the gas-liquid interface are major reaction sites. The stability of CX/CoFe was shown by performing reusability cycles employing magnetic separation of the catalyst after the treatment stage. It was found that the CX/CoFe catalyst can be reused in up to four successive cycles without noteworthy variation of the overall performance of the sonocatalytic process.