Technical Papers
Aug 13, 2019

Hydroxyl Radical Generation and Partitioning in Degradation of Methylene Blue and DEET by Dual-Frequency Ultrasonic Irradiation

Publication: Journal of Environmental Engineering
Volume 145, Issue 10

Abstract

Ultrasonic (US) irradiation is effective for the degradation of a variety of problematic pollutants, and simultaneous US low and high frequencies can lead to improved degradation yields. Hydroxyl radical (·OH) is critical to the efficiency of ultrasonic oxidation processes. We monitored ·OH production and carried out calorimetric measurements during dual-frequency ultrasonic (DFU) irradiation using probe- (20 kHz) and transducer (640 kHz)-type sources. The conditions were optimized based on calorimetric measurements to determine real power density dissipation to the solution for our dual-frequency ultrasonic reactor (DFUR) (20 and 640 kHz) with a power density of 10.1  W·mL1 in which the observed synergistic index reached a maximum of 0.991, whereas it was only 4.1 and 8.1  W·mL1, respectively, for 20 and 640 kHz individually. The production of ·OH was measured using coumarin (COU) as trapping agent under simultaneous and sequential operation of low and high frequencies under different gas saturating conditions (Ar, O2, and N2). Distribution of ·OH within the cavitational zones was assessed by comparing ·OH trapping by hydrophobic COU and ionic terephthalic acid (TA) under DFU. Based on the approximately 6 times more effective trapping of ·OH by COU compared to TA during DFU irradiation, the majority of ·OH leading to degradation appears to be generated at the gas–liquid interface. Methylene blue (MB) and N, N-diethyl-meta-toluamide (DEET) were selected as hydrophilic and hydrophobic model target compounds to probe individual degradation zones within the cavitation process during DFU irradiation. The addition of peroxides H2O2 (PO), persulfate (PS), and monoperoxysulfate (MPS) to the DFU reactor had minimal or modest effects on the DFU-induced degradation of target compounds. The results revealed that combining low and high frequency US has a positive effect on enhancing the cavitational yields of ·OH and is favorable for treatment of both hydrophilic and hydrophobic compounds.

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Acknowledgments

This study was funded by The Scientific and Technological Research Council of Turkey (TUBITAK) and partially funded by NSF.

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Go to Journal of Environmental Engineering
Journal of Environmental Engineering
Volume 145Issue 10October 2019

History

Received: Dec 22, 2018
Accepted: Mar 18, 2019
Published online: Aug 13, 2019
Published in print: Oct 1, 2019
Discussion open until: Jan 13, 2020

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Dept. of Environmental Engineering, Ataturk Univ., Erzurum 25240, Turkey (corresponding author). ORCID: https://orcid.org/0000-0003-1633-2547. Email: [email protected]
Kevin O’Shea
Professor, Dept. of Chemistry and Biochemistry, Florida International Univ., Miami, FL 33199.

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