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 () is critical to the efficiency of ultrasonic oxidation processes. We monitored 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 in which the observed synergistic index reached a maximum of 0.991, whereas it was only 4.1 and , respectively, for 20 and 640 kHz individually. The production of was measured using coumarin (COU) as trapping agent under simultaneous and sequential operation of low and high frequencies under different gas saturating conditions (Ar, , and ). Distribution of within the cavitational zones was assessed by comparing trapping by hydrophobic COU and ionic terephthalic acid (TA) under DFU. Based on the approximately 6 times more effective trapping of by COU compared to TA during DFU irradiation, the majority of leading to degradation appears to be generated at the gas–liquid interface. Methylene blue (MB) and , -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 (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 and is favorable for treatment of both hydrophilic and hydrophobic compounds.
Get full access to this article
View all available purchase options and get full access to this article.
Acknowledgments
This study was funded by The Scientific and Technological Research Council of Turkey (TUBITAK) and partially funded by NSF.
References
Ashokkumar, M., J. Lee, S. Kentish, and F. Grieser. 2007. “Bubbles in an acoustic field: An overview.” Ultrason. Sonochem. 14 (4): 470–475. https://doi.org/10.1016/j.ultsonch.2006.09.016.
Brotchie, A., M. Ashokkumar, and F. Grieser. 2007. “Effect of water-soluble solutes on sonoluminescence under dual-frequency sonication.” J. Phys. Chem. C 111 (7): 3066–3070. https://doi.org/10.1021/jp067524r.
Brotchie, A., M. Ashokkumar, and F. Grieser. 2008a. “Sonochemistry and sonoluminescence under simultaneous high- and low-frequency irradiation.” J. Phys. Chem. C 112 (22): 8343–8348. https://doi.org/10.1021/jp8006987.
Brotchie, A., F. Grieser, and M. Ashokkumar. 2008b. “Sonochemistry and sonoluminescence under dual-frequency ultrasound irradiation in the presence of water-soluble solutes.” J. Phys. Chem. C 112 (27): 10247–10250. https://doi.org/10.1021/jp801763v.
Cui, D., A. M. Mebel, L. E. Arroya-Mora, C. Zhao, A. De Caprio, and K. O’shea. 2018. “Fundamental study of the ultrasonic induced degradation of the popular antihistamine, diphenhydramine (DPH).” Water Res. 144 (1): 265–273. https://doi.org/10.1016/j.watres.2018.07.032.
Dhaka, S., R. Kumar, S. Lee, M. B. Kurade, and B. H. Jeon. 2018. “Degradation of ethyl paraben in aqueous medium using advanced oxidation processes: Efficiency evaluation of UV-C supported oxidants.” J. Cleaner Prod. 180 (Apr): 505–513. https://doi.org/10.1016/j.jclepro.2018.01.197.
EPA. 2002. Federal water pollution control act. Washington, DC: USEPA.
Eren, Z. 2012. “Ultrasound as a basic and auxiliary process for dye remediation: A review.” J. Environ. Manage. 104 (Aug): 127–141. https://doi.org/10.1016/j.jenvman.2012.03.028.
Eren, Z., and N. H. Ince. 2010. “Sonolytic and sonocatalytic degradation of azo dyes by low and high frequency ultrasound.” J. Hazard. Mater. 177 (1–3): 1019–1024. https://doi.org/10.1016/j.jhazmat.2010.01.021.
Ferkous, H., O. Hamdaoui, and S. Merouani. 2015. “Sonochemical degradation of naphthol blue black in water: Effect of operating parameters.” Ultrason. Sonochem. 26 (Sep): 40–47. https://doi.org/10.1016/j.ultsonch.2015.03.013.
Ghaedi, M., S. Hajjati, Z. Mahmudi, I. Tyagi, S. Agarwal, A. Maity, and V. K. Gupta. 2015. “Modeling of competitive ultrasonic assisted removal of the dyes—Methylene blue and Safranin-O using nanoparticles.” Chem. Eng. J. 268 (May): 28–37. https://doi.org/10.1016/j.cej.2014.12.090.
Gielen, B., S. Marchal, J. Jordens, L. C. J. Thomassen, L. Braeken, and T. Van Gerven. 2016. “Influence of dissolved gases on sonochemistry and sonoluminescence in a flow reactor.” Ultrason. Sonochem. 31 (Jul): 463–472. https://doi.org/10.1016/j.ultsonch.2016.02.001.
Gogate, P. R., S. Mujumdar, J. Thampi, A. M. Wilhelm, and A. B. Pandit. 2004. “Destruction of phenol using sonochemical reactors: Scale up aspects and comparison of novel configuration with conventional reactors.” Sep. Purif. Technol. 34 (1–3): 25–34. https://doi.org/10.1016/S1383-5866(03)00171-0.
Gogate, P. R., V. S. Sutkar, and A. B. Pandit. 2011. “Sonochemical reactors: Important design and scale up considerations with a special emphasis on heterogeneous systems.” Chem. Eng. J. 166 (3): 1066–1082. https://doi.org/10.1016/j.cej.2010.11.069.
Gupta, V. K., I. Ali, T. A. Saleh, M. N. Siddiqui, and S. Agarwal. 2013. “Chromium removal from water by activated carbon developed from waste rubber tires.” Environ. Sci. Pollut. Res. 20 (3): 1261–1268. https://doi.org/10.1007/s11356-012-0950-9.
Gupta, V. K., C. K. Jain, I. Ali, S. Chandra, and S. Agarwal. 2002. “Removal of lindane and malathion from wastewater using bagasse fly ash sugar industry waste.” Water Res. 36 (10): 2483–2490. https://doi.org/10.1016/S0043-1354(01)00474-2.
Gupta, V. K., R. Jain, A. Nayak, S. Agarwal, and M. Shrivastava. 2011. “Removal of the hazardous dye—Tartrazine by photodegradation on titanium dioxide surface.” Mater. Sci. Eng. 31 (5): 1062–1067. https://doi.org/10.1016/j.msec.2011.03.006.
Gupta, V. K., A. Nayak, and S. Agarwal. 2015. “Bioadsorbents for remediation of heavy metals: Current status and their future prospects.” Environ. Eng. Res. 20 (1): 001–018. https://doi.org/10.4491/eer.2015.018.
Gupta, V. K., A. Nayak, S. Agarwal, and I. Tyagi. 2014. “Potential of activated carbon from waste rubber tire for the adsorption of phenolics: Effect of pre-treatment conditions.” J. Colloid Interface Sci. 417 (Mar): 420–430. https://doi.org/10.1016/j.jcis.2013.11.067.
Gupta, V. K., and T. A. Saleh. 2013. “Sorption of pollutants by porous carbon, carbon nanotubes and fullerene: An overview.” Environ. Sci. Pollut. Res. 20 (5): 2828–2843. https://doi.org/10.1007/s11356-013-1524-1.
Hirano, K., and T. Kobayashi. 2016. “Coumarin fluorometry to quantitatively detectable OH radicals in ultrasound aqueous medium.” Ultrason. Sonochem. 30 (May): 18–27. https://doi.org/10.1016/j.ultsonch.2015.11.020.
Iernetti, G., P. Ciuti, N. V. Dezhkunov, M. Reali, P. Ciuti, and A. Francescutto. 1997. “Enhancement of high-frequency acoustic cavitation effects by a low-frequency stimulation.” Ultrason. Sonochem. 4 (3): 263–268. https://doi.org/10.1016/S1350-4177(97)00034-5.
Ince, N. H. 2018. “Ultrasound-assisted advanced oxidation processes for water decontamination.” Ultrason. Sonochem. 40 (B): 97–103. https://doi.org/10.1016/j.ultsonch.2017.04.009.
Ince, N. H., G. Tezcanlı, R. K. Belen, and I. G. Apikyan. 2001. “Ultrasound as a catalyzer of aqueous reaction systems: The state of the art and environmental applications.” Appl. Catal. B 29 (3): 167–176. https://doi.org/10.1016/S0926-3373(00)00224-1.
Khani, H., M. K. Rofouei, P. Arab, V. K. Gupta, and Z. Vafaei. 2010. “Multi-walled carbon nanotubes-ionic liquid-carbon paste electrode as a super selectivity sensor: Application to potentiometric monitoring of mercury ion(II).” J. Hazard. Mater. 183 (1–3): 402–409. https://doi.org/10.1016/j.jhazmat.2010.07.039.
Kimura, T., T. Sakamoto, J. M. Leveque, H. Sohmiya, M. Fujita, S. Ikeda, and T. Ando. 1996. “Standardization of ultrasonic power for sonochemical reaction.” Ultrason. Sonochem. 3 (3): 157–161. https://doi.org/10.1016/S1350-4177(96)00021-1.
Lee, M., and J. Oh. 2011. “Synergistic effect of hydrogen peroxide production and sonochemiluminescence under dual frequency ultrasound irradiation.” Ultrason. Sonochem. 18 (3): 781–788. https://doi.org/10.1016/j.ultsonch.2010.11.022.
Manickam, S., N. Z. Abidin, S. Parthasarathy, I. Alzorqi, E. H. Ng, T. J. Tiong, R. L. Gomes, and A. Ali. 2014. “Role of in the fluctuating patterns of COD (chemical oxygen demand) during the treatment of palm oil mill effluent (POME) using pilot scale triple frequency ultrasound cavitation reactor.” Ultrason. Sonochem. 21 (Jul): 1519–1526. https://doi.org/10.1016/j.ultsonch.2014.01.002.
Mason, T. J. 1999. An introduction to the uses of power ultrasound in chemistry: Sonochemistry. New York: Oxford University Press.
Mason, T. J., and J. P. Lorimer. 2002. The uses of power ultrasound in chemistry and processing: Applied Sonochemistry. Weinheim, Germany: Wiley.
Mason, T. J., J. P. Lorimer, and D. M. Bates. 1992. “Quantifying sonochemistry: Casting some light on a ‘black art’.” Ultrasonics 30 (1): 40–42. https://doi.org/10.1016/0041-624X(92)90030-P.
Medel, A., J. A. Ramirez, J. Cardenas, I. Sires, and Y. Meas. 2019. “Evaluating the electrochemical and photoelectrochemical production of hydroxyl radical during electrocoagulation process.” Sep. Prufi. Technol. 208 (Jan): 59–67. https://doi.org/10.1016/j.seppur.2018.05.021.
Merouani, S., H. Ferkous, O. Hamdaoui, Y. Rezgui, and M. Guemini. 2015. “New interpretation of the effects of argon-saturating gas toward sonochemical reactions.” Ultrason. Sonochem. 23 (Mar): 37–45. https://doi.org/10.1016/j.ultsonch.2014.09.009.
Mittal, A., J. Mittal, A. Malviya, and V. K. Gupta. 2010. “Removal and recovery of Chrysoidine Y from aqueous solutions by waste materials.” J. Colloid Interface Sci. 344 (2): 497–507. https://doi.org/10.1016/j.jcis.2010.01.007.
Mohammadi, N., H. Khani, V. K. Gupta, E. Amereh, and S. Agarwal. 2011. “Adsorption process of methyl orange dye onto mesoporous carbon material–kinetic and thermodynamic studies.” J. Colloid Interface Sci. 362 (2): 457–462. https://doi.org/10.1016/j.jcis.2011.06.067.
Page, S. E., W. A. Arnold, and K. McNeill. 2010. “Terephthalate as a probe for photochemically generated hydroxyl radical.” J. Environ. Monit. 12 (9): 1658–1665. https://doi.org/10.1039/c0em00160k.
Prabhu, A. V., P. R. Gogate, and A. B. Pandit. 2004. “Optimization of multiple-frequency sonochemical reactors.” Chem. Eng. Sci. 59 (22–23): 4991–4998. https://doi.org/10.1016/j.ces.2004.09.033.
Rahimi, M., S. Safari, M. Faryadi, and N. Moradi. 2014. “Experimental investigation on proper use of dual high-low frequency ultrasound waves: Advantage and disadvantage.” Chem. Eng. Process. 78 (Apr): 17–26. https://doi.org/10.1016/j.cep.2014.02.003.
Rooze, J., E. V. Rebrov, J. C. Schouten, and T. F. Keurentjes. 2013. “Dissolved gas and ultrasonic cavitation: A review.” Ultrason. Sonochem. 20 (1): 1–11. https://doi.org/10.1016/j.ultsonch.2012.04.013.
Saleh, T. A., and V. K. Gupta. 2011. “Functionalization of tungsten oxide into MWCNT and its application for sunlight-induced degradation of rhodamine B.” J. Colloid Interface Sci. 362 (2): 337–344. https://doi.org/10.1016/j.jcis.2011.06.081.
Saleh, T. A., and V. K. Gupta. 2012. “Photo-catalyzed degradation of hazardous dye methyl orange by use of a composite catalyst consisting of multi-walled carbon nanotubes and titanium dioxide.” J. Colloid Interface Sci. 371 (1): 101–106. https://doi.org/10.1016/j.jcis.2011.12.038.
Saravanan, R., S. Karthikeyan, V. K. Gupta, G. Sekaran, V. Narayanan, and A. Stephen. 2013a. “Enhanced photocatalytic activity of ZnO/CuO nanocomposite for the degradation of textile dye on visible light illumination.” Mater. Sci. Eng. C 33 (1): 91–98. https://doi.org/10.1016/j.msec.2012.08.011.
Saravanan, R., S. Joicy, V. K. Gupta, V. Narayanan, and A. Stephen. 2013b. “Visible light induced degradation of methylene blue using and catalysts.” Mater. Sci. Eng. C 33 (8): 4725–4731. https://doi.org/10.1016/j.msec.2013.07.034.
Saravanan, R., N. Karthikeyan, V. K. Gupta, E. Thirumal, P. Thangadurai, V. Narayanan, and A. Stephen. 2013c. “ZnO/Ag nanocomposite: An efficient catalyst for degradation studies of textile effluents under visible light.” Mater. Sci. Eng. C 33 (4): 2235–2244. https://doi.org/10.1016/j.msec.2013.01.046.
Saravanan, R., M. M. Khan, V. K. Gupta, E. Mosquera, F. Gracia, V. Narayanan, and A. Stephen. 2015. “ZnO/Ag/CdO nanocomposite for visible light-induced photocatalytic degradation of industrial textile effluents.” J. Colloid Interface Sci. 452 (Aug): 126–133. https://doi.org/10.1016/j.jcis.2015.04.035.
Shaida, M. A., A. K. Sen, and R. K. Dutta. 2018. “Alternate use of sulphur rich coals as solar photo-Fenton agent for degradation of toxic azo dyes.” J. Cleaner Prod. 195 (Sep): 1003–1014. https://doi.org/10.1016/j.jclepro.2018.05.286.
Siddique, M., R. Farooq, and G. J. Price. 2014. “Synergistic effects of combining ultrasound with the Fenton process in the degradation of Reactive Blue 19.” Ultrason. Sonochem. 21 (3): 1206–1212. https://doi.org/10.1016/j.ultsonch.2013.12.016.
Song, W., W. J. Cooper, B. M. Peake, S. P. Mezyk, M. G. Nickelsen, and K. E. O’shea. 2009. “Free radical induced oxidative and reductive degradation of -diethyl-m-toluamide (DEET): Kinetic studies and degradation pathway.” Water Res. 43 (3): 635–642. https://doi.org/10.1016/j.watres.2008.11.018.
Suslick, K. S. 1990. “Sonochemistry.” Science 247 (4949): 1439–1445. https://doi.org/10.1126/science.247.4949.1439.
Torres, A., C. Petrier, E. Combet, M. Carrier, and C. Pulgarin. 2008. “Ultrasonic cavitation applied to the treatment of bisphenol A. Effect of sonochemical parameters and analysis of BPA by-products.” Ultrason. Sonochem. 15 (4): 605–611. https://doi.org/10.1016/j.ultsonch.2007.07.003.
Xiao, R., D. Diaz-Rivera, Z. He, and L. K. Weavers. 2013. “Using pulsed wave ultrasound to evaluate the suitability of hydroxyl radical scavengers in sonochemical systems.” Ultrason. Sonochem. 20 (3): 990–996. https://doi.org/10.1016/j.ultsonch.2012.11.012.
Xu, Z., and K. Yasuda. 2011. “Enhancement of sonochemical reaction by dual-pulse ultrasound.” Jpn. J. Appl. Phys. 50 (7S): 07HE07. https://doi.org/10.7567/JJAP.50.07HE07.
Yasui, K., T. Tuziuti, T. Kozuka, A. Towata, and Y. Iida. 2007. “Relationship between the bubble temperature and main oxidant created inside an air bubble under ultrasound.” J. Chem. Phys. 127 (15): 154502. https://doi.org/10.1063/1.2790420.
Information & Authors
Information
Published In
Copyright
©2019 American Society of Civil Engineers.
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
Authors
Metrics & Citations
Metrics
Citations
Download citation
If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.