Cavitation-Induced Oxidative Deterioration of Amoxicillin in Aqueous Solutions

Abstract

Antibiotics are ecotoxicants and pose a potential risk to aquatic environments. Given their regular detection in wastewater, it is imperative to develop effective methods for their degradation. Advanced oxidation processes are actively researched and implemented as a means of oxidizing persistent organic pollutants, including antibiotics, in aquatic environments. Their efficacy is achieved through the intense formation of reactive oxygen species. In the article, a laboratory setup was designed and constructed, demonstrating the feasibility of implementing the oxidative degradation process of the antibiotic Amoxicillin using persulfate under the simultaneous influence of hydrodynamic cavitation and acoustic cavitation --- HAC. Kinetic patterns and optimal conditions for the oxidative degradation and mineralization of Amoxicillin in model aqueous solutions were established. A comparative assessment of individual, combined, and hybrid oxidative systems was provided. The maximum degree of degradation (90 %) and mineralization of Amoxicillin (33 %) was achieved only in the hybrid HAC/PS/Fe²⁺ system. Experimentally using radical inhibition methods, it was proven that both SO₄^•– and HO^• radicals participate in the oxidation of Amoxicillin in the hybrid HAC/PS/Fe²⁺ system. An assessment of the toxicity of the oxidative degradation products of AMX was provided through biotesting methods. The obtained data characterizing the hybrid HAC/PS/Fe²⁺ system demonstrate significant potential for the effective oxidative degradation of biorefractory organic pollutants and can be utilized in the scale-up process during pilot trials

The work was carried out within the framework of the State Assignment of the Baikal Institute of Nature Management of the Siberian Branch, Russian Academy of Sciences (project FWSU-2021-0006) using the equipment of the Collective Use Center of the Baikal Institute of Nature Management of the Siberian Branch, Russian Academy of Sciences

Please cite this article in English as:

Aseev D.G. Cavitation-induced oxidative deterioration of Amoxicillin in aqueous solutions. Herald of the Bauman Moscow State Technical University, Series Natural Sciences, 2024, no. 6 (117), pp. 55--71 (in Russ.). EDN: DGXJEJ

References

[1] Watkinson A.J., Murby E.J., Costanzo S.D. Removal of antibiotics in conventional and advanced wastewater treatment: implications for environmental discharge and wastewater recycling. Water Res., 2007, vol. 41, iss. 18, pp. 4164--4176. DOI: https://doi.org/10.1016/j.watres.2007.04.005

[2] Martinez J.L. Environmental pollution by antibiotics and by antibiotic resistance determinants. Environ. Pollut., 2009, vol. 157, iss. 11, pp. 2893--2902. DOI: https://doi.org/10.1016/j.envpol.2009.05.051

[3] Bergamonti L., Bergonzi C., Graiff C., et al. 3D printed chitosan scaffolds: a new TiO₂ support for the photocatalytic degradation of amoxicillin in water. Water Res., 2019, vol. 163, art. 114841. DOI: https://doi.org/10.1016/j.watres.2019.07.008

[4] Kovalakova P., Cizmas L., McDonald T.J., et al. Occurrence and toxicity of antibiotics in the aquatic environment: a review. Chemosphere, 2020, vol. 251, art. 126351. DOI: https://doi.org/10.1016/j.chemosphere.2020.126351

[5] Miklos D.B., Remy C., Jekel M., et al. Evaluation of advanced oxidation processes for water and wastewater treatment --- a critical review. Water Res., 2018, vol. 139, pp. 118--131. DOI: https://doi.org/10.1016/j.watres.2018.03.042

[6] Yin R., Chen Y., He S., et al. In situ photoreduction of structural Fe(III) in a metal-organic framework for peroxydisulfate activation and efficient removal of antibiotics in real wastewater. J. Hazard. Mater., 2020, vol. 388, art. 121996. DOI: https://doi.org/10.1016/j.jhazmat.2019.121996

[7] Andreozzi R., Caprio V., Insola A., et al. Advanced oxidation processes (AOP) for water purification and recovery. Catal. Today, 1999, vol. 53, no. 1, pp. 51--59. DOI: https://doi.org/10.1016/S0920-5861(99)00102-9

[8] Brillas E., Sires I., Oturan M.A. Electro-Fenton process and related electrochemical technologies based on Fenton’s reaction chemistry. Chem. Rev., 2009, vol. 109, iss. 12, pp. 6570--6631. DOI: https://doi.org/10.1021/cr900136g

[9] Fang Y., Hariuv D., Yamamoto T., et al. Acoustic cavitation assisted plasma for wastewater treatment: degradation of Rhodamine B in aqueous solution. Ultrason. Sonochem., 2019, vol. 52, pp. 318--325. DOI: https://doi.org/10.1016/j.ultsonch.2018.12.003

[10] Dewil R., Mantzavinos D., Poulios I., et al. New perspectives for advanced oxidation processes. J. Environ. Manag., 2017, vol. 195, part 2, pp. 93--99. DOI: https://doi.org/10.1016/j.jenvman.2017.04.010

[11] Tufail A., Price W.E., Hai F.I. A critical review on advanced oxidation processes for the removal of trace organic contaminants: a voyage from individual to integrated processes. Chemosphere, 2020, vol. 260, art. 127460. DOI: https://doi.org/10.1016/j.chemosphere.2020.127460

[12] Cravotto G., Gaudino E.C., Cintas P. On the mechanochemical activation by ultrasound. Chem. Soc. Rev., 2013, vol. 42, iss. 18, pp. 7521--7534. DOI: https://doi.org/10.1039/C2CS35456J

[13] Adewuyi Y.G. Sonochemistry: environmental science and engineering applications. Ind. Eng. Chem. Res., 2001, vol. 40, iss. 22, pp. 4681--4715. DOI: https://doi.org/10.1021/ie010096l

[14] Panda D., Saharan V.K., Manickam S. Controlled hydrodynamic cavitation: a review of recent advances and perspectives for greener processing. Processes, 2020, vol. 8, iss. 2, art. 220. DOI: https://doi.org/10.3390/pr8020220

[15] Bethi B., Sonawane S., Bhanvase B. Role of process intensification by ultrasound. In: Handbook of Ultrasonics and Sonochemistry. Singapore, Springer, 2016, pp. 841--866. DOI: https://doi.org/10.1007/978-981-287-278-4_59

[16] Calcio Gaudino E., Canova E., Liu P., et al. Degradation of antibiotics in wastewater: new advances in cavitational treatments. Molecules, 2021, vol. 26, iss. 3, art. 617. DOI: https://doi.org/10.3390/molecules26030617

[17] Wu Z., Yuste-Cordoba F.J., Cintas P., et al. Effects of ultrasonic and hydrodynamic cavitation on the treatment of cork wastewater by flocculation and Fenton processes. Ultrason. Sonochem., 2018, vol. 40, part B, pp. 3--8. DOI: https://doi.org/10.1016/j.ultsonch.2017.04.016

[18] Braeutigam P., Franke M., Schneider R.J., et al. Degradation of carbamazepine in environmentally relevant concentrations in water by Hydrodynamic-Acoustic-Cavitation (HAC). Water Res., 2012, vol. 46, iss. 7, pp. 2469--2477. DOI: https://doi.org/10.1016/j.watres.2012.02.013

[19] Hassani A., Scaria J., Ghanbari F., et al. Sulfate radicals-based advanced oxidation processes for the degradation of pharmaceuticals and personal care products: a review on relevant activation mechanisms, performance, and perspectives. Environ. Res., 2023, vol. 217, art. 114789. DOI: https://doi.org/10.1016/j.envres.2022.114789

[20] Matzek L.W., Carter K.E. Activated persulfate for organic chemical degradation: a review. Chemosphere, 2016, vol. 151, pp. 178--188. DOI: https://doi.org/10.1016/j.chemosphere.2016.02.055

[21] Lakshmi N.J., Gogate P.R., Pandit A.B. Treatment of acid violet 7 dye containing effluent using the hybrid approach based on hydrodynamic cavitation. Process Saf. Environ. Prot., 2021, vol. 153, pp. 178--191. DOI: https://doi.org/10.1016/j.psep.2021.07.023

[22] Danilov V.S., Zarubina A.P., Eroshnikov G.E., et al. Sensor bioluminescent systems based on lux-operons of different species of luminescent bacteria. Vestnik Moskovskogo Universiteta. Ser. 16. Biologiya, 2002, no. 3, pp. 20--24 (in Russ.).

[23] Yuefei J., Ferronato C., Salvador A., et al. Degradation of ciprofloxacin and sulfamethoxazole by ferrous-activated persulfate: Implications for remediation of groundwater contaminated by antibiotics. Sci. Total Environ., 2014, vol. 472, pp. 800--808. DOI: https://doi.org/10.1016/j.scitotenv.2013.11.008

[24] Wang J., Wang S. Activation of persulfate (PS) and peroxymonosulfate (PMS) and application for the degradation of emerging contaminants. Chem. Eng. J., 2018, vol. 334, pp. 1502--1517. DOI: https://doi.org/10.1016/j.cej.2017.11.059

[25] Xu X., Bao T. Research on the removal of near-well blockage caused by asphaltene deposition using sonochemical method. Ultrason. Sonochem., 2020, vol. 64, art. 104918. DOI: https://doi.org/10.1016/j.ultsonch.2019.104918

[26] Xu X., Karami B., Shahsavari D. Time-dependent behavior of porous curved nanobeam. Int. J. Eng. Sci., 2021, vol. 160, art. 103455. DOI: https://doi.org/10.1016/j.ijengsci.2021.103455

[27] Binota T., Aniruddha B.P., Qiu P. A review on sonoelectrochemical technology as an upcoming alternative for pollutant degradation. Ultrason. Sonochem., 2015, vol. 27, pp. 210--234. DOI: https://doi.org/10.1016/j.ultsonch.2015.05.015

[28] Bu L., Shi Z., Zhou S. Modeling of Fe(II)-activated persulfate oxidation using atrazine as a target contaminant. Sep. Purif. Technol., 2016, vol. 169, pp. 59--65. DOI: https://doi.org/10.1016/j.seppur.2016.05.037

[29] Zhang, Y., Xiao, Y., Zhong Y., et al. Comparison of amoxicillin photodegradation in the UV/H₂O₂ and UV/persulfate systems: reaction kinetics, degradation path-ways, and antibacterial activity. Chem. Eng. J., 2019, vol. 372, pp. 420--428. DOI: https://doi.org/10.1016/j.cej.2019.04.160

[30] Wojnarovits L., Toth T., Takacs E. Critical evaluation of rate coefficients for hydroxyl radical reactions with antibiotics: a review. Crit. Rev. Environ. Sci. Technol., 2018, vol. 48, iss. 6, pp. 575--613. DOI: https://doi.org/10.1080/10643389.2018.1463066

[31] Chang K., Lim T.M., Tsen L., et al. Photocatalytic degradation and mineralization of bisphenol A by TiO₂ and platinized TiO₂. Appl. Catal. A Gen., 2004, vol. 261, iss. 4, pp. 225--237. DOI: https://doi.org/10.1016/j.apcata.2003.11.004