Generic placeholder image

Current Analytical Chemistry

Editor-in-Chief

ISSN (Print): 1573-4110
ISSN (Online): 1875-6727

Research Article

Application of Oxides Electrodes (Ru, Ti, Ir and Sn) for the Electrooxidation of Levofloxacin

Author(s): Juliane C. Forti*, Robson S. Rocha, Adalgisa R. De Andrade and Marcos R.V. Lanza

Volume 15, Issue 1, 2019

Page: [66 - 74] Pages: 9

DOI: 10.2174/1573411013666180705142302

Price: $65

Abstract

Background: The main sources of antibiotic pollution are industries, hospitals, and urban effluents, as well as wastewater from farms that use antibiotics for veterinary purposes. Fluoroquinolones are very useful as antimicrobial agents and are probably among the most important classes of synthetic antibiotics in veterinary and human medicines worldwide. Despite this relevance, studies on the analysis of fluoroquinolones in wastewaters and alternative processes to degrade these compounds, and their effects on human health and environment are scarce. Here, we prepared different oxide electrodes (Ti/Ru0.3Ti0.7O2, Ti/Ru0.3Sn0.7O2, Ti/Ir0.3Ti0.7O2, and Ti/Ir0.3Sn0.7O2) and used them in the electrochemical oxidation of levofloxacin, an antibiotic belonging to the class of fluoroquinolones.

Methods: The oxide electrodes with nominal compositions: Ti/Ru0.3Ti0.7O2, Ti/Ru0.3Sn0.7O2, Ti/Ir0.3Ti0.7O2, and Ti/Ir0.3Sn0.7O2 were prepared by the traditional method. Briefly, the precursor solution was dissolved in isopropanol and applied by brushing on both sides of the titanium substrate. The resulting material was thermally decomposed at 400°C for 5 min in a preheated oven, which was followed by cooling. This procedure was repeated until the desired oxide thickness was achieved (2 mm). Using the electrochemical cell, the electrolysis experiments were carried out by applying current densities of 25, 50, and 100 mA cm-2 on the oxide electrodes for 60 min. During this experiment, aliquots were removed at times: 5, 10, 15, 20, 30, 45 and 60 min for quantification. Levofloxacin was quantitatively determined by High-Performance Liquid Chromatography (HPLC).

Results: The catalytic efficiency of different electrodes is measured as the yield of levofloxacin degradation, which in most cases reaches 50% within 1 h of electrolysis, regardless of the applied current. The electrodes bearing ruthenium afford the same % residual levofloxacin (18%) after 1 h of electrolysis under 100 mA cm-2. The electrodes that contain iridium provide similar results at all the applied currents, being less efficient as compared to the ruthenium-based electrodes. The electrode Ti/Ru0.3Sn0.7O2 presented the highest levofloxacin degradation value (levofloxacin residual is 8% at 50 mA cm-2) and levofloxacin removal rate was calculated considering order 1 kinetics (-lnC/Co=kt), for each of the applied current densities reaching 4.4, 4.9 and 4.5 mg L-1min-1 for the experiments at 25, 50, 100 mA cm-2. Therefore, the Ti/Ru0.3Sn0.7O2 electrode affords the highest yield and the best cost/benefit ratio.

Conclusion: In this work, electrodes were prepared with different compositions to study the catalytic efficiency in the degradation of levofloxacin, an antibiotic belonging to the class of fluoroquinolones. The mixed oxide electrodes prepared herein have proven to be an efficient alternative to treat effluents contaminated with organic compounds. The electrode containing RuO2 and SnO2 oxidizes levofloxacin the most efficiently, reaching a removal efficiency of 92% (4.9 mg L-1 min-1) under 50 mA cm-2. Hence, the substitution of Ti for Sn generates better degradation efficiency.

Keywords: Antibiotics, electrooxidation, levofloxacin, oxides electrodes, fluoroquinolones, antimicrobial agents.

Graphical Abstract
[1]
Godoy, A.A.; Kummrow, F.; Pamplin, P.A.Z. Occurrence, ecotoxicological effects and risk assessment of antihypertensive pharmaceutical residues in the aquatic environment - A review. Chemosphere, 2015, 138, 281-291.
[2]
Magureanu, M.; Mandache, N.B.; Parvulescu, V.I. Degradation of pharmaceutical compounds in water by non-thermal plasma treatment. Water Res., 2015, 81, 124-136.
[3]
Patneedi, C.B.; Durga, P.; Chanti, B.R. Impact of pharmaceutical wastes on human life and environment. J. Chem., 2015, 8(1), 67-70.
[4]
Taylor, D.; Senac, T. Human pharmaceutical products in the environment - The “problem” in perspective. Chemosphere, 2014, 115, 95-99.
[5]
Adachi, F.; Yamamoto, A.; Takakura, K-I.; Kawahara, R. Occurrence of fluoroquinolones and fluoroquinolone-resistance genes in the aquatic environment. Sci. Total Environ., 2013, 444, 508-514.
[6]
Lu, Z.; Na, G.; Gao, H.; Wang, L.; Bao, C.; Yao, Z. Fate of sulfonamide resistance genes in estuary environment and effect of anthropogenic activities. Sci. Total Environ., 2015, 527-528, 429-438.
[7]
Wang, J.; Mao, D.; Mu, Q.; Luo, Y. The fate and proliferation of typical antibiotic resistance genes in five full-scale pharmaceutical wastewater treatment plants. Sci. Total Environ., 2015, 526, 366-373.
[8]
Batt, A.L.; Bruce, I.B.; Aga, D.S. Evaluating the vulnerability of surface waters to antibiotic contamination from varying wastewater treatment plant discharges. Environ. Pollut., 2006, 142, 295-302.
[9]
Brown, K.D.; Kulis, J.; Thomson, B.; Chapman, T.H.; Mawhinney, D.B. Occurrence of antibiotics in the hospital, residential, and dairy effluent, municipal wastewater, and the Rio Grande in New Mexico. Sci. Total Environ., 2006, 366, 772-783.
[10]
Mompelat, S.; Le Bot, B.; Thomas, O. Occurrence, and fate of pharmaceutical products and by-products, from resource to drinking water. Environ. Int., 2009, 35, 803-814.
[11]
Speltini, A.; Sturini, M.; Maraschi, F.; Viti, S.; Sbarbada, D.; Profumo, A. Fluoroquinolone residues in compost by green enhanced microwave-assisted extraction followed by ultra-performance liquid chromatography-tandem mass spectrometry. J. Chromatogr. A, 2015, 1410, 44-50.
[12]
Picó, Y.; Andreu, V. Fluoroquinolones in soil-risks and challenges. Anal. Bioanal. Chem., 2007, 387, 1287-1299.
[13]
Van Doorslaer, X.; Dewulf, J.; Van Langenhove, H.; Demeestere, K. Fluoroquinolone antibiotics: An emerging class of environmental micropollutants. Sci. Total Environ., 2014, 500-501, 250-269.
[14]
Andreozzi, R.; Raffaele, M.; Nicklas, P. Pharmaceuticals in STP effluents and their solar photodegradation in the aquatic environment. Chemosphere, 2003, 50(10), 1319-1330.
[15]
Rosendahl, I.; Siemens, J.; Kindler, R.; Groeneweg, J.; Zimmermann, J.; Czerwinski, S.; Lamshöft, M.; Laabs, V.; Wilke, B-M.; Vereecken, H.; Amelung, W. Persistence of the fluoroquinolone antibiotic difloxacin in soil and lacking effects on nitrogen turnover. J. Environ. Qual., 2012, 41, 1275-1283.
[16]
Calisto, V.; Esteves, V.I. Psychiatric pharmaceuticals in the environment. Chemosphere, 2009, 77, 1257-1274.
[17]
Le-Minh, N.; Khan, S.J.; Drewes, J.E.; Stuetz, R.M. Fate of antibiotics during municipal water recycling treatment processes. Water Res., 2010, 44(15), 4295-4323.
[18]
Barros, W.R.P.; Borges, M.P.; Steter, J.R.; Forti, J.C.; Rocha, R.S.; Lanza, M.R.V. Degradation of dipyrone by electrogenerated H2O2 Combined with Fe2+ using a modified gas diffusion electrode. J. Electrochem. Soc., 2014, 161(14), H867-H873.
[19]
Eleotério, I.C.; Forti, J.C.; Andrade, A.R. Electrochemical treatment of wastewater of veterinary industry containing antibiotics. Electrocatalysis, 2013, 4, 283-289.
[20]
Fornazaria, A.L. de T. Aquino Neto, S.; Andrade, A.R.; Miwa, D.W.; Motheo A.J.; Malpassa, G.R.P. Materiais de composição Ti/PbxTi1-XO2 para degradação eletroquímica foto-assistida de poluentes orgânicos. Quim. Nova, 2016, 39(5), 535-541.
[21]
Hu, Y.; Nagai, Y.; Rahmawaty, D. Characteristics of the photocatalytic oxidation of methane into methanol on V-Containing MCM-41 Catalysts. Catal. Lett., 2008, 124, 80-84.
[22]
Wang, C.B.; Herman, R.G.; Shi, C.; Roberts, J.E.V. 2O5-SiO2 xerogels for methane oxidation to oxygenates: preparation, characterization, and catalytic properties. Appl. Catal. A., 2003, 247(2), 321-333.
[23]
Zhang, Q.; He, D.; Han, Z.; Zhang, X.; Zhu, Q. Controlled partial oxidation of methane to methanol/formaldehyde over Mo-V-Cr-Bi-Si oxide catalysts. Fuel, 2002, 81, 1599-1603.
[24]
Indarto, A. A review of direct methane conversion to methanol by a dielectric barrier discharge. IEEE Trans. Dielectr. Electr. Insul., 2008, 15, 1038-1043.
[25]
Holmen, A. Direct conversion of methane to fuels and chemicals. Catal. Today, 2009, 142, 2-8.
[26]
Khokhar, M.D.; Shukla, R.S.; Jasra, R.V. Selective oxidation of methane by molecular oxygen catalyzed by a bridged binuclear ruthenium complex at moderate pressures and ambient temperature. J. Mol. Catal A. Chem., 2009, 299, 108-116.
[27]
Coteiro, R.D.; Andrade, A.R. Electrochemical oxidation of 4-chlorophenol and its by-products using Ti/Ru0.3M0.7O2 (M = Ti or Sn) anodes: preparation route versus degradation efficiency. J. Appl. Electrochem., 2007, 37, 691-698.
[28]
Forti, J.C.; Olivi, P.; Andrade, A.R. Characterisation of DSA®-type coatings with nominal composition Ti/Ru0.3Ti(0.7−x)SnxO2 prepared via a polymeric precursor. Electrochim. Acta, 2001, 47, 913-920.
[29]
Forti, J.C.; Ribeiro, J.; Lanza, M.R.V.; Andrade, A.R.; Bertazzoli, R. Electrochemical Characterization of DSA®-Type Electrodes Using Niobium Substrate. Electrocatalysis, 2010, 1, 129-138.
[30]
Forti, J.C.; Andrade, A.R. Formaldehyde oxidation on a DSA-type electrode modified by Pt or PbO2 electrodeposition. J. Electrochem. Soc., 2007, 154(1), E19-E24.
[31]
Colombo, R.; Ferreira, T.C.R.; Ferreira, R.A.; Lanza, M.R.V. Removal of Mefenamic acid from aqueous solutions by oxidative process: Optimization through experimental design and HPLC/UV analysis. J. Environ. Manage., 2016, 167, 206-213.
[32]
Trasatti, S. Electrochemistry of Novel Materials; Trasatti, S., eds.; Jacek Lipkowski e Philip N. Ross: New York, 1994.
[33]
Lassali, T.A.F.; Castro, C.De; Boodts, J.F.C. Structural, morphological and surface properties as a function of the composition of Ru+Ti+Pt mixed-oxide electrodes. Electrochim. Acta, 1998, 43(16-17), 2515-2525.
[34]
Ribeiro, J.; Alves, P.D.P.; de Andrade, A.R. Effect of the preparation methodology on some physical and electrochemical properties of Ti/IrxSn(1-x)O2 materials. J. Mater. Sci., 2007, 42(22), 9293-9299.
[35]
Panizza, M.; Cerisola, G. Application of diamond electrodes to electrochemical processes. Electrochim. Acta, 2005, 51, 191-199.

Rights & Permissions Print Cite
© 2024 Bentham Science Publishers | Privacy Policy