Degradation and Mineralization of Metformin by Electro-Oxidation on Ti/DSA (Ta2O5-Ir2O5) Anode and Combined Electro-Oxidation and Electro-Coagulation on Stainless Steel (SS) Anode

Document Type : Research Article

Authors

Department of Chemical Engineering, Sant Longowal Institute of Engineering and Technology, Longowal, Sangrur, Punjab, INDIA

Abstract

We conducted electro-oxidation, and combined electro-oxidation and electro-coagulation batch experiments on synthetic wastewater containing an anti-diabetic drug metformin hydrochloride (MET-HCl). Degradation and mineralization were studied on Ti/DSA (Ta2O5-Ir2O5) and stainless steel (SS) anodes. Electrochemical behavior was observed by cyclic voltammetry techniques. The effect of applied current density was evaluated at 50 ppm concentration of supporting electrolyte sodium sulphate (Na2SO4). Electro-oxidation on Ti/DSA anode resulted in maximum degradation of 94.88% at the corresponding specific charge (Q) of 2.1 Ah/L, current density of 0.93 mA/cm2 and Na2SO4 concentration of 100 ppm. Similarly, maximum mineralization obtained was 70.64% at corresponding specific charge (Q) of 2.1 Ah/L, current density of 0.93 mA/cm2 and Na2SO4 concentration of 50 ppm. Energy consumption was 2081.56 kWh/kgTOC. Further, under identical conditions, combined electro-oxidation and electro-coagulation on SS anode resulted in maximum degradation of 99.48% at corresponding specific charge (Q) of 2.1 Ah/L, current density of 0.93 mA/cm2 and Na2SO4 concentration of 100 ppm. Similarly, maximum mineralization obtained was 99.04% at corresponding specific charge (Q) of 2.1 Ah/L, current density of 0.93 mA/cm2, and Na2SO4 concentration 75 ppm. Energy consumption was 870.98 kWh/kgTOC.

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References

[1] Viollet B., Guigas B., Garcia N.S., Leclerc J., Foretz M., Andreelli F., Cellular and Molecular Mechanisms of Metformin: An Overview, Clin. Sci., 122: 253 (2012).
[2] Zhu S., Liu Y.G.,  Liu S.B., Zeng G.M., Jiang .LH., Tan X.F., Zhou L., Zeng W., Li T.T., Yang C.P., Adsorption of Emerging Contaminant Metformin using Graphene Oxide, Chemosphere, 179: 20 (2017).
[3] Orona-Navar C., Garcia-Morales R., Rubio-Govea R., Mahlknecht J., Hernandez-Aranda R.I., Ramirez J.G., Nigam K.D.P., Ornelas-Soto N.,  Adsorptive Removal of Emerging Pollutants from Groundwater by Using Modified Titanate Nanotubes, Journal of Environmental Chemical Engineering, 6: 5332 (2018).
[4] Lesser L.E., Mora A., Moreau C., Mahlknecht J., Hernández-Antonio A., Ramírez A.I., Barrios-Piña H., Survey of 218 Organic Contaminants in Groundwater Derived from the world’s Largest Untreated Wastewater Irrigation System: Mezquital Valley, Mexico, Chemosphere, 198: 510 (2018).
[5] Oliveira T.S., Murphy M., Mendola N., Wong V., Carlson D., Waring L.,  Characterization of Pharmaceuticals and Personal Care Products in Hospital Effluent and Waste Water Influent/Effluent by Direct-Injection LC-MS-MS, Sci. Total Environ, 518–519: 459 (2015).
[6] Scheurer M., Michel A., Brauch H.J., Ruck W., Sacher F., Occurrence and Fate of the Antidiabetic Drug Metformin and its Metabolite Guanylurea in the Environment and During Drinking Water Treatment, Water Res., 46: 4790 (2012). 
[7] Kim M., Guerra P., Shah A., Parsa M., Alaee M., Smyth S.A., Removal of Pharmaceuticals and Personal Care Products in a Membrane Bioreactor Wastewater Treatment Plant, Water Sci. Technol, 69(11): 2221 (2014).
[8] USEPA, Targeted National Sewage Sludge Survey Sampling and Analysis Technical Report (Vol. EPA-822-R-), USEPA, Washington, DC, (2009).
[9] Oosterhuis M., Sacher F., Laak T.L.T., Prediction of Concentration Levels of Metformin and other High Consumption Pharmaceuticals in Wastewater and Regional Surface Water Based on Sales Data, Sci. Total. Environ., 442: 380 (2013). 
[10] Trautwein C., Berset J.D., Wolschke H., Kümmerer K., Occurrence of the Antidiabetic Drug Metformin and its Ultimate Transformation Product Guanylurea in Several Compartments of the Aquatic Cycle, Environ. Int. ,70: 203 (2014). 
[11] Ghoshdastidar A.J., Fox S., Tong A.Z., The Presence of the Top Prescribed Pharmaceuticals in Treated Sewage Effluents and Receiving Waters in Southwest Nova Scotia, Canada, Environ. Sci. Pollut. Res., 22: 689 (2015).
[12] Aseman-Bashiz E., Sayyaf H.,  Metformin Degradation in Aqueous Solutions by Electro-Activation of Persulfate and Hydrogen using Natural and Synthetic Ferrous Ion Sources, Journal of Molecular liquids, 300: 112285 (2020).
[13] Cunningham V.L., “Pharmaceuticals in the Environment: Sources, Fate, Effects and Risks”, Springer Berlin, (2008).
[14] Nikolaou A., Meric S., Fatta D., Occurrence Patterns of Pharmaceuticals in Water and Wastewater Environments, Anal. Bioanal.  Chem., 387(4):  1225 (2007).
[15] Benotti M.J., Brownawell B.J., Distributions of Pharmaceuticals in An Urban Estuary During both Dry- and Wet-Weather Conditions, Environ. Sci. Technol., 41: 5795 (2007).
[16] Debska J., Kot-Wasik A., Namiesnik J., Fate and Analysis of Pharmaceutical Residues in the Aquatic Environment, Crit. Rev. Anal. Chem, 34(1): 51 (2004).
[17] Joss A., Siegrist  H., Ternes T.A., Are We About to Upgrade Wastewater Treatment for Removing Organic Micropollutants? Water Sci. Technol, 57(2): 251 (2008).
[18] Eggen T., Asp T.N., Grave K., Hormazabal V., Uptake and Translocation of Metformin: Ciprofloxacin and Narasin in Forage- and Crop Plants, Chemosphere, 85: 26 (2011).
[19] Eggen T., Lillo C., Antidiabetic II drug Metformin in Plants: Uptake and Translocation to Edible Parts of Cereals Oily Seeds, Beans, Tomato, Squash, Carrots, and Potatoes, J. Agric. Food. Chem,  60:  6929 (2012).
[20] Hai F.I., Yang S., Asif M.B.,  Sencadas V., Shawkat S., Sanderson-Smith M., Gorman J., Xu Z.Q., Yamamoto K., Carbamazepine as a Possible Anthropogenic Marker in Water: Occurrences, Toxicological Effects, Regulations and Removal by Wastewater Treatment Technologies, Water, 10(2): 107 (2018).
[21] Zainab A., Zainab P., Electrochemical Sensor Based on Nanocomposite of Multi-Walled Carbon Nano-Tubes (MWCNTs)/TiO2/Carbon Ionic Liquid Electrode Analysis of Acetaminophen in Pharmaceutical Formulations, Iran. J. Chem. Chem. Eng. (IJCCE), 40: 1030-1041 (2021).
[22] Zehra A.B., Aghbalaghi Z.A., Electrochemical Determination Venlafaxine at NiO/GR Nanocomposite Modified Carbon Paste Electrode, Iran. J. Chem. Chem. Eng. (IJCCE), 40: 1030-1041 (2021).
 [23] Niemuth N.J., Klaper R.D., Emerging Wastewater Contaminant Metformin Causes Intersex and Reduced Fecundity in Fish, Chemosphere, 135: 38 (2015).
[24] Poursat B.A.J., spanning   R.J.M.V., Braster M., Helmus R., Biodegradation of Metformin and its Transformation Product, Guanylurea, by Natural and Exposed Microbial Communities, Ecotoxicol. Environ. Saf., 182: 109414 (2019). 
[25] Trautwein C., Kümmerer K., Incomplete Aerobic Degradation of the Antidiabetic Drug Metformin and Identification of the Bacterial Dead-End Transformation Product Guanylurea, Chemosphere, 85:765 (2011).
[26] Cahill J.D., Furlong E.T., Burkhardt M.R., Kolpin D., Anderson L.G., Determination of Pharmaceutical Compounds in Surface- and Ground-Water Samples by Solid-Phase Extraction and High-Performance Liquid Chromatography-Electrospray Ionization Mass Spectrometry, J. Chromatogr. A, 1041: 171 (2004). 
[27] Bones J., Thomas K., Nesterenko P.N., Paull B., On-Line Preconcentration of Pharmaceutical Residues from Large Volume Water Samples using Short Reversed-Phase Monolithic Cartridges Coupled to LC-UV-ESI-MS, Talanta, 70: 1117 (2006).
[28] Chelliapan S., Wilby T., Sallis P.J., Performance of an Up-Flow Anaerobic Stage Reactor (UASR) in the Treatment of Pharmaceutical Wastewater Containing Macrolide Antibiotics, Water Res., 40: 507(2006).  
[29] Writer J.H., Ferrer I., Barber L.B., Thurman E.M., Widespread Occurrence of Neuroactive Pharmaceuticals and Metabolites in 24 Minnesota Rivers and Wastewaters, Sci. Total Environ., 461–462: 519 (2013).
[30] Castiglioni S., Bagnati R., Fanelli R., Pomati F., Calamari D., Zuccato E., Removal of Pharmaceuticals in Sewage Treatment Plants in Italy, Environ. Sci. Technol., 40: 357 (2006).
[31] Dodd M.C., Kohler H.E., Gunten U.V., Oxidation of Antibacterial Compounds by Ozone and Hydroxyl Radical: Elimination of Biological Activity During Aqueous Ozonation Processes Oxidation of Antibacterial Compounds by Ozone and Hydroxyl Radical: Elimination of Biological Activity during Aqueo, Environ. Sci. Technol., 43: 2498 (2009).
[32] Pelaez M., Nolan N.T., Pillai S.C., Seery M.K., Falaras P., Kontos A.G.,  Dunlop P.S.M., Hamilton J.W.J., Byrne J.A., O’Shea K., Entezari M.H., Dionysiou D.D., A Review on the Visible Light Active Titanium Dioxide Photocatalysts for Environmental Applications, Appl. Catal. B Environ., 125: 331 (2012).
[33] Tabish T.A., Pranjol M.Z.I., Jabeen F., Abdullah T., Latif A., Khalid A., Ali M., Hayat H., Winyard P.G., Whatmore J.L., Zhang S., Investigation into the Toxic Effects of Graphene Nanopores on Lung Cancer Cells and Biological Tissues, Appl. Mater. Today, 12: 389 (2018).
[34] Sattarahmady N., Heli H., Faramarza F., Nickel Oxide Nanotubes-Carbon Microparticles/Nafion Nanocomposite for the Electrooxidation and Sensitive Detection of Metformin, Talanta, 82: 1126 (2010).
[35] Jeong J., Lee J., Electrochemical Oxidation of Industrial Wastewater with the Tube Type Electrolysis   Module System, Sep. Purif. Technol, 84: 35 (2012).
[36] Keshipour S., Faraji M., Aboozari Asl P, Sonochemical Fabrication of Pd/TiO2-Nanotubes/Ti Plate as a Green Catalyst for Oxidation of Alkylarenes and Benzyl Alcohols, J. Iran. Chem. Soc., 16: 1423-1429 (2019).
[37] Keshipour S., Alizadeh S.M., Nickel Phthalocyanine@ Grapheme Oxide/TiO2 as an Efficient Degradation Catalyst of Formic Acid Toward Hydrogen Production, Sci. rep., 11: 16148 (2021).
[38] Keshipour S., Alizadeh S.M., Razeghi M.H., Copper Phthalocyanine@Graphene Oxide as a Cocatalyst of TiO2 in Hydrogen Generation, J. Phys. Chem. Solids., 161: 110434 (2022).
[39] Ghatak H. R., Comparative Removal of Commercial Diclofenac Sodium by Electro-Oxidation on Platinum Anode and Combined Electro Oxidation and Electro-Coagulation on Stainless Steel Anode, Environ. Technol., 35(19): 2483 (2014).
[40] Ghatak H.R., Simulated Process Integration of Wastewater Electrooxidation with Recuperated   Micro Gas Turbine for Energy Recovery, Int. J. Hydrog. Energy, 45(56): 31466 (2020).
[41] Silva S.W.D., Navarro E.M.O., Rodrigues M.A.S., Bernardes M.A., Herranz V.P.,  Using p-Si/BDD Anode for the Electrochemical Oxidation of Norfloxacin, J.  Electroanal. Chem., 832: 112 (2019).
[42] Davis J., Baygents J.C., Farrell J., Understanding Persulfate Production at Boron Doped     Diamond Film Anodes, Electrochimica Acta, 150: 68 (2014)
[43] Samet Y., Agengui L., Abdelhédi R., Electrochemical Degradation of Chlorpyrifos Pesticide in Aqueous Solutions by Anodic Oxidation at Boron-Doped Diamond Electrodes, Chem. Eng. J., 161: 167 (2010).
[44] Cai J., Zhou M., Pan Y., Lu X., Degradation of 2,4-Dichlorophenoxyacetic Acid by Anodic Oxidation and Electro-Fenton using BDD Anode:Influencing Factors and Mechanism, Sep. Purif. Technol., 230: 115867 (2020).
[45] You S.,  Liu B., Gao L., Wang Y., Tang C.Y., Huang Y., Ren N.,  Monolithic Porous Magnéli-Phase Ti4O7 for Electro-Oxidation Treatment of Industrial Wastewater, Electrochim. Acta, 214: 326 (2016). 
[46] Martinez-Huitle C.A., Rodrigo M.A., Sires I., Scialdone I., Single and Coupled Electrochemical Processes and Reactors for the Abatement of Organic Water Pollutants: A Critical Review, Chem. Rev., 115: 13362 (2015).
[47] Hamza M., Abdelhedi R., Brillas E,, Sirés I.,  Comparative Electrochemical Degradation of the Triphenylmethane Dye Methyl Violet with Boron-Doped Diamond and Pt Anodes, J. Electroanal. Chem, 627: 41 (2009).
[48] Guinea E., Garrido J.A., Rodríguez R.M., Cabot P.L., Arias C., Centellas F., Brillas E., Degradation of the Fluoroquinolone Enrofloxacin by Electrochemical Advanced Oxidation Processes based on Hydrogen Peroxide Electrogeneration,  Electrochim.Acta, 55: 2101 (2010).
Iranian Journal of Chemistry and Chemical Engineering
Volume 41, Issue 12 - Serial Number 122
December 2022
Pages 4048-4063

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