FENTON OXIDATION OF CARBAMAZEPINE IN WASTEWATER WITH FEWER REAGENTS

Yıl 2018, Cilt: 36 Sayı: 1, 289 - 298, 01.03.2018

Sevde Üstün Odabaşı , Bareera Maryam Hanife Büyükgüngör

Öz

Pharmaceutical in natural waters could be an environmental problem because of their potential toxic risk on living organisms. Conventional wastewater treatment plant processes are not enough to remove pharmaceuticals therefore advanced oxidation process have become an attractive solution. Carbamazepine (CBZ), is an antiepileptic drug, is a most widely used medicine in almost every part of world. In present study, advance oxidation, using H2O2 and FeSO4 (Fenton process) is used to degrade the concentrations of CBZ from water. Fenton process is known to be most effective and common methods for the treatment of such wastewaters. This study investigated the degradation of CBZ by H2O2 and FeSO4 under changing pH and contact time of (3, 3.5, 4), (15, 20, 30 min) respectively. Results showed 75.86 % COD and 45.69 % TOC removal. But real degradation of CBZ were elucidated using liquid chromatography mass spectrometry (LCMS) coupled to tandem mass spectrometry (MS) indicating 53.73 % removal.

Anahtar Kelimeler

Carbamazepine, pharmaceuticals, fenton process, water, wastewater

Kaynakça

• [1] Rogawski M.A., (2006). Molecular Targets Versus Models for New Antiepileptic Drug Discovery, Epilepsy Research 68, 22–28.
• [2] Miao X.S., Metcalfe C.D., (2003) Determination of Carbamazepine and Its Metabolities in Aqueous Samples Using Liquid-Chromatography-Electrospray Tandem Mass Spectrometry, Analytical Chemistry 75, 3731–8.
• [3] Pomati F., Castiglioni S., Zuccato E., Fanelli R., Vigetti D., Rossetti C., Calamari D., (2006) Effects of a Complex Mixture of Therapeutic Drugs at Environmental Levels on Human Embryonic Cells, Environmental Science and Technology 40(7), 2442–2447.
• [4] Radjenovic J, Petrovic M, Barcelo D., (2009) Fate and Distribution of Pharmaceuticals in Wastewater and Sewage Sludge of the Conventional Activated Sludge and Advanced Membrane Bioreactor Treatment, Water Research 43, 831–41.
• [5] Miao X.S., Yang J.J., Metcalfe C.D., (2005) Carbamazepine and Its Metabolites in Wastewater and in Biosolids in a Municipal Wastewater Treatment Plant, Environmental Science and Technology 39(74), 69–75.
• [6] Mohapatra D.P., Brar S.K., Tyagi R.D., Picard P., Surampalli R.Y., (2014). Analysis and Advanced Oxidation Treatment of a Persistent Pharmaceutical Compound in Wastewater and Wastewater Sludge-Carbamazepine, Science of the Total Environment 470-471, 58-75.
• [7] Ding, Y., Huang, W., Ding, Z., Nie, G., Tang, H., (2016) Dramatically Enhanced Fenton Oxidation of Carbamazepine with Easily Recyclable Microscaled CuFeO2 By Hydroxylamine: Kinetic And Mechanism Study, Separation and Purification Technology, 168, 223-231.
• [8] Zhang Y, Geißen S.U., Gal C., (2008) Carbamazepine and Diclofenac: Removal in Wastewater Treatment Plants and Occurrence in Water Bodies, Chemosphere, 73:1151–61.
• [9] Liu W., Wang Y., Ai Z., Zhang L., (2015) Hydrothermal Synthesis of FeS2 as a High Efficiency Fenton Reagent to Degrade Alachlor via Superoxide-Mediated Fe(II)/ Fe(III) Cycle, ACS Applied Materials & Interfaces 7, 28534–28544.
• [10] Anipsitakis, G.P., Dionysiou, D.D., (2004) Transition Metal/UV based Advanced Oxidation Technologies for Water Decontamination, Applied Catalysis B: Environmental. 54 (3), 155-163.
• [11] Naddeo V, Meric S, Kassinos D, Belgiorno V, Guida M., (2009) Fate of Pharmaceuticals in Contaminated Urban Wastewater Effluent Under Ultrasonic Irradiation, Water Research, 43,4019–27.
• [12] Furman, O., Teel, A., Watts, R., (2010). Mechanism of Base Activation of Persulfate, Environmental Science and Technology, 44, 6423-6428.
• [13] Ghauch, A., Baydoun, H., Dermesropian, P., (2011) Degradation of Aqueous Carbamazepine in Ultrasonic/Fe0/H2O2 Systems, The Chemical Engineering Journal 172, 18-27.
• [14] Ghauch, A., Tuqan, A., (2012) Oxidation of Bisoprolol in Heated Persulfate/H2O Systems: Kinetics and Products, The Chemical Engineering Journal 183, 162-171.
• [15] Li W, Nanaboina V, Zhou Q, Korshin G.V., (2012) Effects of Fenton Treatment on the Properties of Effluent Organic Matter and Their Relationship with the Degradation of Pharmaceuticals and Personal Care Products, Water Research 46,403–12.
• [16] García-Gómez C., Drogui, P., Seyhi B., Gortáres-Moroyoqui P., Buelna G., Estrada Alvgarado, M.I., Álvarez L.H., (2016) Combined Membrane Bioreactor and Electrochemical Oxidation Using Ti/PbO2 Anode for the Removal of Carbamazepine, Journal of the Taiwan Institute of Chemical Engineers 64, 211-219.
• [17] Clesceri L.S., Greenberg A.E., Eaton A.D., (1999) Standard Methods for Examination of Water and Wastewater 20th Edition, American Public Health Association, American Water Works Association, Water Environment, USA, Baltimore, Maryland.
• [18] Zhou S., Xia Y., Li T., Yao T., Shi Z., Zhu S., (2016) Degradation of Carbamazepine by UV/Chlorine Advanced Oxidation Process and Formation of Disinfection By-Products, Environmental Science and Pollution Research 23, 16448-16455.
• [19] Sonmez G., (2015) Removal of Some Pharmaceutical Residues by Advanced Chemical Oxidation Process, PhD Thesis, Science Enstitue, Aksaray University, Aksaray,
• [20] Dominguez J.R., Gonzáles T., Palo P., Cuerda-Correa E. M., (2012) Fenton + Fenton-like Integrated Process for Carbamazepine Degradation: Optimizing the System, Industrial & Engineering Chemistry Research, 51,2531-2538.
• [21] Dwivedi K., Morone A., Chakrabarti T., Pandey R.A., (2016) Evaluation and Optimization of Fenton Pretreatment Integrated with Granulated Activated Carbon (GAC) Filtration for Carbamazepine Removal from Complex Wastewater of Pharmaceutical Industry, Journal of Environmental Chemical Engineering, http://dx.doi.org/10.2016/j.jece.2016.12.054.
• [22] Expósito A.J., Monteagudo J.M., Durán A., San Martin I., Gonzáles L., (2018) Study of Intensification of Solar Photo-Fenton Degradation of Carbamazepine with Ferrioxalate Complexes and Ultrasound, Journal of Hazardous Materials, 342,597-605.
• [23] Mohapatra D.P., Brar S.K., Tyagi R.D., Picard P., Surampalli R.Y., (2013) A Comparative Study of Ultrasonication, Fenton’s Oxidation and Ferro-sonication Treatment for Degradation of Carbamazepine from Wastewater and Toxicity Test by Yeast Estrogen Screen (YES) Assay, Science the Total Environment, 447, 280-285.
• [24] Arzate S., Carcía-Sanchez J.L., Soriano-Molina P., Casas-López J.L., Campas-Mánas M.C., Agüera A., Sánchez Pérez J.A., (2017) Effect of Residence Time on Micropollutant Removal in WWTP Secondary Effluents by Continuous Solar Photo-Fenton Process in Raceway Pond Reactors, Chemical Engineering Journal, 316, 1114-1121.
• [25] Dai C., Zhou X., Zhang Y., Duan Y., Qiang Z., Zhang T.C., (2012) Comparative Study of the Degradation of Carbamazepine in Water by Advanced Oxidation Process, Environmental Technology, 33, 1101-1109.
• [26] De La Cruz N., Gimenez J., Espluga S., Grandjean D., de Alencastro L.F., Pulgarin C., (2012) Degradation of 32 Emergent Contaminants by UV and Neutral Photo-Fenton in Domestic Wastewater Effluent Previously Treated by Activated Sludge, Water Research, 46(6), 1947-1957.
• [27] Ding Y., Huang W., Ding Z., Nie G., Tang H., (2016) Dramatically Enhanced Fenton Oxidation of Carbamazepine with Easily Recyclable Microscaled CuFeO2 by Hydroxylamine: Kinetic and Mechanism Study, Separation and Purification Technology, 168, 223-231.
• [28] Monsalvo V.M., Lopez J., Munoz M., de Pedro Z.M., Casas J.A., Mohedano A.F., Rodriguez J.J., (2015) Application of Fenton-like Oxidation as Pre-treatment for Carbamazepine Biodegradation, Chemical Engineering Journal, 264, 856–862.
• [29] Lee H.J., Lee H., Lee C., (2014) Degradation of Diclofenac and Carbamazepine by the Copper(II)-Catalyzed Dark and Photo-assisted Fenton-like Systems, Chemical Engineering Journal, 245, 258–264.
• [30] Ahmed M. M., Chiron S., (2014) Solar Photo-Fenton Like Using Persulphate for Carbamazepine Removal from Domestic Wastewater, Water Research, 48, 229-236.
• [31] Calza P., Medana C., Padovano E., Giancotti V., Baiocchi C., (2012) Identification of the Unknown Transformation Products Derived from Clarithromycin and Carbamazepine Using Liquid Chromatography/High-Resolution Mass Spectrometry, Rapid Communications in Mass Spectrometry 26, 1687-1704.
• [32] Hübner U., Seiwert B., Reemtsma T., Jekel M., (2014) Ozonation Products of Carbamazepine and Their Removal from Secondary Effluents by Soil Aquifer Treatment: Indications from Column Experiments, Water Res. 49, 34-43.
• [33] Yang B., Kookana R.S., Williams M., Du J., Hai D., Kumar A., (2016) Removal of Carbamazepine in Aqueous Solutions through Solar Photolysis of Free Available Chlorine, Water Research 100, 413-420.
• [34] Tekin H., Bilkay O., Ataberk S.S., Balta T.H., Ceribasi I.H., Sanin F.D., Dilek F.B., Yetis U., (2006) Use of Fenton Oxidation to Improve the Biodegradability of a Pharmaceutical Wastewater, Journal of Hazardous Materials B 136, 258–265.
• [35] Mohapatra D.P., Brar S.K., Tyagi R.D., Picard P., Surampalli R.Y., (2012) Carbamazepine in Municipal Wastewater and Wastewater Sludge: Ultrafast Quantification by Laser Diode Thermal Desorption-Atmospheric Pressure Chemical Ionization Coupled with Tandem Mass Spectrometry, Talanta, 99:247–55.
• [36] Kang Y.W., and Hwang K., (2000) Effect of Reaction Conditions on the Oxidation Efficiency in the Fenton Process, Water Research 10, 2786-2790.