Abstract
This work used a time-integrated performance index to significantly address the low cost of the Electrocoagulation process to strengthen its tetracycline removal performance. The main goal was controlling the time-depending tetracycline removal efficiency of the electrocoagulation process was searched by choosing a better combination of the electrode material and electrolyte species types for getting a stabilization condition of the total electric voltage. The response surface methodology was included to address, compare and rescue the best results of the time-integrated performance index. The electrolyte type, pH of the aqueous media, electric conductivity, and electric voltage were assessed to better respond to the performance of tetracycline removal. In this regard, an iron-based electrocoagulation reactor was operated over 40 to 67 A m−2 of electric current density supported by 5 to 10 mS cm−1 electric conductivity values, testing a 10-to-90 min electrocoagulation time range. A 10-to-60 mol m−3 concentration range of Cr, Zn, Ca, and K cationic species was tested to set 5-to-10 mS cm−1 electric conductivity values and assess their influences on EC performance due to each one separately. In combination with Fe electrodes, Ca2+ electrolytes have driven to a stable electric conductivity in time besides pH buffering at the alkaline region with the best electrocoagulation performance, resulting getting a low and stable total electric voltage (less than 10 V). Using Fe electrodes and Ca2+ electrolytes, a Box-Behnken experimental design was performed regarding ranges of 4-to-8 solution pH, 40-to-94 A m−2 electric current density, and 10-to-30 min time. A time-integrated performance index as the response variable was proposed for addressing a better tetracycline removal. Finally, a 40 A m−2 electric current density allowed the maximal time-integrated performance index value over 30 min, removing above 97% tetracycline with minimal electric power consumption.
Graphical Abstract
Similar content being viewed by others
References
Ebenstein A (2012) The consequences of industrialisation: evidence from water pollution and digestive cancers in China, vol 94. Rev Econ Stat, Cambridge, Mass, pp 186–201
Chen G, Zhao L, Dong Y (2011) Oxidative degradation kinetics and products of chlortetracycline by manganese dioxide. J Hazard Mater 193:128–138. https://doi.org/10.1016/j.hazmat.2011.07.039
Daghrir R, Drogui P (2013) Tetracycline antibiotics in the environment: a review. Environ Chem Lett 11(3):209–227. https://doi.org/10.1007/s10311-013-0404-8
Dai C, Shi S, Chen D, Liu J, Huang L, Zhang J, Feng Y (2022) Study on the mechanism of tetracycline removal in electrocoagulation coupled with electro-Fenton reaction system with Fe anode and carbon nanotube cathode. Chem Eng J 428:131045. https://doi.org/10.1016/j.cej.2021.131045
Módenes AN, Bazarin G, Borba CE, Locatelli PPP, Borsato FP, Pagno V, Pedrini R, Trigueros DEG, Espinoza-Quiñones FR, Scheufele FB (2020) Tetracycline adsorption by tilapia fish bone-based biochar: Mass transfer assessment and fixed-bed data prediction by hybrid statistical-phenomenological modeling. J Clean Prod 279:123775. https://doi.org/10.1016/j.jclepro.2020.123775
Xu J, Zhang Y, Li B, Fan S, Xu Guan D-X (2022) Improved adsorption properties of tetracycline on KOH/KMnO4 modified biochar derived from wheat straw. Chemosphere 296:133981. https://doi.org/10.1016/j.chemosphere.2022.133981
Sun S, Jiang Q, Zhang W, Tian L, Li T, Zheng L, Gao Y, Zeng X, Zhou L (2022) Efficient adsorption of tetracycline in aquatic system by thermally-treated sediment. Environ Res 214(Part 1):113779. https://doi.org/10.1016/j.envres.2022.113779
Ortiz-Ramos U, Leyva-Ramos R, Mendoza-Mendoza E, Aragón-Piña A (2022) Removal of tetracycline from aqueous solutions by adsorption on raw Ca-bentonite. Effect of operating conditions and adsorption mechanism. Chem Eng J. 432:134428. https://doi.org/10.1016/j.cej.2021.134428
Park J-A, Nam A, Kim J-H, Yun S-T, Choi J-W, Lee S-H (2018) Blend-electrospun graphene oxide/Poly(vinylidene fluoride) nanofibrous membranes with high flux, tetracycline removal and anti-fouling properties. Chemosphere 207:347–356. https://doi.org/10.1016/j.chemosphere.2018.05.096
Pagno V, Módenes AN, Dragunski DC, Fiorentin-Ferrari LD, Caetano J, Guellis C, Gonçalves BC, dos Anjos EV, Pagno F, Martinelli V (2020) Heat treatment of polymeric PBAT/PCL membranes containing activated carbon from Brazil nutshell biomass obtained by electrospinning and applied in drug removal. J Environ Chem Eng 8(5):104159. https://doi.org/10.1016/j.jece.2020.104159
Cui J, Xie A, Liu Y, Xue C, Pan J (2021) Fabrication of multi-functional imprinted composite membrane for selective tetracycline and oil-in-water emulsion separation. Compos Commun 28:100985. https://doi.org/10.1016/j.coco.2021.100985
Nasrollahi N, Vatanpour V, Khataee A (2022) Removal of antibiotics from wastewaters by membrane technology: limitations, successes, and future improvements. Sci Total Environ 838(Part 1):156010. https://doi.org/10.1016/j.scitotenv.2022.156010
Garcia-Segura S, Eiband MMSG, de Melo JV, Martínez-Huitle CA (2017) Electrocoagulation and advanced electrocoagulation processes: a general review about the fundamentals, emerging applications and its association with other technologies. J Electroanal Chem 801:267–299. https://doi.org/10.1016/j.jelechem.2017.07.047
Dai Y, Li J, Shan D (2020) Adsorption of tetracycline in aqueous solution by biochar derived from waste Auricularia auricula dregs. Chemosphere 238:124432. https://doi.org/10.1016/j.chemosphere.2019.124432
Kumari S, Kumar RN (2022) How effective aerated continuous electrocoagulation can be for tetracycline removal from river water using aluminium electrodes? Chemosphere 305:135476. https://doi.org/10.1016/j.chemosphere.2022.135476
Liu X, Zhou Y, Zhang J, Luo L, Yang Y, Huang H, Peng H, Tang L, Mu Y (2018) Insight into electro-Fenton and photo-Fenton for the degradation of antibiotics: mechanism study and research gaps. Chem Eng J 347:379–397. https://doi.org/10.1016/j.cej.2018.04.142
Lai C, Huang F, Zeng G, Huang D, Qin L, Cheng M, Zhang C, Li B, Yi H, Liu S, Li L, Chen L (2019) Fabrication of novel magnetic MnFe2O4/bio-char composite and heterogeneous photo-Fenton degradation of tetracycline in near neutral pH. Chemosphere 224:910–921. https://doi.org/10.1016/j.chemosphere.2019.02.193
Cao Z, Jia Y, Wang Q, Cheng H (2021) High-efficiency photo-Fenton Fe/g-C3N4/kaolinite catalyst for tetracycline hydrochloride degradation. Appl Clay Sci 212:106213. https://doi.org/10.1016/j.clay.2021.106213
AlJaberi FY, Ahmed SA, Makki HF, Naje AS, Zwain HM, Salman AD, Juzsakova T, Viktor S, Van B, Le PC, La DD, Chang SW, Um MJ, Ngo HH, Nguyen DD (2023) Recent advances and applicable flexibility potential of electrochemical processes for wastewater treatment. Sci Total Environ 867:161361. https://doi.org/10.1016/j.scitotenv.2022.161361
Tegladza ID, Xu Q, Xu K, Lv G, Lu J (2021) Electrocoagulation processes: a general review about role of electro-generated flocs in pollutant removal. Process Saf Environ Prot 146:169–189. https://doi.org/10.1016/j.psep.2020.08.048
Liu YJ, Hu CY, Lo SL (2019) Direct and indirect electrochemical oxidation of amine-containing pharmaceuticals using graphite electrodes. J Hazard Mater 366:592–605. https://doi.org/10.1016/j.jhazmat.2018.12.037
Cuprys A, Thomson P, Ouarda Y, Suresh G, Rouissi T, Kaur Brar S, Drogui P, Surampalli RY (2020) Ciprofloxacin removal via sequential electrooxidation and enzymatic oxidation. J Hazard Mater 389:121890. https://doi.org/10.1016/j.jhazmat.2019.121890
Al-Raad AA, Hanafiah MM, Naje AS, Ajeel MA (2020) Optimized parameters of the electrocoagulation process using a novel reactor with rotating anode for saline water treatment. Environ Pollut 265(Part B):115049. https://doi.org/10.1016/j.envpol.2020.115049
Naje AS, Ajeel MA, Ali IM, Al-Zubaidi HAM, Alaba PA (2019) Raw landfill leachate treatment using an electrocoagulation process with a novel rotating electrode reactor. Water Sci Technol 80:458–465. https://doi.org/10.2166/wst.2019.289
Nadais H, Li X, Alves N, Couras C, Andersen HR, Angelidaki I, Zhang Y (2018) Bio-electro-Fenton process for the degradation of non-steroidal anti-inflammatory drugs in wastewater. Chem Eng J 338:401–410. https://doi.org/10.1016/j.cej.2018.01.014
Avancini Dias O, Perini Muniz E, da Silva Porto PS (2019) Electrocoagulation using perforated electrodes: an increase in metalworking fluid removal from wastewater. Chem Eng and Process Process Intensif 139:113–120. https://doi.org/10.1016/j.cep.2019.03.021
Devlin TR, Kowalski MS, Pagaduan E, Zhang X, Wei V, Oleszkiewicz JA (2019) Electrocoagulation of wastewater using aluminum, iron, and magnesium electrodes. J Hazard Mater 368:862–868. https://doi.org/10.1016/j.jhazmat.2018.10.017
AlJaberi FY (2018) Analysis of electrodes consumption via the electrocoagulation treatment of Lead removal from simulated wastewater. Muthanna J Eng Technol 6:120–129. https://doi.org/10.52113/3/eng/mjet/2018-06-02/120-129
Meiramkulova K, Jakupova Z, Orynbekov D, Tashenov E, Kydyrbekova A, Mkilima T, Inglezakis VJ (2020) Evaluation of electrochemical methods for poultry slaughterhouse wastewater treatment. Sustainability 12:5110. https://doi.org/10.3390/su12125110
Espinoza-Quiñones FR, de Souza ARC, Módenes AN, Trigueros DEG, de Pauli AR, de Souza PSC, Kroumov AD (2016) Removal performance, antibacterial effects, and toxicity assessment of ciprofloxacin treated by the electrocoagulation process. Water Air Soil Pollut 227:460. https://doi.org/10.1007/s11270-016-3165-8
de Pauli AR, Espinoza-Quiñones FR, Trigueros DEG, Módenes AN, de Souza ARC, Borba FH, Kroumov AD (2018) Integrated two-phase purification procedure for abatement of pollutants from sanitary landfill leachates. Chem Eng J 334:19–29. https://doi.org/10.1016/j.cej.2017.10.028
Espinoza-Quiñones FR, Dall’Oglio IC, de Pauli AR, Romani M, Módenes AN, Trigueros DEG (2020) Insights into brewery wastewater treatment by the electro-Fenton hybrid process: how to get a significant decrease in organic matter and toxicity. Chemosphere 263:128367. https://doi.org/10.1016/j.chemosphere.2020.128367
Romani M, Espinoza-Quiñones FR, Módenes AN, Borba CE (2020) New insights into the improvement of electrocoagulation performance on the basis of a time-integrated performance index: the pivotal role of electrical conductivity. J Environ Chem Eng 8(4):103902. https://doi.org/10.1016/j.jece.2020.103902
Espinoza-Quiñones FR, Romani M, Borba CE, Módenes AN, Utzig CF, Dall’Oglio IC (2020) A mathematical approach based on the Nernst-Planck equation for the total electric voltage demanded by the electrocoagulation process: effects of a time-dependent electrical conductivity. Chem Eng Sc 220:1–15. https://doi.org/10.1016/j.ces.2020.115626
Yoosefian M, Ahmadzadeh S, Aghasi M, Dolatabadi M (2017) Optimization of electrocoagulation process for efficient removal of ciprofloxacin antibiotic using iron electrode; kinetic and isotherm studies of adsorption. J Mol Liq 225:544–553. https://doi.org/10.1016/j.molliq.2016.11.093
Ghanbari F, Zirrahi F, Olfati D, Gohari F, Hassani A (2020) TiO2 nanoparticles removal by electrocoagulation using iron electrodes: Catalytic activity of electrochemical sludge for the degradation of emerging pollutant. J Mol Liq 310:113217. https://doi.org/10.1016/j.molliq.2020.113217
Mohammed SJ, M-Ridha MJ, Abed KM, Elgharbawy AAM (2021) Removal of levofloxacin and ciprofloxacin from aqueous solutions and an economic evaluation using the electrocoagulation process. Int J Environ Anal Chem. https://doi.org/10.1080/03067319.2021.1913733
Keyikoglu R, Can OT, Aygun A, Tek A (2019) Comparison of the effects of various supporting electrolytes on the treatment of a dye solution by electrocoagulation process. Colloid Interface Sc Commun. 33:100210. https://doi.org/10.1016/j.colcom.2019.100210
Montgomery DC (2010) Design and analysis of experiments, 8th edn. Wiley, Hoboken
Acknowledgements
The authors thank the Multiuser Analytical Center—CAM/NBQ of the State University of West Paraná—Campus Toledo for analyses in the TXRF spectrometer, UV spectrophotometer and TOC analyzer.
Funding
This work was supported by the National Council for Scientific and Technological Development (CNPq) under grants # 303729/2021-0 and # 304324/2021-3, besides the authors W.V.R. Valençola and I.C. Dall'Oglio by the National Council for the Improvement of Higher Education (CAPES)—Finance Code 001.
Author information
Authors and Affiliations
Contributions
F.R. Espinoza-Quiñones and A.N. Módenes conceived of the presented idea. F.R. Espinoza-Quiñones and W.V.R. Valençola designed and performed the experiments, derived the models and analysed the data. W.V.R. Valençola, I.C. Dall’Oglio, P.L. Obregón and Maurício Romani verified the analytical methods. F.R. Espinoza-Quiñones and A.N. Módenes developed the theoretical formalism, performed the analytic calculations and performed the numerical simulations. F.R. Espinoza-Quiñones and A.N. Módenes took the lead in writing the manuscript. All authors provided critical feedback and helped shape the research, analysis and manuscript.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Espinoza-Quiñones, F.R., Módenes, A.N., Valençola, W.V.R. et al. A significant reduction in the cost of the iron electrodes-based electrocoagulation process with higher tetracycline removal performances when addressed by a time-integrated performance index. J Appl Electrochem 54, 25–39 (2024). https://doi.org/10.1007/s10800-023-01947-3
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10800-023-01947-3