Ibuprofen Removal by Electrochemically Activated Peroxymonosulfate Using Iron Electrolysis: Reaction Kinetics, Optimization Using Response Surface Methodology, and Performance in Continuous Flow Mode
Publication: Journal of Environmental Engineering
Volume 148, Issue 10
Abstract
In the present study, ibuprofen (nonsteroidal anti-inflammatory drug) removal was investigated by means of electrochemically activated peroxymonosulfate (EC/PMS) using iron as the sacrificial anode in the reverse-osmosis concentrate (ROC). Complete ibuprofen (IBU) removal was achieved in 30 min at near neutral pH with and current density using the EC/PMS process. EC/PMS performed extremely well in comparison with PMS alone, electrocoagulation (EC) alone, or where was added at the beginning. However, when was added stepwise, PMS activation was more efficient, and the IBU removal rate was close to that of EC/PMS. A response-surface methodology was carried out to understand the effects of pH, , and CD on %IBU removal over 30 min and removal rate constants. It was observed that acidic initial pH, lesser , and highest CD were favorable for higher removal rate constants. Nevertheless, a higher removal rate constant did not necessarily lead to complete removal. to CD ratios significantly affected both %IBU removal and the removal rate constant in the batch EC/PMS process. The EC/PMS process functioned quite well in continuous flow mode. The increase in flow rate from 2 to provided higher %IBU removal from 96.5% to 99.5%, and the residual was reduced from 10 to , respectively. Conclusively, EC/PMS was found to be a promising green treatment method for complex organic compound removal.
Get full access to this article
View all available purchase options and get full access to this article.
Data Availability Statement
The authors confirm that the data supporting the findings of this study are available within the article and its Supplemental Materials.
Acknowledgments
The authors are thankful to DST-PURSE for the Junior Research Fellowship to Katha. The authors also acknowledge the financial support from DST-FIST, the Government of India [No. 329 SR/FST/ETI-395/2015(C)], and the Linde Engineering India Trust for the development of the research facilities at the Environmental Engineering Laboratory of the Civil Engineering Department, FTE MSU.
References
Abd Al-Khodor, Y. A., and T. M. Albayati. 2020. “Employing sodium hydroxide in desulfurization of the actual heavy crude oil: Theoretical optimization and experimental evaluation.” Process Saf. Environ. Prot. 136 (Apr): 334–342. https://doi.org/10.1016/j.psep.2020.01.036.
Adityosulindro, S., C. Julcour, and L. Barthe. 2018. “Heterogeneous Fenton oxidation using Fe-ZSM5 catalyst for removal of ibuprofen in wastewater.” J. Environ. Chem. Eng. 6 (5): 5920–5928. https://doi.org/10.1016/j.jece.2018.09.007.
Bampos, G., A. Petala, and Z. Frontistis. 2021. “Recent trends in pharmaceuticals removal from water using electrochemical oxidation processes.” Environ. MDPI 8 (8): 1–19. https://doi.org/10.3390/environments8080085.
Brillas, E. 2022. “Chemosphere A critical review on ibuprofen removal from synthetic waters, natural waters, and real wastewaters by advanced oxidation processes.” Chemosphere 286 (Part 3): 131849. https://doi.org/10.1016/j.chemosphere.2021.131849.
Bu, L., S. Zhou, Z. Shi, C. Bi, S. Zhu, and N. Gao. 2017. “Iron electrode as efficient persulfate activator for oxcarbazepine degradation: Performance, mechanism, and kinetic modeling.” Sep. Purif. Technol. 178 (May): 66–74. https://doi.org/10.1016/j.seppur.2017.01.007.
Chang, C. F., T. Y. Chen, C. J. M. Chin, and Y. T. Kuo. 2017. “Enhanced electrochemical degradation of ibuprofen in aqueous solution by PtRu alloy catalyst.” Chemosphere 175 (May): 76–84. https://doi.org/10.1016/j.chemosphere.2017.02.021.
Cheng, S., X. Zhang, W. Song, Y. Pan, D. Lambropoulou, Y. Zhong, Y. Du, J. Nie, and X. Yang. 2019. “Photochemical oxidation of PPCPs using a combination of solar irradiation and free available chlorine.” Sci. Total Environ. 682 (Sep): 629–638. https://doi.org/10.1016/j.scitotenv.2019.05.184.
Choina, J., H. Kosslick, C. Fischer, G. U. Flechsig, L. Frunza, and A. Schulz. 2013. “Photocatalytic decomposition of pharmaceutical ibuprofen pollutions in water over titania catalyst.” Appl. Catal., B 129 (Jan): 589–598. https://doi.org/10.1016/j.apcatb.2012.09.053.
Ding, J., Q. Gao, B. Cui, Q. Zhao, G. Zhao, S. Qiu, L. Bu, and S. Zhou. 2021. “Solar-assisted electrooxidation process for enhanced degradation of bisphenol A: Performance and mechanism.” Sep. Purif. Technol. 277 (May): 119467. https://doi.org/10.1016/j.seppur.2021.119467.
Dolatabadi, M., M. T. Ghaneian, C. Wang, and S. Ahmadzadeh. 2021. “Electro-Fenton approach for highly efficient degradation of the herbicide 2,4-dichlorophenoxyacetic acid from agricultural wastewater: Process optimization, kinetic and mechanism.” J. Mol. Liq. 334 (Jul): 116116. https://doi.org/10.1016/j.molliq.2021.116116.
Du, X., W. Yang, J. Zhao, W. Zhang, X. Cheng, J. Liu, Z. Wang, G. Li, and H. Liang. 2019a. “Peroxymonosulfate-assisted electrolytic oxidation/ coagulation combined with ceramic ultrafiltration for surface water treatment: Membrane fouling and sulfamethazine degradation.” J. Cleaner Prod. 235 (Oct): 779–788. https://doi.org/10.1016/j.jclepro.2019.07.035.
Du, X., K. Zhang, B. Xie, J. Zhao, X. Cheng, L. Kai, J. Nie, Z. Wang, G. Li, and H. Liang. 2019b. “Peroxymonosulfate-assisted electro-oxidation/coagulation coupled with ceramic membrane for manganese and phosphorus removal in surface water.” Chem. Eng. J. 365 (Jun): 334–343. https://doi.org/10.1016/j.cej.2019.02.028.
Dubey, M., S. Mohapatra, V. K. Tyagi, S. Suthar, and A. A. Kazmi. 2021. “Occurrence, fate, and persistence of emerging micropollutants in sewage sludge treatment.” Environ. Pollut. 273 (Mar): 116515. https://doi.org/10.1016/j.envpol.2021.116515.
Gao, Y.-Q., J.-Q. Zhou, H. Ning, Y.-Y. Rao, and N.-Y. Gao. 2021. “Electrochemically activated peroxymonosulfate for the abatement of chloramphenicol in water: Performance and mechanism.” Environ. Sci. Pollut. Res. 29 (12): 0123456789. https://doi.org/10.1007/s11356-021-17089-y.
Govindan, K., M. Raja, S. U. Maheshwari, and M. Noel. 2015. “Analysis and understanding of amido black 10B dye degradation in aqueous solution by electrocoagulation with the conventional oxidants peroxomonosulfate, peroxodisulfate and hydrogen peroxide.” Environ. Sci. Water Res. Technol. 1 (1): 108–119. https://doi.org/10.1039/c4ew00030g.
Govindan, K., M. Raja, M. Noel, and E. J. James. 2014. “Degradation of pentachlorophenol by hydroxyl radicals and sulfate radicals using electrochemical activation of peroxomonosulfate, peroxodisulfate and hydrogen peroxide.” J. Hazard. Mater. 272 (May): 42–51. https://doi.org/10.1016/j.jhazmat.2014.02.036.
Hama Aziz, K. H., H. Miessner, S. Mueller, D. Kalass, D. Moeller, I. Khorshid, and M. A. M. Rashid. 2017. “Degradation of pharmaceutical diclofenac and ibuprofen in aqueous solution, a direct comparison of ozonation, photocatalysis, and non-thermal plasma.” Chem. Eng. J. 313 (Apr): 1033–1041. https://doi.org/10.1016/j.cej.2016.10.137.
Hu, A., X. Zhang, D. Luong, K. D. Oakes, M. R. Servos, R. Liang, S. Kurdi, P. Peng, and Y. Zhou. 2012. “Adsorption and photocatalytic degradation kinetics of pharmaceuticals by TiO2 nanowires during water treatment.” Waste Biomass Valorization 3 (4): 443–449. https://doi.org/10.1007/s12649-012-9142-6.
Ji, Y., L. Wang, M. Jiang, Y. Yang, P. Yang, J. Lu, C. Ferronato, and J. M. Chovelon. 2017. “Ferrous-activated peroxymonosulfate oxidation of antimicrobial agent sulfaquinoxaline and structurally related compounds in aqueous solution: Kinetics, products, and transformation pathways.” Environ. Sci. Pollut. Res. 24 (24): 19535–19545. https://doi.org/10.1007/s11356-017-9569-1.
Jothinathan, L., and J. Hu. 2018. “Kinetic evaluation of graphene oxide based heterogenous catalytic ozonation for the removal of ibuprofen.” Water Res. 134 (May): 63–73. https://doi.org/10.1016/j.watres.2018.01.033.
Kadhum, S. T., G. Y. Alkindi, and T. M. Albayati. 2021. “Eco friendly adsorbents for removal of phenol from aqueous solution employing nanoparticle zero-valent iron synthesized from modified green tea bio-waste and supported on silty clay.” Chin. J. Chem. Eng. 36 (Aug): 19–28. https://doi.org/10.1016/j.cjche.2020.07.031.
Kadhum, S. T., G. Y. Alkindi, and T. M. Albayati. 2022. “Remediation of phenolic wastewater implementing nano zerovalent iron as a granular third electrode in an electrochemical reactor.” Int. J. Environ. Sci. Technol. 19 (3): 1383–1392. https://doi.org/10.1007/s13762-021-03205-5.
Kalash, K. R., and T. M. Albayati. 2021. “Remediation of oil refinery wastewater implementing functionalized mesoporous materials mcm-41 in batch and continuous adsorption process.” Desalin. Water Treat. 220 (Apr): 130–141. https://doi.org/10.5004/dwt.2021.27004.
Khan, J. A., X. He, H. M. Khan, N. S. Shah, and D. D. Dionysiou. 2013. “Oxidative degradation of atrazine in aqueous solution by , and processes: A comparative study.” Chem. Eng. J. 218 (Feb): 376–383. https://doi.org/10.1016/j.cej.2012.12.055.
Khedr, T. M., S. M. El-Sheikh, A. Hakki, A. A. Ismail, W. A. Badawy, and D. W. Bahnemann. 2017. “Highly active non-metals doped mixed-phase TiO2 for photocatalytic oxidation of ibuprofen under visible light.” J. Photochem. Photobiol., A 346 (Sep): 530–540. https://doi.org/10.1016/j.jphotochem.2017.07.004.
Kobya, M., E. Gengec, and E. Demirbas. 2016. “Operating parameters and costs assessments of a real dyehouse wastewater effluent treated by a continuous electrocoagulation process.” Chem. Eng. Process. Process Intensification 101 (Mar): 87–100. https://doi.org/10.1016/j.cep.2015.11.012.
Kumar, A., B. Prasad, and K. K. Garg. 2021. “Enhanced catalytic activity of series LaCuxFe1-xO3 (, 0.4, 0.6, 0.8) perovskite-like catalyst for the treatment of highly toxic ABS resin wastewater: Phytotoxicity study, parameter optimization and reaction pathways.” Process Saf. Environ. Prot. 147 (Mar): 162–180. https://doi.org/10.1016/j.psep.2020.09.020.
Lin, L., W. Jiang, M. Bechelany, M. Nasr, J. Jarvis, T. Schaub, R. R. Sapkota, P. Miele, H. Wang, and P. Xu. 2019. “Adsorption and photocatalytic oxidation of ibuprofen using nanocomposites of TiO2 nanofibers combined with BN nanosheets: Degradation products and mechanisms.” Chemosphere 220 (Apr): 921–929. https://doi.org/10.1016/j.chemosphere.2018.12.184.
Ling, L., D. Zhang, C. Fan, and C. Shang. 2017. “A Fe(II)/citrate/UV/PMS process for carbamazepine degradation at a very low Fe(II)/PMS ratio and neutral pH: The mechanisms.” Water Res. 124 (Nov): 446–453. https://doi.org/10.1016/j.watres.2017.07.066.
Ma, M., L. Chen, J. Zhao, W. Liu, and H. Ji. 2019. “Efficient activation of peroxymonosulfate by hollow cobalt hydroxide for degradation of ibuprofen and theoretical study.” Chin. Chem. Lett. 30 (12): 2191–2195. https://doi.org/10.1016/j.cclet.2019.09.031.
Maryam, B., V. Buscio, S. U. Odabasi, and H. Buyukgungor. 2020. “A study on behavior, interaction and rejection of Paracetamol, Diclofenac and Ibuprofen (PhACs) from wastewater by nanofiltration membranes.” Environ. Technol. Innovation 18 (May): 100641. https://doi.org/10.1016/j.eti.2020.100641.
Méndez-Arriaga, F., S. Esplugas, and J. Giménez. 2010. “Degradation of the emerging contaminant ibuprofen in water by photo-Fenton.” Water Res. 44 (2): 589–595. https://doi.org/10.1016/j.watres.2009.07.009.
Minella, M., S. Bertinetti, K. Hanna, C. Minero, and D. Vione. 2019. “Degradation of ibuprofen and phenol with a Fenton-like process triggered by zero-valent iron (ZVI-Fenton).” Environ. Res. 179 (May): 108750. https://doi.org/10.1016/j.envres.2019.108750.
Peng, F., R. Yin, Y. Liao, X. Xie, J. Sun, D. Xia, and C. He. 2019. “Kinetics and mechanisms of enhanced degradation of ibuprofen by piezo-catalytic activation of persulfate.” Chem. Eng. J. 392 (Jul): 123818. https://doi.org/10.1016/j.cej.2019.123818.
Quero-Pastor, M. J., M. C. Garrido-Perez, A. Acevedo, and J. M. Quiroga. 2014. “Ozonation of ibuprofen: A degradation and toxicity study.” Sci. Total Environ. 466–467 (Jan): 957–964. https://doi.org/10.1016/j.scitotenv.2013.07.067.
Radjenovic, J., A. Bagastyo, R. A. Rozendal, Y. Mu, J. Keller, and K. Rabaey. 2011. “Electrochemical oxidation of trace organic contaminants in reverse osmosis concentrate using RuO2/IrO2-coated titanium anodes.” Water Res. 45 (4): 1579–1586. https://doi.org/10.1016/j.watres.2010.11.035.
Rodriguez-Narvaez, O. M., M. O. A. Pacheco-Alvarez, K. Wróbel, J. Páramo-Vargas, E. R. Bandala, E. Brillas, and J. M. Peralta-Hernandez. 2020. “Development of a Co2+/PMS process involving target contaminant degradation and PMS decomposition.” Int. J. Environ. Sci. Technol. 17 (1): 17–26. https://doi.org/10.1007/s13762-019-02427-y.
Ruggeri, G., G. Ghigo, V. Maurino, C. Minero, and D. Vione. 2013. “Photochemical transformation of ibuprofen into harmful 4-isobutylacetophenone: Pathways, kinetics, and significance for surface waters.” Water Res. 47 (16): 6109–6121. https://doi.org/10.1016/j.watres.2013.07.031.
Salgado, R., D. Brito, J. P. Noronha, B. Almeida, M. R. Bronze, A. Oehmen, G. Carvalho, and M. T. Barreto Crespo. 2020. “Metabolite identification of ibuprofen biodegradation by Patulibacter medicamentivorans under aerobic conditions.” Environ. Technol. 41 (4): 450–465. https://doi.org/10.1080/09593330.2018.1502362.
Scheers, T., L. Appels, B. Dirkx, L. Jacoby, L. van Vaeck, B. van der Bruggen, J. Luyten, J. Degrèv, J. van Impe, and R. Dewil. 2012. “Evaluation of peroxide based advanced oxidation processes (AOPs) for the degradation of ibuprofen in water.” Desalin. Water Treat. 50 (1–3): 189–197. https://doi.org/10.1080/19443994.2012.708568.
Skoumal, M., R. M. Rodríguez, P. L. Cabot, F. Centellas, J. A. Garrido, C. Arias, and E. Brillas. 2009. “Electro-Fenton, UVA photoelectro-Fenton and solar photoelectro-Fenton degradation of the drug ibuprofen in acid aqueous medium using platinum and boron-doped diamond anodes.” Electrochim. Acta 54 (7): 2077–2085. https://doi.org/10.1016/j.electacta.2008.07.014.
Song, H., L. Yan, Y. Wang, J. Jiang, J. Ma, C. Li, G. Wang, J. Gu, and P. Liu. 2020. “Electrochemically activated PMS and PDS: Radical oxidation versus nonradical oxidation.” Chem. Eng. J. 391 (Jul): 123560. https://doi.org/10.1016/j.cej.2019.123560.
Sravanth, T., S. T. Ramesh, R. Gandhimathi, and P. V. Nidheesh. 2020. “Continuous treatability of oily wastewater from locomotive wash facilities by electrocoagulation.” Sep. Sci. Technol. 55 (3): 583–589. https://doi.org/10.1080/01496395.2019.1567548.
Sun, Z., S. Li, H. Ding, Y. Zhu, X. Wang, H. Liu, Q. Zhang, and C. Zhao. 2020. “Electrochemical/Fe3+/peroxymonosulfate system for the degradation of Acid Orange 7 adsorbed on activated carbon fiber cathode.” Chemosphere 241 (Feb): 125125. https://doi.org/10.1016/j.chemosphere.2019.125125.
Tamura, H., K. Goto, T. Yotsuyanagi, and M. Nagayama. 1974. “Spectrophotometric determination of iron(II) with 1,10-phenanthroline in the presence of large amounts of iron(III).” Talanta 21 (4): 314–318. https://doi.org/10.1016/0039-9140(74)80012-3.
Wang, C., R. Huang, R. Sun, J. Yang, and M. Sillanpää. 2021a. “A review on persulfates activation by functional biochar for organic contaminants removal: Synthesis, characterizations, radical determination, and mechanism.” J. Environ. Chem. Eng. 9 (5): 106267. https://doi.org/10.1016/j.jece.2021.106267.
Wang, C., R. Sun, and R. Huang. 2021b. “Highly dispersed iron-doped biochar derived from sawdust for Fenton-like degradation of toxic dyes.” J. Cleaner Prod. 297 (May): 126681. https://doi.org/10.1016/j.jclepro.2021.126681.
Wang, C., R. Sun, R. Huang, and H. Wang. 2021c. “Superior Fenton-like degradation of tetracycline by iron loaded graphitic carbon derived from microplastics: Synthesis, catalytic performance, and mechanism.” Sep. Purif. Technol. 270 (Sep): 118773. https://doi.org/10.1016/j.seppur.2021.118773.
Wang, Y. R., and W. Chu. 2011. “Degradation of a xanthene dye by Fe(II)-mediated activation of Oxone process.” J. Hazard. Mater. 186 (2–3): 1455–1461. https://doi.org/10.1016/j.jhazmat.2010.12.033.
Wei, X., X. Xie, Y. Wang, and S. Yang. 2020. “Shape-dependent Fenton-like catalytic activity of Fe3O4 nanoparticles.” J. Environ. Eng. 146 (3): 04020005. https://doi.org/10.1061/(ASCE)EE.1943-7870.0001648.
Yang, N., J. Cui, L. Zhang, W. Xiao, N. Alshawabkeh, and X. Mao. 2015. “Iron electrolysis-assisted peroxymonosulfate chemical oxidation for the remediation of chlorophenol-contaminated groundwater.” J. Chem. Technol. Biotechnol. 91 (4): 938–947. https://doi.org/10.1002/jctb.4659.
Yang, Z., R. Su, S. Luo, R. Spinney, M. Cai, R. Xiao, and Z. Wei. 2017. “Comparison of the reactivity of ibuprofen with sulfate and hydroxyl radicals: An experimental and theoretical study.” Sci. Total Environ. 590–591 (Jul): 751–760. https://doi.org/10.1016/j.scitotenv.2017.03.039.
Yuan, Z., M. Sui, B. Yuan, P. Li, J. Wang, J. Qin, and G. Xu. 2017. “Degradation of ibuprofen using ozone combined with peroxymonosulfate.” Environ. Sci. Water Res. Technol. 3 (5): 960–969. https://doi.org/10.1039/c7ew00174f.
Zhang, K., X. Min, T. Zhang, M. Si, W. Chen, Q. Wang, Y. Shi, and L. Chai. 2021a. “Efficient peroxymonosulfate activation in electron-rich/poor reaction sites induced by copper: Iron oxide heterojunctions/interfaces: Performance and mechanism.” Chem. Eng. J. 423 (Nov): 129971. https://doi.org/10.1016/j.cej.2021.129971.
Zhang, Y., B. T. Zhang, Y. Teng, J. Zhao, and X. Sun. 2021b. “Heterogeneous activation of persulfate by carbon nanofiber supported Fe3O4@carbon composites for efficient ibuprofen degradation.” J. Hazard. Mater. 401 (Jan): 123428. https://doi.org/10.1016/j.jhazmat.2020.123428.
Ziylan, A., and N. H. Ince. 2015. “Catalytic ozonation of ibuprofen with ultrasound and Fe-based catalysts.” Catal. Today 240 (Part A): 2–8. https://doi.org/10.1016/j.cattod.2014.03.002.
Information & Authors
Information
Published In
Journal of Environmental Engineering
Volume 148 • Issue 10 • October 2022
Copyright
© 2022 American Society of Civil Engineers.
History
Received: Mar 19, 2022
Accepted: Apr 30, 2022
Published online: Jul 19, 2022
Published in print: Oct 1, 2022
Discussion open until: Dec 19, 2022
ASCE Technical Topics:
- Chemical compounds
- Chemical properties
- Chemicals
- Chemistry
- Comparative studies
- Continuum mechanics
- Density currents
- Dynamics (solid mechanics)
- Electrokinetics
- Engineering fundamentals
- Engineering mechanics
- Environmental engineering
- Flow (fluid dynamics)
- Fluid dynamics
- Fluid mechanics
- Hydrologic engineering
- Iron compounds
- Kinetics
- Methodology (by type)
- Models (by type)
- Optimization models
- Overland flow
- pH
- Research methods (by type)
- Solid mechanics
- Waste management
- Water and water resources
Authors
Metrics & Citations
Metrics
Citations
Download citation
If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.