Phenol Reduction of Petroleum Refinery Wastewater Using Electro-Coagulation/Electro-Oxidation Technique

Document Type : Research Paper

Authors

Chem. Eng. Dept., University of Babylon, Babil, Iraq.

Abstract

Water pollution from industrial waste, toxic biological waste, and crude oil refining wastewater: All of these pollutants are released into the environment and pose a major problem today due to their toxic organic and inorganic contaminants. The study found that two electrical methods, electro-coagulation (EC) followed by electro-oxidation (EO) and electro-oxidation alone, effectively reduced organic phenol (C₆H₅OH) levels in oil-refining wastewater from Najaf refineries in Iraq. Both methods achieved remarkable success, though with differences in the factors affecting dissolved phenol removal. The work was done using aluminum and graphite electrodes as the cover of the electric cell and steel (SS) electrodes as the cathode of the cell, made of resistant plastic, in the first method, and graphite electrodes as the anode of the cell with steel (SS) electrodes in the other method. The initial concentration of phenol in the treated water was 50 ppm under the following conditions for both methods: electric current density of 10, 15, and 20 mA/cm², sodium chloride (NaCl) with concentration of 0, 1.5, and 3 g/l, and acidity of 3, 7, and 10 pH, with a fixed time of 1 hour for the EC process and 2.5 hours for the EO process for the first method, while in the other method, the time was varied from 2-4 hours. The results showed that the removal rate was directly proportional to the high current density and NaCl concentration under mild acidic conditions for the first method, with the optimum conditions for the removal process being a current density of 20 mA/cm2, pH 7, and a NaCl concentration of 3 g/L. A removal rate of 95.05% was achieved for the first method under the aforementioned conditions. The results for the removal rate in the second method were obtained under the following conditions: a current density of 15 mA/cm2, a pH of 3, a NaCl concentration of 3 g/L, and a time period of 3 hours. A removal rate of 96.3% was achieved under the mentioned conditions. Optimization tests were performed using the response surface methodology with Box-Behnken design to identify key operational factors influencing phenol removal from wastewater.

Keywords

Main Subjects


  1. V Nidheesh, J. Scaria, D. S. Babu, and M. S. Kumar, “An overview on combined electrocoagulation-degradation processes for the effective treatment of water and wastewater,” Chemosphere, vol. 263, p. 127907, 2021. https://doi.org/10.1016/j.chemosphere.2020.127907
  2. A. Gasim, S. R. M. Kutty, M. H. Isa, and M. P. M. Isa, “Treatment of petroleum refinery wastewater by using UASB reactors,” International Journal of Chemical and Biological Engineering, vol. 6, no. 1, pp. 174–177, 2012. https://doi.org/10.1016/j.watres.2011.05.049
  3. Wei, S. Guo, G. Yan, C. Chen, and X. Jiang, “Electrochemical pretreatment of heavy oil refinery wastewater using a three-dimensional electrode reactor,” Electrochim Acta, vol. 55, no. 28, pp. 8615–8620, 2010. https://doi.org/10.1016/j.electacta.2010.08.011
  4. Fang, C. He, Y. Li, K. H. Chung, C. Xu, and Q. Shi, “Fractionation and characterization of dissolved organic matter (DOM) in refinery wastewater by revised phase retention and ion-exchange adsorption solid phase extraction followed by ESI FT-ICR MS,” Talanta, vol. 162, pp. 466–473, 2017. https://doi.org/10.1016/j.talanta.2016.10.064
  5. A. Younis, N. S. El-Gendy, W. I. El-Azab, and Y. M. Moustafa, “Kinetic, isotherm, and thermodynamic studies of polycyclic aromatic hydrocarbons biosorption from petroleum refinery wastewater using spent waste biomass. Desalin Water Treat 56: 3013–3023,” 2015. https://doi.org/10.1080/19443994.2014.964331
  6. Santos, J. G. Crespo, M. A. Santos, and S. Velizarov, “Oil refinery hazardous effluents minimization by membrane filtration: An on-site pilot plant study,” J Environ Manage, vol. 181, pp. 762–769, 2016. https://doi.org/10.1016/j.jenvman.2016.07.027Get rights and content
  7. Singh and P. Kumar, “Pre-treatment of petroleum refinery wastewater by coagulation and flocculation using mixed coagulant: Optimization of process parameters using response surface methodology (RSM),” Journal of water process engineering, vol. 36, p. 101317, 2020. https://doi.org/10.1016/j.jwpe.2020.101317
  8. H. Abbar and S. S. Alkurdi, “Performance evaluation of a combined electrocoagulation–electrooxidation process for the treatment of petroleum refinery wastewater,” in IOP Conference Series: Materials Science and Engineering, IOP Publishing, 2021, p. 12027. Doi: https://doi.org/10.1088/1757899X/1076/1/012027
  9. [9] Vasudevan, “An efficient removal of phenol from water by peroxi-electrocoagulation processes,” Journal of Water Process Engineering, vol. 2, pp. 53–57, 2014. https://doi.org/10.1016/j.jwpe.2014.05.002
  10. Ozyonar and B. Karagozoglu, “Treatment of pretreated coke wastewater by electrocoagulation and electrochemical peroxidation processes,” Sep Purif Technol, vol. 150, pp. 268–277, 2015. https://doi.org/10.1016/j.seppur.2015.07.011
  11. Ozyonar, “Treatment of train industry oily wastewater by electrocoagulation with hybrid electrode pairs and different electrode connection modes,” Int J Electrochem Sci, vol. 11, no. 2, pp. 1456–1471, 2016. https://doi.org/10.1016/S1452-3981(23)15933-5
  12. O. E. Abdel‐Salam, E. M. Abou Taleb, and A. A. Afify, “Electrochemical treatment of chemical oxygen demand in produced water using flow‐by porous graphite electrode,” Water and Environment Journal, vol. 32, no. 3, pp. 404–411, 2018. https://doi.org/10.1111/wej.12336
  13. C.-H. Lee, E.-S. Lee, Y.-K. Lim, K.-H. Park, H.-D. Park, and D.-S. Lim, “Enhanced electrochemical oxidation of phenol by boron-doped diamond nanowire electrode,” RSC Adv, vol. 7, no. 11, pp. 6229–6235, 2017. DOI: https://doi.org/10.1039/C6RA26287B
  14. Z. Isik, E. B. Arikan, Y. Ozay, H. D. Bouras, and N. Dizge, “Electrocoagulation and electrooxidation pre-treatment effect on fungal treatment of pistachio processing wastewater,” Chemosphere, vol. 244, p. 125383, 2020. https://doi.org/10.1016/j.chemosphere.2019.125383
  15. H. M. Ibrahim and R. H. Salman, “Real wastewater treatment by electrocoagulation-electro-oxidation combined system: optimization using Taguchi approach,” Egypt J Chem, vol. 65, no. 3, pp. 135–145, 2022. https://dx.doi.org/10.21608/ejchem.2021.88245.4247
  16. R. H. Salman and A. H. Abbar, “Optimization of a combined electrocoagulation-electro-oxidation process for the treatment of Al-Basra Majnoon Oil field wastewater: Adopting a new strategy,” Chemical Engineering and Processing-Process Intensification, vol. 183, p. 109227, 2023. https://doi.org/10.1016/j.cep.2022.109227
  17. M. A. Oturan and J.-J. Aaron, “Advanced oxidation processes in water/wastewater treatment: principles and applications. A review,” Crit Rev Environ Sci Technol, vol. 44, no. 23, pp. 2577–2641, 2014. https://doi.org/10.1080/10643389.2013.829765
  18. P. Bhatt, B. A. Engel, K. B. Shivaram, R. F. Turco, Z. Zhou, and H. Simsek, “Treatment and optimization of high-strength egg-wash wastewater effluent using electrocoagulation and electrooxidation methods,” Chemosphere, vol. 347, p. 140632, 2024. https://doi.org/10.1016/j.chemosphere.2023.140632
  19. F. Sopaj, M. A. Rodrigo, N. Oturan, F. I. Podvorica, J. Pinson, and M. A. Oturan, “Influence of the anode materials on the electrochemical oxidation efficiency. Application to oxidative degradation of the pharmaceutical amoxicillin,” Chemical Engineering Journal, vol. 262, pp. 286–294, 2015. https://doi.org/10.1016/j.cej.2014.09.100
  20. M. A. Alkhadra et al., “Electrochemical methods for water purification, ion separations, and energy conversion,” Chem Rev, vol. 122, no. 16, pp. 13547–13635, 2022. https://doi.org/10.1021/acs.chemrev.1c00396
  21. I. Sirés, E. Brillas, M. A. Oturan, M. A. Rodrigo, and M. Panizza, “Electrochemical advanced oxidation processes: today and tomorrow. A review,” Environmental Science and Pollution Research, vol. 21, pp. 8336–8367, 2014. https://doi.org/10.1007/s11356-014-2783-1
  22. M. S. Ahmad, M. H. Ab Rahim, T. M. Alqahtani, T. Witoon, J.-W. Lim, and C. K. Cheng, “A review on advances in green treatment of glycerol waste with a focus on electro-oxidation pathway,” Chemosphere, vol. 276, p. 130128, 2021. https://doi.org/10.1016/j.chemosphere.2021.130128
  23. F. E. Stuart, “Electronic water purification progress report on the electronic coagulator–a new device which gives promise of unusually speedy effective results,” Water sewage, vol. 84, pp. 24–26, 1946.
  24. G. Chen, “Electrochemical technologies in wastewater treatment,” Sep Purif Technol, vol. 38, no. 1, pp. 11–41, 2004. https://doi.org/10.1016/j.seppur.2003.10.006
  25. T. Shahriari, A. R. Karbassi, and M. Reyhani, “Treatment of oil refinery wastewater by electrocoagulation–flocculation (Case Study: Shazand Oil Refinery of Arak),” International Journal of Environmental Science and Technology, vol. 16, pp. 4159–4166, 2019. https://doi.org/10.1007/s13762-018-1810-z
  26. J. N. Hakizimana et al., “Electrocoagulation process in water treatment: A review of electrocoagulation modeling approaches,” Desalination, vol. 404, pp. 1–21, 2017. https://doi.org/10.1016/j.desal.2016.10.011
  27. I. Kabdaşlı, I. Arslan-Alaton, T. Ölmez-Hancı, and O. Tünay, “Electrocoagulation applications for industrial wastewaters: a critical review,” Environmental Technology Reviews, vol. 1, no. 1, pp. 2–45, 2012. https://doi.org/10.1080/21622515.2012.715390
  28. S. K. Ajjam, B. H. Hlih, and H. H. Alwan, “Enhancing lead ion removal from simulated wastewater through continuous electrocoagulation process: investigating operating parameters and adsorption behavior,” Chemical Papers, 2024, doi: 10.1007/s11696-024-03771-1. https://doi.org/10.21203/rs.3.rs-3477742/v1
  29. A. M. Al-Yaqoobi, M. N. Al-Rikabey, and K. H. R. Algharrawi, “Treatment of dairy wastewater by electrocoagulation and ultrasonic-assisted electrocoagulation methods.,” Environmental Engineering & Management Journal (EEMJ), vol. 20, no. 6, 2021. http://www.eemj.icpm.tuiasi.ro/; http://www.eemj.eu
  30. A. M. Al-Yaqoobi, M. N. Al-Rikabey, and M. K. H. Al-Mashhadani, “Electrochemical harvesting of microalgae꞉ Parametric and cost-effectivity comparative investigation,” Chemical Industry and Chemical Engineering Quarterly, vol. 27, no. 2, pp. 121–130, 2021. https://doi.org/10.2298/CICEQ191213031A
  31. A. N. Kassob and A. H. Abbar, “Treatment of petroleum refinery wastewater by graphite–graphite electro fenton system using batch recirculation electrochemical reactor,” Journal of Ecological Engineering, vol. 23, no. 10, pp. 291–303, 2022. https://doi.org/10.12911/22998993/152524
  32. M. A. Aljaleel and H. H. Alwan, “Modeling the Effect of Operation Variables on Copper Ions Removal by Electrocoagulation,” in 2022 2nd International Conference on Advances in Engineering Science and Technology (AEST), 2022, pp. 111–115. https://doi.org/10.1109/AEST55805.2022.10413162
  33. S. R. Korake and P. D. Jadhao, “Investigation of Taguchi optimization, equilibrium isotherms, and kinetic modeling for cadmium adsorption onto deposited silt,” Heliyon, vol. 7, no. 1, 2021. https://doi.org/10.1016/j.heliyon.2020.e05755
  34. U. Sutrisno, Y. Wulandari, S. Arifin, M. M. Manurung, and M. Faisal, “Trends, Contributions and Prospects: Bibliometric Analysis of ANOVA Research in 2022-2023,” Indonesian Journal of Applied Mathematics and Statistics, vol. 1, no. 1, pp. 27–38, 2024. https://doi.org/10.71385/idjams.v1i1.7
  35. E. GilPavas, I. Dobrosz-Gómez, and M.-Á. Gómez-García, “Efficient treatment for textile wastewater through sequential electrocoagulation, electrochemical oxidation and adsorption processes: Optimization and toxicity assessment,” Journal of Electroanalytical Chemistry, vol. 878, p. 114578, 2020. https://doi.org/10.1016/j.jelechem.2020.114578
  36. H. M. Ibrahim, “Study the optimization of petroleum refinery wastewater treatment by successive electrocoagulation and electro-oxidation systems,” Iraqi Journal of Chemical and Petroleum Engineering, vol. 23, no. 1, pp. 31–41, 2022. https://doi.org/10.31699/IJCPE.2022.1.5
  37. Alwan, H. H., Abd, A. A., Makki, H. F., & Othman, M. R. (2024). Optimizing hydrodesulfurization of naphtha using NiMo/graphene catalyst. Journal of Industrial and Engineering Chemistry, 135, 539-551. https://doi.org/10.1016/j.jiec.2024.01.066
  38. R. H. Salman, “Removal of manganese ions (Mn2+) from a simulated wastewater by electrocoagulation/electroflotation technologies with stainless steel mesh electrodes: process optimization based on Taguchi approach,” Iraqi Journal of Chemical and Petroleum Engineering, vol. 20, no. 1, pp. 39–48, 2019. https://doi.org/10.31699/IJCPE.2019.1.6
  39. S. Salvestrini, A. Fenti, S. Chianese, P. Iovino, and D. Musmarra, “Electro-oxidation of humic acids using platinum electrodes: an experimental approach and kinetic modelling. Water 12, 2250,” 2020. https://doi.org/10.3390/w12082250
  40. Q. Li, G. Liu, L. Qi, H. Wang, and G. Xian, “Chlorine-mediated electrochemical advanced oxidation process for ammonia removal: Mechanisms, characteristics and expectation,” Science of The Total Environment, vol. 896, p. 165169, 2023. https://doi.org/10.1016/j.scitotenv.2023.165169
  41. H. Rubí-Juárez, C. Barrera-Díaz, I. Linares-Hernández, C. Fall, and B. Bilyeu, “A combined electrocoagulation-electrooxidation process for carwash wastewater reclamation,” Int J Electrochem Sci, vol. 10, no. 8, pp. 6754–6767, 2015. https://doi.org/10.1016/S1452-3981(23)06759-7
  42. A. S. Fajardo et al., “Electrochemical oxidation of phenolic wastewaters using a batch-stirred reactor with NaCl electrolyte and Ti/RuO2 anodes,” Journal of Electroanalytical Chemistry, vol. 785, pp. 180–189, 2017. https://doi.org/10.1016/j.jelechem.2016.12.033
  43. A. Habl, A. Amooey, M. Mustafa, and H. A. Alalwan, “Electro oxidation process for wastewater treatment in petroleum refineries,” Pollution, vol. 10, no. 2, pp. 819–832, 2024. https://doi.org/10.22059/poll.2024.371677.2236
  44. S. M. Safwat, N. Y. Mohamed, M. N. A. Meshref, and A. Elawwad, “Adsorption of phenol onto aluminum oxide nanoparticles: performance evaluation, mechanism exploration, and principal component analysis (PCA) of thermodynamics,” Adsorpt. Sci. Technol., vol. 2022, p. 1924117, 2022. https://doi.org/10.1155/2022/1924117
  45. N. A. Akhtar and M. Kobya, “Efficient degradation of phenol by electrooxidation process at boron-doped diamond anode system,” MANAS J. Eng., vol. 13, no. 1, pp. 52–63, 2025. https://doi.org/10.51354/mjen.1656854
  46. E. M. Abou‐Taleb, M. S. Hellal, and K. H. Kamal, “Electro‐oxidation of phenol in petroleum wastewater using a novel pilot‐scale electrochemical cell with graphite and stainless‐steel electrodes,” Water Environ. J., vol. 35, no. 1, pp. 259–268, 2021. https://doi.org/10.1111/wej.12624
  47. Y. Zhu, K. Wen, B. Li, Y. Hao, and J. Zhou, “Electrocatalytic Degradation of Phenolic Wastewater Using a Zero-Gap Flow-Through Reactor Coupled with a 3D Ti/RuO2-TiO2@ Pt Electrode,” Molecules, vol. 29, no. 5, p. 1182, 2024. https://doi.org/10.3390/molecules29051182