PbO2 /graphite and graphene/carbon fiber as an electrochemical cell for oxidation of organic contaminants in refinery wastewater by electrofenton process; electrodes preparation, characterization and performance

Year 2024, Volume: 7 Issue: 2, 175 - 185, 30.06.2024

Rowaida Abbas Ammar S. Abbas

https://doi.org/10.35208/ert.1378232

Abstract

The electro-Fenton oxidation process was used to treat organic pollutants in industrial wastewater as it is one of the most efficient advanced oxidation processes. The novel cell in this process consists of a prepared PbO2 electrode by electrodeposition on graphite substrate and carbon fiber modified with graphene as a cathode. X-ray diffraction, fluorescence, analysis system, atomic force microscopy, and scan electron microscopy were used to characterize the prepared anode and cathode. XRD patterns clearly show the characteristic reflection of the mixture of  - and β phases of PbO2 on graphite and carbon fiber, and AFM results for cathode and anode present that PbO2 on graphite substrate and graphene on carbon fiber surface are on a nanoscale. Contact angle measurement was determined for the carbon fiber cathode before and after modification. The anodic polarization curve showed a higher anodic current when utilizing the PbO2 anode than the graphite anode. Phenol in simulated wastewater was removed by electro-Fenton oxidation at 8 mA/cm2 current density, 0.4 mM of ferrous ion concentration at 35 °C up to 6 h of electrolysis. Chemical oxygen demand for the treated solution was removed by 94.02 % using the cell consisting of modified anode and cathode compared with 81.23% using modified anode and unmodified cathode and 79.87 % when using unmodified anode and modified cathode.

Keywords

Phenol removal, graphene, electro-fenton, oxidation, carbon fiber, graphite

References

• H. Abbar, and A. S. Abbas, “A kinetic study of oxalic acid electrochemical oxidation on a manganese dioxide rotating cylinder anode,” Portugaliae Electrochimica Acta, Vol. 36(5), pp. 325–337, 2018. [CrossRef]
• X. Duan, F. Ma, Z. Yuan, L. Chang, and X. Jin, “Electrochemical degradation of phenol in aqueous solution using PbO2 anode,” Journal of the Taiwan Institute of Chemical Engineers, Vol. 44(1), pp. 95–102, 2013. [CrossRef]
• R. G. Saratale, K.-J. Hwang, J.-Y. Song, G. Dattatray Saratale, and D.-S. Kim, “Electrochemical oxidation of phenol for wastewater treatment using Ti/PbO2 electrode,” Journal of Environmental Engineering(United States), Vol. 142(2), pp. 1–9, 2016. [CrossRef]
• R. N. Abbas, and A. S. Abbas, “Feasibility of using carbon fiber, graphite, and their modified versions by PbO2 as electrodes in electrochemical oxidation of phenolic wastewater,” AIP Conference Proceedings, Vol. 2660, 2022. [CrossRef]
• I. Polaert, A. M. Wilhelm, and H. Delmas, “Phenol wastewater treatment by a two-step adsorption-oxidation process on activated carbon, Chemie-Ingenieur-Technik, Vol. 73(6), pp. 1585–1590, 2001. [CrossRef]
• F. Zhang, M. Li, W. Li, C. Feng, Y. Jin, X. Guo, and J. Cui, “Degradation of phenol by a combined independent photocatalytic and electrochemical process,” in Chemical Engineering Journal, Vol. 175(1), pp. 349–355, 2011. [CrossRef]
• R. N. Abbas, and A. S. Abbas, “The Taguchi approach in studying and optimizing the electro-fenton oxidation to reduce organic contaminants in refinery wastewater using novel electrodes,” Engineering, Technology & Applied Science Research, Vol. 12(4), pp. 8928–8935, 2022. [CrossRef]
• N. Bensalah, and A. Bedoui, “Enhancing the performance of electro-peroxone by incorporation of UV irradiation and BDD anodes,” Environmental Technology, Vol. 38(23), pp. 1–28, 2017. [CrossRef]
• P. H. Britto-Costa and L. A. M. M. Ruotolo, “Phenol removal from wastewaters by electrochemical oxidation using boron doped diamond (BDD) and ti/ti0.7ru0.3o2 dsa® electrodes,” Brazilian Journal of Chemical Engineering, Vol. 29(4), pp. 763–773, 2012. [CrossRef]
• P. Jin, R. Chang, D. Liu, K. Zhao, L. Zhang, and Y. Ouyang, “Phenol degradation in an electrochemical system with TiO 2/activated carbon fiber as electrode,” The Journal of Environmental Chemical Engineering, Vol. 2(2), pp. 1040–1047, 2014. [CrossRef]
• M. H. El-Naas, S. Al-Zuhair, and M. A. Alhaija, “Removal of phenol from petroleum refinery wastewater through adsorption on date-pit activated carbon,” in Chemical Engineering Journal, Vol. 162(3), pp. 997–1005, 2010. [CrossRef]
• Y. X. Liu, Z. Y. Liao, X. Y. Wu, C. J. Zhao, Y. Xin Lei, and D. B. Ji “Electrochemical degradation of methylene blue using electrodes of stainless steel net coated with single-walled carbon nanotubes,” Desalination and Water Treatment, Vol. 54(10), pp. 2757–2764, 2015. [CrossRef]
• N. Jarrah, and N. D. Mu'Azu, “Simultaneous electro-oxidation of phenol, CN-, S2- and NH4+ in synthetic wastewater using boron doped diamond anode,” Journal of Environmental Chemical Engineering, Vol. 4(3), pp. 2656–2664, 2016. [CrossRef]
• Q. J. Rasheed, K. Pandian, and K. Muthukumar, “Treatment of petroleum refinery wastewater by ultrasound-dispersed nanoscale zero-valent iron particles,” Ultrasonics Sonochemistry, Vol. 18(5), pp. 1138–1142, 2011. [CrossRef]
• M. Zhou, Q. Yu, L. Lei, and G. Barton, and “Electro-Fenton method for the removal of methyl red in an efficient electrochemical system,” Separation and Purification Technology, Vol. 57, pp. 380–387, 2007. [CrossRef]
• E. Rosales, M. Pazos, M. A. Longo, and M. A. Sanromán, “Electro-Fenton decoloration of dyes in a continuous reactor : A promising technology in colored wastewater treatment,” Chemical Engineering Journal, Vol. 155, pp. 62–67, 2009. [CrossRef]
• 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(14), pp. 8336–8367, 2014. [CrossRef]
• M. S. Lucas, and J. A. Peres, “Decolorization of the azo dye Reactive Black 5 by Fenton and photo-Fenton oxidation,” Dyes and Pigments, Vol. 71(3), pp. 236–244, 2006. [CrossRef]
• A. Alvarez-Gallegos, and D. Pletcher, “The removal of low level organics via hydrogen peroxide formed in a reticulated vitreous carbon cathode cell, Part 1. The electrosynthesis of hydrogen peroxide in aqueous acidic solutions,” Electrochimica Acta, Vol. 44(5), pp. 853–861, 1998. [CrossRef]
• M. Panizza, and G. Cerisola, “Electrochemical generation of H2O2 in low ionic strength media on gas diffusion cathode fed with air,” Electrochimica Acta, Vol. 54(2), pp. 876–878, 2008. [CrossRef]
• Z. I. Abbas, and A. S. Abbas, “Oxidative degradation of phenolic wastewater by electro-fenton process using MnO2-graphite electrode,” The Journal of Environmental Chemical Engineering, Vol. 7(3), Article 103108, 2019. [CrossRef]
• R. N. Abbas, and A. S. Abbas, “Kinetics and energetic parameters study of phenol removal from aqueous solution by electro-fenton advanced oxidation using modified electrodes with PbO2 and graphene. Iraqi Journal of Chemical and Petroleum Engineering, Vol. 23(2), pp. 1–8, 2022. [CrossRef]
• M. Panizza, and M. A. Oturan, “Degradation of Alizarin Red by electro-Fenton process using a graphite-felt cathode,” Electrochimica Acta, Vol. 56(20), pp. 7084–7087, 2011. [CrossRef]
• Y. Yavuz, A. S. Koparal, and Ü. B. Öǧütveren, “Treatment of petroleum refinery wastewater by electrochemical methods,” Desalination, Vol. 258(1–3), pp. 201–205, 2010. [CrossRef]
• A. S. Abbas, M. H. Hafiz, and R. H. Salman, “Indirect electrochemical oxidation of phenol using rotating cylinder reactor,” Iraqi Journal of Chemical and Petroleum Engineering, Vol. 17(4), pp. 43–55, 2016. [CrossRef]
• A. H. Abbar, R. H. Salman, and A. S. Abbas, “Electrochemical ıncineration of oxalic acid at manganese dioxide rotating cylinder anode: Role of operative parameters in the presence of NaCl,” Journal of the Electrochemical Society, Vol. 163(13), pp. E333–E340, 2016. [CrossRef]
• D. Rajkumar, J. G. Kim, and K. Palanivelu, “Indirect electrochemical oxidation of phenol in the presence of chloride for wastewater treatment,” Chemical Engineering & Technology, Vol. 28(1), pp. 98–105, 2005. [CrossRef]
• Y. Jiang, H. Zhao, J. Liang, L. Yue, T. Li, Y. Luo, Q. Liu, S. Lu, A. M. Asiri, Z. Gong, and X. Sun, “Anodic oxidation for the degradation of organic pollutants: Anode materials, operating conditions, and mechanisms. A mini review,” Electrochemistry Communications, Vol. 123, Article 106912, 2021. [CrossRef]
• C. Shao, F. Zhang, X. Li, J. Zhang, Y. Jiang, H. Cheng, and K. Zhu, “Influence of Cr doping on the oxygen evolution potential of SnO2/Ti and Sb-SnO2/Ti electrodes,” Journal of Electroanalytical Chemistry, Vol. 832, pp. 436–443, 2019. [CrossRef]
• R. M. Farinos, R. L. Zornitta, and L. A. M. M. Ruotolo, “Development of three-dimensional electrodes of PbO2 electrodeposited on reticulated vitreous carbon for organic eletrooxidation,” Journal of the Brazilian Chemical Society, Vol. 28(1), pp. 187–196, 2017. [CrossRef]
• X. Wu, H. Xu, L. Lu, H. Zhao, J. Fu, Y. Shen, P. Xu, and Y. Dong, “PbO2-modified graphite felt as the positive electrode for an all-vanadium redox flow battery,” Journal of Power Sources, Vol. 250, pp. 274–278, 2014. [CrossRef]
• V. Suryanarayanan, I. Nakazawa, S. Yoshihara, and T. Shirakashi, “The influence of electrolyte media on the deposition/dissolution of lead dioxide on boron-doped diamond electrode - A surface morphologic study,” Journal of Electroanalytical Chemistry, Vol. 592(2), pp. 175–182, 2006. [CrossRef]
• C. Borrás, P. Rodríguez, T. Laredo, J. Mostany, and B. R. Scharifker, “Electrooxidation of aqueous p-methoxyphenol on lead oxide electrodes,” Journal of Applied Electrochemistry, Vol. 34(6), pp. 583–589, 2004. [CrossRef]
• Y. Wang, Y. Liu, K. Wang, S. Song, P. Tsiakaras, and H. Liu, “Preparation and characterization of a novel KOH activated graphite felt cathode for the electro-Fenton process,” Applied Catalysis B: Environmental, Vol. 165, pp. 360–368, 2015. [CrossRef]
• Z. Pan, K. Wang, Y. Wang, P. Tsiakaras, and S. Song, “In-situ electrosynthesis of hydrogen peroxide and wastewater treatment application: A novel strategy for graphite felt activation,” Applied Catalysis B: Environmental, Vol. 237, pp. 392–400, 2018. [CrossRef]
• W. Yang, M. Zhou, N. Oturan, Y. Li, and M. A. Oturan, “Electrocatalytic destruction of pharmaceutical imatinib by electro-Fenton process with graphene-based cathode,” Electrochimica Acta, Vol. 305, pp. 285–294, 2019. [CrossRef]
• H. Mo, Y. Tang, X. Wang, J. Liu, D. Kong, Y. Chen, P. Wan, H. Cheng, T. Sun, L. Zhang, M. Zhang, S. Liu, Y. Sun, N. Wang, L. Xing, L. Wang, Y. Jiang, X. Xu, Y. Zhang, and X. Meng, “Development of a three-dimensional structured carbon fiber Felt/β-PbO2 electrode and ıts application in chemical oxygen demand determination,” Electrochimica Acta, Vol. 176, pp. 1100–1107, 2015. [CrossRef]
• N. Yu, L. Gao, S. Zhao, and Z. Wang, “Electrodeposited PbO2 thin film as positive electrode in PbO2/AC hybrid capacitor,” Electrochimica Acta, Vol. 54(14), pp. 3835–3841, 2009. [CrossRef]
• T. M. Garakani, P. Norouzi, M. Hamzehloo, and M. R. Ganjali, “Electrodeposition of nano-structured PbO 2 on glassy carbon electrodes by FFT continuous cyclic voltammetry,” International Journal of Electrochemical Science, Vol. 7(1), pp. 857–874, 2012. [CrossRef]
• W. Yang, M. Zhou, J. Cai, L. Liang, G. Ren, and L. Jiang, “Ultrahigh yield of hydrogen peroxide on graphite felt cathode modified with electrochemically exfoliated graphene,” Journal of Materials Chemistry A, Vol. 5(17), pp. 8070–8080, 2017. [CrossRef]
• T. X. Houng Le, M. Bechelany, S. Lacour, N. Oturan, M. A. Oturan, and M. Cretin, “High removal efficiency of dye pollutants by electron-Fenton process using a graphene-based cathode,” Carbon NY, Vol. 94, pp. 1003–1011, 2015. [CrossRef]
• L. P. Bicelli, B. Bozzini, C. Mele, and L. D. Urzo, “A review of nanostructural aspects of metal electrodeposition,” International Journal of Electrochemical Science, Vol. 3, pp. 356–408, 2008. [CrossRef]
• J. Liu, X. Sun, P. Song, Y. Zhang, W. Xing, and W. Xu, “High-performance oxygen reduction electrocatalysts based on cheap carbon black, nitrogen, and trace Iron,” Advanced Materials, Vol. 25(47), pp. 6879–6883, 2013. [CrossRef]
• C. Trellu, N. Oturan, F. K. Keita, C. Fourdrin, Y. Pechaud, and M. A. Oturan, “Regeneration of activated carbon fiber by the electro-fenton process,” Environmental Science & Technology, Vol. 52(13), pp. 7450–7457, 2018. [CrossRef]
• J. Guo, T. Zhang, C. Hu, and L. Fu, “A three-dimensional nitrogen-doped graphene structure: A highly efficient carrier of enzymes for biosensors,” Nanoscale, Vol. 7(4), pp. 1290–1295, 2015. [CrossRef]
• S. D. Sklari, K. V Plakas, P. N. Petsi, V. T. Zaspalis, and A. J. Karabelas, “Toward the development of a novel electro-fenton system for eliminating toxic organic substances from water. Part 2. Preparation, characterization, and evaluation of ıron-ımpregnated carbon felts as cathodic electrodes,” Industrial & Engineering Chemistry Research, Vol. 54(7), pp. 2059–2073, 2015. [CrossRef]
• W. Yang, M. Zhou, and L. Liang, “Highly efficient in-situ metal-free electrochemical advanced oxidation process using graphite felt modified with N-doped graphene, Chemical Engineering Journal, Vol. 338, pp. 700–708, 2018. [CrossRef]
• G. Divyapriya, I. M. Nambi, and J. Senthilnathan, “An innate quinone functionalized electrochemically exfoliated graphene/Fe3O4 composite electrode for the continuous generation of reactive oxygen species,” Chemical Engineering Journal, Vol. 316, pp. 964–977, 2017. [CrossRef]
• Y. Zhou, Q. Bao, L. A. L. Tang, Y. Zhong, and K. P. Loh, “Hydrothermal dehydration for the 'green' reduction of exfoliated graphene oxide to graphene and demonstration of tunable optical limiting properties,” Chemistry of Materials, Vol. 21(13), pp. 2950–2956, 2009. [CrossRef]
• T. H. Magn, A. Ping, G. Jingyang, S. Caroline, M. Christos, and C. G. Chen, “Highly-Ordered Magnéli Ti4O7 Nanotube Arrays as Effective Anodic Material for Electro-oxidation,” Elsevier Ltd, 2014.
• G. Li, and Y. Zhang, “Highly selective two-electron oxygen reduction to generate hydrogen peroxide using graphite felt modified with N-doped graphene in an electro-Fenton system,” New Journal of Chemistry, Vol. 43, pp. 1265712667, 2019. [CrossRef]
• A. Mir, D. K. Singh, and A. Shukla, “Size distribution of trilayer graphene flakes obtained by electrochemical exfoliation of graphite: Effect of the synthesis parameters,” Materials Chemistry and Physics, Vol. 220, pp. 87–97, 2018. [CrossRef]
• T. X. Huong Le, B. Alemán, J. J. Vilatela, M. Bechelany, and M. Cretin, “Enhanced electro-fenton mineralization of acid orange 7 using a carbon nanotube fiber-based cathode,” Frontiers of Materials, Vol. 5, pp. 5–10, 2018. [CrossRef]
• S. Akcöltekin, M. El Kharrazi, B. Köhler, A. Lorke, and M. Schleberger, “Graphene on insulating crystalline substrates,” Nanotechnology, Vol. 20(15), 2009. [CrossRef]
• Q. Zhou, X. Zhou, R. Zheng, Z. Liu, and J. Wang, “Application of lead oxide electrodes in wastewater treatment: A review,” Science of Total Environment, Vol. 806, Article 150088, 2022. [CrossRef]
• Z. Zhang, H. Meng, Y. Wang, L. Shi, X. Wang, and S. Chai, “Fabrication of graphene@graphite-based gas diffusion electrode for improving H2O2 generation in Electro-Fenton process,” Electrochimica Acta, Vol. 260, pp. 112–120, 2018. [CrossRef]
• R. N. Abbas, and A. S. Abbas, “Phenol deterioration in refinery wastewater through advanced electrochemical oxidation reactions using different carbon fiber and graphite electrodes configurations,” Egyptian Journal of Chemistry, Vol. 65(12), pp. 463–472, 2022.
• A. S. Fahem, and A. H. Abbar, “Treatment of petroleum refinery wastewater by electro-Fenton process using porous graphite electrodes,” Egyptian Journal of Chemistry, Vol. 63(12), pp. 4805–4819, 2020.
• S. K. Kamal, Z. M. Mustafa, and A. S. Abbas, “Comparative study of organics removal from refinery wastewater by photocatalytic fenton reaction coupled with visible light and ultraviolet ırradiation,” Iraqi Journal of Industrial Research, Vol. 10(3), pp. 22–32, 2023. [CrossRef]
• S. K. Kamal, and A. S. Abbas, “Fenton oxidation reaction for removing organic contaminants in synesthetic refinery wastewater using heterogeneous Fe-Zeolite: An experimental study, optimization, and simulation,” Case Studies in Chemical and Environmental Engineering, Vol. 8, pp. 100458–100458, 2023. [CrossRef]
• S. K. Kamal and A. Abbas, “Decrease in the organic content of refinery wastewater by photocatalytic Fenton oxidation using iron-doped zeolite: Catalyst preparation, characterization, and performance,” Chemical Engineering and Processing - Process Intensification, Vol. 193, pp. 109549–109549, 2023. [CrossRef]