مجله آب و فاضلاب

مجله آب و فاضلاب

حذف رنگ از آب حاوی رنگ‌زای آزو Ponceau 4R با استفاده از فرایند هیبریدی ازن-الکتروفنتون: مطالعه تأثیر پارامترهای عملیاتی و سینتیک فرایند

نوع مقاله : مقاله پژوهشی

نویسندگان
1 کارشناسی ارشد، گروه آب و محیط‌زیست، دانشکده مهندسی عمران، دانشگاه علم و صنعت ایران، تهران، ایران
2 استادیار، گروه آب و محیط‌زیست، دانشکده مهندسی عمران، دانشگاه علم و صنعت ایران، تهران، ایران
10.22093/wwj.2026.588230.3560
چکیده
هدف از انجام این پژوهش، بررسی حذف رنگ از آب حاوی رنگ‌زای آزو Ponceau 4R با استفاده از فرایند هیبریدی ازن- الکتروفنتون و مقایسه آن با هریک از فرایندهای ازن‌زنی و الکتروفنتون به‌تنهایی بود. آزمایش‌ها به‌صورت ناپیوسته و بر اساس روش OFAT انجام شد. تأثیر پارامترهای عملیاتی شامل غلظت الکترولیت سدیم سولفات (Na2SO4) (25/0، 5/2 و mM 25)،pH اولیه (3، 7 و 5/8)، غلظت یون فروس (Fe2+) (1/0، 1 و mM 10)، چگالی جریان اعمالی (05/1، 25/6 و mA/cm26/14) و نرخ تزریق ازن (2/0، 1 و g/h 2) بر بازدهی فرایند ارزیابی شد. در همه آزمایش‌ها، غلظت اولیه رنگ‌زا برابر با 200 و مدت‌زمان واکنش تا 90 دقیقه در نظر گرفته شد. تحت مقدار بهینه پارامترهای عملیاتی (غلظت الکترولیت: mM5/2، pH معادل 3، غلظت یون فروس: m 1، چگالی جریان: mA/cm2 25/6، نرخ تزریق ازن: g/h 2)، بازدهی حذف رنگ در سیستم هیبریدی ازن- الکتروفنتون تنها پس از گذشت 60 دقیقه از زمان واکنش به حدود 100 درصد رسید. در مقایسه، هریک از فرایندهای ازن‌زنی و الکتروفنتون، پس از 90 دقیقه واکنش تحت شرایط بهینه خود، نتوانستند به ترتیب بیش از 89 و 51 درصد حذف رنگ داشته باشند. همچنین نتایج نشان داد که افزایش زمان واکنش تا 90 دقیقه، نامطلوب بودن مقدار همه پارامترهای عملیاتی موردسنجش به‌جز نرخ تزریق ازن را جبران می‌کند. این نتیجه، نقش کلیدی ازن را در تولید رادیکال آزاد هیدروکسیل ( ) در فرایند هیبریدی ازن- الکتروفنتون آشکار ساخت. بررسی مدل‌های سینتیکی نشان داد که سینتیک مرتبه اول با ضریب هم‌بستگی (R2) 994/0، در مقایسه با سینتیک‌ مرتبه دوم با ضریب هم‌بستگی 575/0، از قابلیت بسیار بهتری در تخمین بازدهی فرایند هیبریدی ازن- الکتروفنتون در حذف رنگ، آب حاوی رنگ‌زای P4R دارد. به‌طورکلی، سیستم هیبریدی ازن- الکتروفنتون عملکرد بسیار بهتری نسبت به هر یک از دو فرایند ازن‌زنی و الکتروفنتون نشان داد و با ایجاد هم‌افزایی بین دو فرایند، موجب افزایش سرعت واکنش و دستیابی به رنگ‌زدایی کامل در مدت‌زمان کوتاه شد. ازاین‌رو، می‌توان این فرایند هیبریدی را به‌عنوان جایگزین مناسبی برای سایر روش‌های حذف رنگ‌زا، که عموماً از سرعت کم و عدم دستیابی به حذف کامل آلاینده رنج می‌برند، در نظر گرفت. همچنین، انجام پژوهش در خصوص ابعاد فنی و اقتصادی سیستم هیبریدی ازن- الکتروفنتون، برای پیاده‌سازی فرایند در مقیاس واقعی، ارزشمند بود.
کلیدواژه‌ها
موضوعات

عنوان مقاله English

Decolorization of Ponceau 4R Azo Dye-Containing Water Using Ozone–Electro-Fenton Hybrid Process: Study of the Effect of Operational Parameters and Process Kinetics

نویسندگان English

MirMohammad Azimi Khatibani 1
Maryam Hasani Zonoozi 2
Soroush Dayani Najafabadi 1
1 Master of Science, Water and Environment Group, Dept. of Civil Engineering, Iran University of Science and Technology (IUST), Tehran, Iran
2 Assist. Prof., Water and Environment Group, Dept. of Civil Engineering, Iran University of Science and Technology (IUST), Tehran, Iran
چکیده English

This study aims to investigate the decolorization of Ponceau 4R azo dye-containing water using ozone–Electro-Fenton hybrid process and compare it with each of the ozonation and Electro-Fenton processes alone. The experiments were conducted in a batch mode and based on the OFAT (One Factor at a Time) method. The effect of parameters including sodium sulfate (Na2SO4) electrolyte concentration (0.25, 2.5 and 25 mM), initial pH (3, 7 and 8.5), ferrous ion (Fe2+) concentration (0.1, 1 and 10 mM), applied current density (1.05, 6.25 and 14.6 mA/cm2), and ozone injection rate (0.2, 1 and 2 g/h) on decolorization efficiency was evaluated. In all experiments, the initial dye concentration was kept constant on 200 mg/L and the reaction time was considered to be up to 90 minutes. According to the obtained results, under the optimal values of the operating parameters (electrolyte concentration: 2.5 mM, pH=3, ferrous ion concentration: 1 mM, current density: 6.25 mA/cm2, ozone injection rate: 2 g/h), the decolorization efficiency in the ozone–Electro-Fenton hybrid system reached about 100% only after 60 min of reaction time. In comparison, each of the ozonation and Electro-Fenton processes, failed to achieve more than 89% and 51% efficiencies, respectively, even after 90 minutes of reaction under their optimal conditions. The results also showed that increasing the reaction time to 90 min compensated for the undesirability of all the operating parameters measured except the ozone injection rate. This result revealed the key role of ozone in the production of hydroxyl free radicals ( ) in the ozone-Electro-Fenton hybrid process. Examination of kinetic models showed that the first-order kinetics with a correlation coefficient (R2) of 0.994, compared to the second-order kinetics with a correlation coefficient of 0.575, has a much better ability to estimate the decolorization performance of the hybrid process. In general, the ozone–Electro-Fenton hybrid system showed much better performance than either ozonation or Electro-Fenton processes. The hybrid system increased the reaction speed and achieved complete decolorization in a short time by creating synergy between the two processes. Therefore, the ozone–Electro-Fenton hybrid system can be considered as a suitable alternative to other dye removal methods, which generally suffer from low speed and failure to achieve complete removal of the pollutant. Accordingly, conducting researches on the technical and economic aspects of the ozone–Electro-Fenton hybrid process is valuable for implementing the process on a real scale.

کلیدواژه‌ها English

Advanced Oxidation
Dye Containing Wastewater
Ponceau 4R Azo Dye
Ozonation
Electro-Fenton
Ozone-Electro-Fenton Hybrid Process
Abdolkarimi-Mahabadi, M. and Bayat, A., 2023. Investigating the treatment of paper industry effluent using ozonation process. Journal of Water and Wastewater, 34(4), 123-136. (In Persian). https://doi.org/10.22093/wwj.2023.401406.3363.
Abdolkarimi-Mahabadi, M. and Bayat, A., 2024. Optimization of the peroxone process for paper industry wastewater treatment using the Box-Behnken Design method. Journal of Water and Wastewater, 35(1), 40-57. (In Persian). https://doi.org/10.22093/wwj.2024.416748.3371.
Alabdraba, W. M. S., Hamed, H. H. and Mohammed, A. E., 2020. Performance evaluation of combined O3/Fenton process on decolorization and COD removal of disperse blue 79 dye from aqueous solution. Desalination and Water Treatment, 173, 420-426. https://doi.org/10.5004/dwt.2020.24680.
Azbar, N., Yonar, T. and Kestioglu, K., 2004. Comparison of various advanced oxidation processes and chemical treatment methods for COD and color removal from a polyester and acetate fiber dyeing effluent. Chemosphere, 55(1), 35–43. https://doi.org/10.1016/j.chemosphere.2003.10.046.
Basiri Parsa, J. and Abbasi, M., 2012. Application of in situ electrochemically generated ozone for degradation of anthraquinone dye Reactive Blue 19. Journal of Applied Electrochemistry, 42(6), 435-442. https://doi.org/10.1007/s10800-012-0417-1.
Basiri Parsa, J., Golmirzaei, M. and Abbasi, M., 2014. Degradation of azo dye C.I. Acid Red 18 in aqueous solution by ozone-electrolysis process. Journal of Industrial and Engineering Chemistry, 20(2), 689–694. https://doi.org/10.1016/j.jiec.2013.05.034.
Brillas, E. and Martínez-Huitle, C. A., 2015. Decontamination of wastewaters containing synthetic organic dyes by electrochemical methods: an updated review. Applied Catalysis B: Environmental, 166-167, 603-643. https://doi.org/10.1016/j.apcatb.2014.11.016.
Cañizares, P., Hernández-Ortega, M., Rodrigo, M. A., Barrera-Díaz, C. E., Roa-Morales, G. and Sáez, C., 2009. A comparison between conductive-diamond electrochemical oxidation and other advanced oxidation processes for the treatment of synthetic melanoidins. Journal of Hazardous Materials, 164(1), 120-125. https://doi.org/10.1016/j.jhazmat.2008.07.134.
Carneiro, P. A., Osugi, M. E., Fugivara, C. S., Boralle, N., Furlan, M. and Zanoni, M. V. B., 2005. Evaluation of different electrochemical methods on the oxidation and degradation of Reactive Blue 4 in aqueous solution. Chemosphere, 59(3), 431-439. https://doi.org/10.1016/j.chemosphere.2004.10.043.
Chen, G. S. and Sheu, R. D., 2004. Application of two preconditioned generalized conjugate gradient methods to three-dimensional neutron and photon transport equations. Progress in Nuclear Energy, 45(1), 11–23. https://doi.org/10.1016/j.pnucene.2004.08.003.
Chen, T. Y., Kao, C. M.,  Hong, A.,  Lin, C. E. and  Liang, S. H., 2009. Application of ozone on the decolorization of reactive dyes- Orange-13 and Blue-19. Desalination, 249(3), 1238-1242. https://doi.org/10.1016/j.desal.2008.10.032.
Chowdhury, S. and Bhattacharyya, K. G., 2019. Oxidative degradation of Congo red using zeolite Y as a support for Co(II), Ni(II) and Cu(II) ions. SN Applied Sciences, 1, 1224. https://doi.org/10.1007/s42452-019-1261-2.
Cuiping, B., Xianfeng, X., Wenqi, G., Dexin, F., Mo, X., Zhongxue, G. et al., 2011. Removal of rhodamine B by ozone-based advanced oxidation process. Desalination, 278(1-3), 84-90. https://doi.org/10.1016/j.desal.2011.05.009.
De Oliveira, G. R., Fernandes, N. S., De Melo, J. V., Da Silva, D. R., Urgeghe, C. and Martínez-Huitle, C. A., 2011. Electrocatalytic properties of Ti-supported Pt for decolorizing and removing dye from synthetic textile wastewaters. Chemical Engineering Journal, 168(1), 208-214. https://doi.org/10.1016/j.cej.2010.12.070.
De Souza, S. M. D. A. G. U., Bonilla, K. A. S. and De Souza, A. A. U., 2010. Removal of COD and color from hydrolyzed textile azo dye by combined ozonation and biological treatment. Journal of Hazardous Materials, 179(1), 35-42. https://doi.org/10.1016/j.jhazmat.2010.02.053.
Ding, Y., Wang, J. and Tan, B., 2024. The removal of organic contaminants from condensed wastewater using electrolysis combined with ozonation: a pilot-scale study. Separations, 11(10), 281. https://doi.org/10.3390/separations11100281.
Divyapriya, G. and Nidheesh, P. V., 2021. Electrochemically generated sulfate radicals by boron doped diamond and its environmental applications. Current Opinion in Solid State and Materials Science, 25(3), 100921. https://doi.org/10.1016/j.cossms.2021.100921.
Do, N. H. N., Truong, B. Y., Nguyen, P. T. X.,  Le, K. A., Duong, H. M. and Le, P. K., 2022. Composite aerogels of TEMPO-oxidized pineapple leaf pulp and chitosan for dyes removal. Separation and Purification Technology, 283, 120200. https://doi.org/10.1016/j.seppur.2021.120200.
Foo, K. Y. and Hameed, B. H., 2010. Insights into the modeling of adsorption isotherm systems. Chemical Engineering Journal, 156(1), 2-10. https://doi.org/10.1016/j.cej.2009.09.013.
García-Espinoza, J. D., Robles, I., Durán-Moreno, A. and Godínez, L. A., 2021. Study of simultaneous electro-Fenton and adsorption processes in a reactor containing porous carbon electrodes and particulate activated carbon. Journal of Electroanalytical Chemistry, 895, 115476. https://doi.org/10.1016/j.jelechem.2021.115476.
Gujar, S. K. and Gogate, P. R., 2021. Application of hybrid oxidative processes based on cavitation for the treatment of commercial dye industry effluents. Ultrasonics Sonochemistry, 75, 105586. https://doi.org/10.1016/j.ultsonch.2021.105586.
Gunten, U. V., 2003. Ozonation of drinking water: Part I. oxidation kinetics and product formation. Water Research, 37(7), 1443–1467. https://doi.org/10.1016/S0043-1354(02)00457-8.
Herrera-Chávez, S., Pacheco-Álvarez, M., Godínez, L. A., Brillas, E. and Peralta-Hernández, J. M., 2025. Hybrid solar photoelectro-fenton and ozone processes for the sustainable removal of COVID-19 pharmaceutical contaminants. Processes, 13(10), 3234. https://doi.org/10.3390/pr13103234.
Jung, Y. J., Baek, K. W., Soo Oh, B. and Kang, J. W., 2010. An investigation of the formation of chlorate and perchlorate during electrolysis using Pt/Ti electrodes: the effects of pH and reactive oxygen species and the results of kinetic studies. Water Research, 44(18), 5345-5355. https://doi.org/10.1016/j.watres.2010.06.029.
Kishimoto, N., Morita, Y., Tsuno, H., Oomura, T. and Mizutani, H., 2005. Advanced oxidation effect of ozonation combined with electrolysis. Water Research, 39(19), 4661-4672. https://doi.org/10.1016/j.watres.2005.09.001.
Konsowa, A. H., Ossman, M. E., Chen, Y. and  Crittenden, J. C., 2010. Decolorization of industrial wastewater by ozonation followed by adsorption on activated carbon. Journal of Hazardous Materials, 176(1-3), 181–185. https://doi.org/10.1016/j.jhazmat.2009.11.010.
Koparal, A. S., Yavuz, Y., Gürel, C. and Öğütveren, Ü. B., 2007. Electrochemical degradation and toxicity reduction of C.I. Basic Red 29 solution and textile wastewater by using diamond anode. Journal of Hazardous Materials, 145(1-2), 100–108. https://doi.org/10.1016/j.jhazmat.2006.10.090.
Kusic, H., Koprivanac, N. and Bozic, A. L., 2006. Minimization of organic pollutant content in aqueous solution by means of AOPs: UV- and ozone-based technologies. Chemical Engineering Journal, 123(3), 127-137. https://doi.org/10.1016/j.cej.2006.07.011.
Madhavan, J., Grieser, F. and Ashokkumar, M., 2010. Degradation of orange-G by advanced oxidation processes. Ultrasonics Sonochemistry, 17(2), 338-343. https://doi.org/10.1016/j.ultsonch.2009.10.008.
Mansour, D., Fourcade, F., Bellakhal, N., Dachraoui, M., Hauchard, D. and Amrane, A., 2012. Biodegradability improvement of sulfamethazine solutions by means of an electro-fenton process. Water, Air and Soil Pollution, 223(5), 2023-2034. https://doi.org/10.1007/s11270-011-1002-7.
Mansour, D., Fourcade, F., Huguet, S., Soutrel, I., Bellakhal, N., Dachraoui, M. et al., 2014. Improvement of the activated sludge treatment by its combination with electro fenton for the mineralization of sulfamethazine. International Biodeterioration and Biodegradation, 88, 29-36. https://doi.org/10.1016/j.ibiod.2013.11.016.
Muthukumar, M., Karuppiah, M. T. and Raju, G. B., 2007. Electrochemical removal of C.I. Acid Orange 10 from aqueous solutions. Separation and Purification Technology, 55(2), 198-205. https://doi.org/10.1016/j.seppur.2006.11.014.
Najafinejad, M. S., Chianese, S., Fenti, A., Iovino, P. and Musmarra, D., 2023. Application of electrochemical oxidation for water and wastewater treatment: an overview. Molecules, 28(10), 4208. https://doi.org/10.3390/molecules28104208.
Oturan, M. A., 2021. Outstanding performances of the BDD film anode in electro-fenton process: applications and comparative performance. Current Opinion in Solid State and Materials Science, 25(3), 100925. https://doi.org/10.1016/j.cossms.2021.100925.
Paba, G. M., Ávila, R. B. and Baldiris, D. B., 2021. Application of environmental bacteria as potential methods of azo dye degradation systems. Global Journal of Environmental Science and Management, 7(1), 131–154. https://doi.org/10.22034/gjesm.2021.01.10.
Panizza, M., Barbucci, A., Ricotti, R. and Cerisola, G., 2007. Electrochemical degradation of methylene blue. Separation and Purification Technology, 54(3), 382-387. https://doi.org/10.1016/j.seppur.2006.10.010.
Puga, A., Moreira, M. M., Figueiredo, S. A., Matos, C. D., Pazos, M.,  Rosales, E., et al., 2021. Electro-Fenton degradation of a ternary pharmaceutical mixture and its application in the regeneration of spent biochar. Journal of Electroanalytical Chemistry, 886, 115135. https://doi.org/10.1016/j.jelechem.2021.115135.
Rosenfeldt, E. J., Linden, K. G., Canonica, S. and Gunten, U. V., 2006. Comparison of the efficiency of OH radical formation during ozonation and the advanced oxidation processes O3/H2O2 and UV/H2O2. Water Research, 40(20), 3695–3704. https://doi.org/10.1016/j.watres.2006.09.008.
Saha, P., Wang, J., Zhou, Y., Carlucci, L., Jeremiasse A. W., Rijnaarts, H. H. M. et al., 2022. Effect of electrolyte composition on electrochemical oxidation: active sulfate formation, benzotriazole degradation, and chlorinated by-products distribution. Environmental Research, 211, 113057. https://doi.org/10.1016/j.envres.2022.113057.
Sevimli, M. F. and Sarikaya, H. Z., 2005. Effect of some operational parameters on the decolorization of textile effluents and dye solutions by ozonation. Environmental Technology, 26(2), 135-144. https://doi.org/10.1080/09593332608618573.
Shaban, M., Abukhadra, M. R., Ibrahim, S. S. and Shahien, M. G., 2017. Photocatalytic degradation and photo-Fenton oxidation of Congo red dye pollutants in water using natural chromite-response surface optimization. Applied Water Science, 7(8), 4743-4756. https://doi.org/10.1007/s13201-017-0637-y.
Shen, Y., Xu, Q., Shi, J., Li, M. and Zhang, Y., 2017. Optimization and mechanism study of C.I. Acid Blue 25 wastewater degradation by ozone/fenton oxidation process: response surface methodology, intermediate products and degradation pathway. Desalination and Water Treatment, 65, 313–326. https://doi.org/10.5004/dwt.2017.20288.
Tanveer, R., Yasar, A., Tabinda, A. B., Ikhlaq, A., Nissar, H. and Nizami, A. S., 2022. Comparison of ozonation, fenton, and photo-fenton processes for the treatment of textile dye-bath effluents integrated with electrocoagulation. Journal of Water Process Engineering, 46, 102547. https://doi.org/10.1016/j.jwpe.2021.102547.
Wakelyn, P. J., 2007. Health and Safety Issues in Cotton Production and Processing, In Gordon, S. and Hsieh, Y. L., Eds. Cotton. Woodhead Publishing, Elsevier, pp. 460-483. https://doi.org/10.1533/9781845692483.3.460.
Wang, L., Cao, M., Ai, Z. and Zhang, L., 2015. Design of a highly efficient and wide ph electro-fenton oxidation system with molecular oxygen activated by ferrous–tetrapolyphosphate complex. Environmental Science and Technology, 49(5), 3032–3039. https://doi.org/10.1021/es505984y.
Zhou, J., 2020. Efficient photo-Fenton degradation of dye and drug molecules over Fe2O3/C composite with 1,4-benzoquinone as sacrificial agent. Desalination and Water Treatment, 183, 335-345. https://doi.org/10.5004/dwt.2020.25239.
Zhou, S., Bu, L., Shi, Z., Bi, C. and Yi, Q., 2016. A novel advanced oxidation process using iron electrodes and ozone in atrazine degradation: performance and mechanism. Chemical Engineering Journal, 306, 719-725. https://doi.org/10.1016/j.cej.2016.08.001.
Zwane, B. N. Orimolade, B. O., Koiki, B. A., Mabuba, N., Gomri, C., Petit, E. et al., 2021. Combined electro-fenton and anodic oxidation processes at a sub-stoichiometric titanium oxide (Ti4O7) ceramic electrode for the degradation of tetracycline in water. Water, 13(19), 2772. https://doi.org/10.3390/w13192772.