Persülfatın Heterojen Aktivasyonu için Aktif Karbon Destekli Kobalt-Bazlı Katalizör Kullanılarak Fenoprofenin Degradasyonu

Yıl 2022, Cilt: 3 Sayı: 2, 71 - 81, 30.12.2022

Hatice Erdem , Mehmet Erdem

Öz

Bu çalışma aktif karbon destekli kobalt-bazlı katalizör (Co-AC) ile persülfatın (PS) heterojen aktivasyonu yoluyla fenoprofenin (FNP) degradsyonununu araştırmayı amaçlamaktadır. FNP degradasyonuna PS konsantrasyonu, Co-AC dozajı, başlangıç pH’sı, ve anyonların etkileri incelenmiştir. 120 dk temas süresi, 0.75 g/L Co-AC, 2 mM PS, doğal pH ve 25 °C optimum işletme koşullarında FNP’nin tam degradasyonu ve mineralizasyonu sağlanmıştır. FNP degradasyonunun pseudo-birinci dereceden kinetik modele en iyi uyduğu bulunmuştur. Belirli alkoller kullanılarak geçekleştirilen söndürme çalışmaları ile degradasyonda etkili reaktif oksijen türleri tespit edilmiştir ve SO4•−‘ün dominant radikal olduğu bulunmuştur. İlaveten, NO3−, SO42− ve PO43− anyonlarının varlığının FNP degradasyonunu inhibe ettiği belirlenmiştir. Elde edilen bu sonuçlar sucul ortamlardan FNP degradasyonu için Co-AC/PS sisteminin umut vaat eden etkili bir proses olduğunu göstermektedir.

Anahtar Kelimeler

fenoprofen, cobalt, aktif karbon, sülfat radikali, degradasyon, heterojen katalizör

Destekleyen Kurum

TÜBİTAK

Proje Numarası

117Y300

Degradation of Fenoprofen Using Activated Carbon Supported Cobalt-Based Catalyst for Heterogeneous Activation of Persulfate

Öz

This study aims to investigate the degradation of fenoprofen (FNP) by heterogeneous activation of persulfate (PS) with the activated carbon supported cobalt-based catalyst (Co-AC). The effects of PS concentration, Co-AC dosage, initial pH, and anions on FNP degradation were investigated. FNP was completely degraded and mineralized under optimum operating conditions of 120 min contact time, 0.75 g/L Co-AC, 2 mM PS, natural pH and 25 °C. FNP degradation was found to best fit the pseudo-first order kinetic model. With quenching studies using certain alcohols, the reactive oxygen species effective in degradation were determined and SO4•− was found to be the dominant radical. In addition, the presence of NO3−, SO42− and PO43− anions were found to inhibit FNP degradation. These results indicate that the Co-AC/PS system is a promising and effective process for the degradation of FNP from aquatic environments.

Proje Numarası

117Y300

Kaynakça

• 1. Marinho, B.A., Suhadolnik, L., Likozar, B., Huš, M., Marinko, Ž., Čeh, M. Photocatalytic, electrocatalytic and photoelectrocatalytic degradation of pharmaceuticals in aqueous media: Analytical methods, mechanisms, simulations, catalysts and reactors. Journal of Cleaner Production, 343, 131061, 2022, doi:https://doi.org/10.1016/j.jclepro.2022.131061
• 2. Ihsanullah, I., Khan, M.T., Zubair, M., Bilal, M., Sajid, M. Removal of pharmaceuticals from water using sewage sludge-derived biochar: A review. Chemosphere, 289, 133196, 2022, doi:https://doi.org/10.1016/j.chemosphere.2021.133196
• 3. Shanavas, S., Haija, M.A., Singh, D.P., Ahamad, T., Roopan, S.M., Van Le, Q., Acevedo, R., Anbarasan, P.M. Development of high efficient Co3O4/Bi2O3/rGO nanocomposite for an effective photocatalytic degradation of pharmaceutical molecules with improved interfacial charge transfer. Journal of Environmental Chemical Engineering, 10(2), 107243, 2022, doi:https://doi.org/10.1016/j.jece.2022.107243
• 4. Zhang, H., Li, H., Wang, Z., Li, B., Cheng, X., Cheng, Q. Synthesis of Magnetic CoFe₂O₄ Nanoparticles and Their Efficient Degradation of Diclofenac by Activating Persulfate via Formation of Sulfate Radicals. J Nanosci Nanotechnol, 18(10), 6942-6948, 2018, doi:https://doi.org/10.1166/jnn.2018.15800
• 5. Duan, X., Niu, X., Gao, J., Wacławek, S., Tang, L., Dionysiou, D.D. Comparison of sulfate radical with other reactive species. Current Opinion in Chemical Engineering, 38, 100867, 2022, doi:https://doi.org/10.1016/j.coche.2022.100867
• 6. Wu, M., Fu, K., Deng, H., Shi, J. Cobalt tetracarboxyl phthalocyanine-manganese octahedral molecular sieve (OMS-2) as a heterogeneous catalyst of peroxymonosulfate for degradation of diclofenac. Chemosphere, 219, 756-765, 2019, doi:https://doi.org/10.1016/j.chemosphere.2018.12.030
• 7. Li, Z., Yang, Q., Zhong, Y., Li, X., Zhou, L., Li, X., Zeng, G. Granular activated carbon supported iron as a heterogeneous persulfate catalyst for the pretreatment of mature landfill leachate. RSC Advances, 6(2), 987-994, 2016, doi: https://doi.org/10.1039/C5RA21781D
• 8. Chen, L., Ji, H., Qi, J., Huang, T., Wang, C.-C., Liu, W. Degradation of acetaminophen by activated peroxymonosulfate using Co(OH)2 hollow microsphere supported titanate nanotubes: Insights into sulfate radical production pathway through CoOH+ activation. Chemical Engineering Journal, 406, 126877, 2021, doi:https://doi.org/10.1016/j.cej.2020.126877
• 9. Xiao, S., Cheng, M., Zhong, H., Liu, Z., Liu, Y., Yang, X., Liang, Q. Iron-mediated activation of persulfate and peroxymonosulfate in both homogeneous and heterogeneous ways: A review. Chemical Engineering Journal, 384, 123265, 2020, doi:https://doi.org/10.1016/j.cej.2019.123265
• 10. Zhao, C., Zhong, S., Li, C., Zhou, H., Zhang, S. Property and mechanism of phenol degradation by biochar activated persulfate. Journal of Materials Research and Technology, 9(1), 601-609, 2020, doi:https://doi.org/10.1016/j.jmrt.2019.10.089
• 11. Farghaly, D.A., Aboelwafa, A.A., Hamza, M.Y., Mohamed, M.I. Microemulsion for topical delivery of fenoprofen calcium: in vitro and in vivo evaluation. Journal of Liposome Research, 28(2), 126-136, 2018, doi: https://doi.org/10.1080/08982104.2017.1281951
• 12. Mbhele, Z.E., Ncube, S., Madikizela, L.M. Synthesis of a molecularly imprinted polymer and its application in selective extraction of fenoprofen from wastewater. Environmental Science and Pollution Research 25(36), 36724-36735, 2018, doi: https://doi.org/10.1007/s11356-018-3602-x
• 13. Silver, M., Selke, S., Balsaa, P., Wefer-Roehl, A., Kübeck, C., Schüth, C. Fate of five pharmaceuticals under different infiltration conditions for managed aquifer recharge. Science of The Total Environment, 642, 914-924, 2018, doi:https://doi.org/10.1016/j.scitotenv.2018.06.120
• 14. Patrolecco, L., Capri, S., Ademollo, N. Occurrence of selected pharmaceuticals in the principal sewage treatment plants in Rome (Italy) and in the receiving surface waters. Environmental Science and Pollution Research, 22(8), 5864-5876, 2015, doi: https://doi.org/10.1007/s11356-014-3765-z
• 15. Erdem, H., Erdem, M. Synthesis and characterization of a novel activated carbon–supported cobalt catalyst from biomass mixture for tetracycline degradation via persulfate activation. Biomass Conversion and Biorefinery, 12, 3513–3524, 2022, doi: https://doi.org/10.1007/s13399-020-00963-z
• 16. Erdem, H. Aktif karbon destekli heterojen katalitik sistemlerde sülfat radikalleriyle farmasötik grubu bazı organik kirleticilerin kimyasal oksidasyonu. 2020.
• 17. Wang, B., Li, Y.-n., Wang, L. Metal-free activation of persulfates by corn stalk biochar for the degradation of antibiotic norfloxacin: Activation factors and degradation mechanism. Chemosphere, 237, 124454, 2019, doi:https://doi.org/10.1016/j.chemosphere.2019.124454
• 18. Li, Z., Wang, M., Jin, C., Kang, J., Liu, J., Yang, H., Zhang, Y., Pu, Q., Zhao, Y., You, M., Wu, Z. Synthesis of novel Co3O4 hierarchical porous nanosheets via corn stem and MOF-Co templates for efficient oxytetracycline degradation by peroxymonosulfate activation. Chemical Engineering Journal, 392, 123789, 2020, doi:https://doi.org/10.1016/j.cej.2019.123789
• 19. Song, T., Gao, Y., Li, G., Chen, Y., Li, Q. The Kinetic Simulation of Persulfate Activation by Nano-Ferrosoferric Oxide. Catalysts, 2022, doi: https://doi.org/10.3390/catal12111353
• 20. Xu, M., Li, J., Yan, Y., Zhao, X., Yan, J., Zhang, Y., Lai, B., Chen, X., Song, L. Catalytic degradation of sulfamethoxazole through peroxymonosulfate activated with expanded graphite loaded CoFe2O4 particles. Chemical Engineering Journal, 369, 403-413, 2019, doi:https://doi.org/10.1016/j.cej.2019.03.075
• 21. Feng, Y., Song, Q., Lv, W., Liu, G. Degradation of ketoprofen by sulfate radical-based advanced oxidation processes: Kinetics, mechanisms, and effects of natural water matrices. Chemosphere, 189, 643-651, 2017, doi:https://doi.org/10.1016/j.chemosphere.2017.09.109
• 22. Wei, L., Li, J., Zhou, C., Song, B., Qin, F., Wang, W., Luo, H., Qin, D., Huang, C., Zhang, C., Yang, Y. Design of copper oxide and oxygen codoped graphitic carbon nitride activator for efficient radical and nonradical activation of peroxymonosulfate. Chinese Chemical Letters, 107893, 2022, doi:https://doi.org/10.1016/j.cclet.2022.107893
• 23. Cai, C., Kang, S., Xie, X., Liao, C. Ultrasound-assisted heterogeneous peroxymonosulfate activation with Co/SBA-15 for the efficient degradation of organic contaminant in water. Journal of Hazardous Materials, 385, 121519-121519, 2020, doi:https://doi.org/10.1016/j.jhazmat.2019.121519
• 24. Gao, Y., Cong, S., Yu, H., Zou, D. Investigation on microwave absorbing properties of 3D C@ZnCo2O4 as a highly active heterogenous catalyst and the degradation of ciprofloxacin by activated persulfate process. Separation and Purification Technology, 262, 118330, 2021, doi:https://doi.org/10.1016/j.seppur.2021.118330
• 25. Wu, X., Gu, X., Lu, S., Qiu, Z., Sui, Q., Zang, X., Miao, Z., Xu, M. Strong enhancement of trichloroethylene degradation in ferrous ion activated persulfate system by promoting ferric and ferrous ion cycles with hydroxylamine. Separation and Purification Technology, 147, 186-193, 2015, doi:https://doi.org/10.1016/j.seppur.2015.04.031
• 26. Li, Z., Sun, Y., Yang, Y., Han, Y., Wang, T., Chen, J., Tsang, D.C.W. Biochar-supported nanoscale zero-valent iron as an efficient catalyst for organic degradation in groundwater. Journal of Hazardous Materials, 383, 121240, 2020, doi:https://doi.org/10.1016/j.jhazmat.2019.121240
• 27. He, M., Wan, Z., Tsang, D.C.W., Sun, Y., Khan, E., Hou, D., Graham, N.J.D.: Performance indicators for a holistic evaluation of catalyst-based degradation—A case study of selected pharmaceuticals and personal care products (PPCPs). Journal of Hazardous Materials, 402, 123460, 2021, doi:https://doi.org/10.1016/j.jhazmat.2020.123460