Removal of metronidazole from simulated wastewater using Fe/C catalyst with a combination of heterogenous Fenton and ozonation

https://doi.org/10.22146/jrekpros.75633

Budi Satria Panandita(1), Imam Prasetyo(2), Teguh Ariyanto(3*)

(1) Department of Chemical Engineering, Faculty of Engineering, Universitas Gadjah Mada, 55281 Yogyakarta, Indonesia
(2) Department of Chemical Engineering, Faculty of Engineering, Universitas Gadjah Mada, 55281 Yogyakarta, Indonesia
(3) Department of Chemical Engineering, Faculty of Engineering, Universitas Gadjah Mada, 55281 Yogyakarta, Indonesia
(*) Corresponding Author

Abstract


This study examined roles of iron oxide/porous carbon material (Fe/C) for removing metronidazole in simulated wastewater by adsorption and then followed by a degradation using advanced oxidation process (H2O2, O3 and combination of H2O2/O3). Fe/C was produced by an impregnation of iron oxide precursors during resorcinol-formaldehyde synthesis followed by pyrolysis at 800 °C. For comparison, blank carbon (without iron loading) was also synthesized. The properties of porous carbon were investigated by SEM-EDX and N2-sorption analyzer. Blank carbon and Fe/C featured the specific surface area of 755 m2g-1 and 394 m2g-1, respectively. The loading of iron oxide altered the pore structures of material. The adsorption isotherm data were followed by the Langmuir isotherm model with metronidazole uptake up to 46.07 mg g-1 and 39.97 mg g-1 at 30oC by Fe/C and blank carbon. The degradation study was then carried out with catalyst dosage of 0.1 g/100 mL solution and 120 min reaction time at 30 oC. It is noticeably that, the degradation of metronidazole was better when a combination of H2O2/O3 was employed, compared with an individual of H2O2 or O3. Regarding the stability, Fe/C maintained its high activity upon four consecutive runs.


Keywords


Advanced oxidation, iron oxide, metronidazole, porous carbon

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References

Amelia S, Sediawan WB, Prasetyo I, Munoz M, Ariyanto T. 2020. Role of the pore structure of Fe/C catalysts on heterogeneous Fenton oxidation. Journal of Environmental Chemical Engineering. 8(1):102921. doi:10.1016/j.jece.201 9.102921.

Ariyanto T, Kurniasari M, Laksmana WT, Rochmadi, Prasetyo I. 2019. Pore size control of polymer-derived carbon adsorbent and its application for dye removal. International Journal of Environmental Science and Technology. 16(8):4631–4636. doi:10.1007/s13762-018-2166-0.

Asgharzadeh F, Gholami M, Jafari AJ, Kermani M, Asgharnia H, Kalantary RR. 2020. Heterogeneous photocatalyticdegradation of metronidazole from aqueous solutions using Fe3O4/TiO2 supported on biochar. Desalination and Water Treatment. 175:304–315. doi:10.5004/dwt.20 20.24789.

Balarak D, Khatibi AD, Chandrika K. 2020. Antibiotics removal from aqueous solution and pharmaceutical wastewater by adsorption process : A review. 10(2):106–111. doi:10.5 530/ijpi.2020.2.19.

Carrales-Alvarado DH, Ocampo-Pérez R, Leyva-Ramos R, Rivera-Utrilla J. 2014. Removal of the antibiotic metronidazole by adsorption on various carbon materials from aqueous phase. Journal of Colloid and Interface Science. 436:276–285. doi:10.1016/j.jcis.2014.08.023.

Costanzo SD, Murby J, Bates J. 2005. Ecosystem response to antibiotics entering the aquatic environment. 51:218– 223. doi:10.1016/j.marpolbul.2004.10.038.

Cuerda-Correa EM, Alexandre-Franco MF, FernándezGonzález C. 2020. Advanced oxidation processes for the removal of antibiotics from water. An overview. Water (Switzerland). 12(1). doi:10.3390/w12010102.

Escher BI, Baumgartner R, Koller M, Treyer K, Lienert J, Mcardell CS. 2010. Environmental toxicology and risk assessment of pharmaceuticals from hospital wastewater. Water Research. 45(1):75–92. doi:10.1016/j.watres.2010. 08.019.

Gadipelly C, Pérez-González A, Yadav GD, Ortiz I, Ibáñez R, Rathod VK, Marathe KV. 2014. Pharmaceutical industry wastewater: Review of the technologies for water treatment and reuse. Industrial and Engineering Chemistry Research. 53(29):11571–11592. doi:10.1021/ie501210j.

Goolsby TA, Jakeman B, Gaynes RP. 2018. Clinical relevance of metronidazole and peripheral neuropathy: a systematic review of the literature. International Journal of Antimicrobial Agents. 51(3):319–325. doi:10.1016/j.ijantimicag. 2017.08.033.

He J, Yang X, Men B, Wang D. 2016. Interfacial mechanisms of heterogeneous Fenton reactions catalyzed by iron-based materials: A review. Journal of Environmental Sciences (China). 39:97–109. doi:10.1016/j.jes.2015.12.003.

Ighalo JO, Igwegbe CA, Adeniyi AG, Adeyanju CA, Ogunniyi S, Ighalo JO, Igwegbe CA, Adeniyi AG. 2020. Mitigation of Metronidazole ( Flagyl ) pollution in aqueous media by adsorption : a review. doi:10.1080/21622515.2020.1849409.

Issaka E, AMU-Darko JNO, Yakubu S, Fapohunda FO, Ali N, Bilal M. 2022. Advanced catalytic ozonation for degradation of pharmaceutical pollutants―A review. Chemosphere. 289(December 2021). doi:10.1016/j.chemosphere.2021.1

33208.

Johnson MB, Mehrvar M. 2008. Kinetics , catalysis , and reaction engineering aqueous metronidazole degradation by UV / H2O2 process in single-and multi-lamp tubular photoreactors : jinetics and reactor design:6525–6537. doi: 10.1021/ie071637v.

Malakootian M, Kannan K, Gharaghani MA, Dehdarirad A, Nasiri A, Shahamat YD, Mahdizadeh H. 2019. Removal of metronidazole from wastewater by Fe/charcoal micro electrolysis fluidized bed reactor. Journal of Environmental Chemical Engineering. 7(6):103457. doi:10.1016/ j.jece.2019.103457.

Mirzaei A, Chen Z, Haghighat F, Yerushalmi L. 2017. Removal of pharmaceuticals from water by homo/heterogonous Fenton-type processes – A review. Chemosphere. 174:665–688. doi:10.1016/j.chemosphere.2017.02.019.

Mohd Zawawi N, Hamzah F, Veny H, Mohd Rodhi MN, Sarif M. 2021. Chemical and electrochemical properties of bamboo activated carbon activate using potassium hydroxide assisted by microwave-ultrasonic irradiation. ASEAN Journal of Chemical Engineering. 21(2):211–224. doi:10.2 2146/ajche.64617.

Munoz M, Mora FJ, de Pedro ZM, Alvarez-Torrellas S, Casas JA, Rodriguez JJ. 2017. Application of CWPO to the treatment of pharmaceutical emerging pollutants in different water matrices with a ferromagnetic catalyst. Journal of Hazardous Materials. 331:45–54. doi:10.1016/j.jhazmat.20 17.02.017.

Nasseh N, Arghavan FS, Rodriguez-Couto S, Hossein Panahi A, Esmati M, A-Musawi TJ. 2020. Preparation of activated carbon@ZnO composite and its application as a novel catalyst in catalytic ozonation process for metronidazole degradation. Advanced Powder Technology. 31(2):875– 885. doi:10.1016/j.apt.2019.12.006.

Panandita B. 2022. Adsorpsi metronidazol dengan adsorben fexoy/c dan degradasinya dengan fenton heterogen serta ozonasi katalitik. [Master’s thesis]: Universitas Gadjah Mada.

Patel M, Kumar R, Kishor K, Mlsna T, Pittman CU, Mohan D. 2019. Pharmaceuticals of emerging concern in aquatic systems: Chemistry, occurrence, effects, and removal methods. Chemical Reviews. 119(6):3510–3673. doi:10.1 021/acs.chemrev.8b00299.

Prasetyo I, Fajar Mukti NI, Ariyanto T. 2019. Ethylene adsorption using cobalt oxide-loaded polymer-derived nanoporous carbon and its application to extend shelf life of fruit. Molecules. 24(8). doi:10.3390/molecules2 4081507.

Prasetyo I, Rochmadi, Ariyanto T, Yunanto R. 2013. Simple method to produce nanoporous carbon for various applications by pyrolysis of specially synthesized phenolic resin. Indonesian Journal of Chemistry. 13(2):95–100. doi: 10.22146/ijc.21290.

Rajagopal V, Kathiresan M, Manivel P, Suryanarayanan V, Velayutham D, Ho KC. 2020. Porous organic polymer derived metal-free carbon composite as an electrocatalyst for CO2 reduction and water splitting. Journal of the Taiwan Institute of Chemical Engineers. 106:183–190. doi: 10.1016/j.jtice.2019.10.016.

Saffaj T, Charrouf M, Abourriche A, Aboud Y, Bennamara A, Berrada M. 2006. Spectrophotometric determination of Metronidazole and Secnidazole in pharmaceutical preparations based on the formation of dyes. Dyes and Pigments. 70(3):259–262. doi:10.1016/j.dyepig.200 5.01.009.

Seidmohammadi A, Vaziri Y, Dargahi A, Nasab HZ. 2021. Improved degradation of metronidazole in a heterogeneous photo-Fenton oxidation system with PAC/Fe3O4 magnetic catalyst: biodegradability, catalyst specifications, process optimization, and degradation pathway. Biomass Conversion and Biorefinery. (0123456789). doi: 10.1007/s13399-021-01668-7.

Thommes M, Kaneko K, Neimark AV, Olivier JP, RodriguezReinoso F, Rouquerol J, Sing KSW. 2015. Physisorption of gases, with special reference to the evaluation of sur face area and pore size distribution (IUPAC Technical Report). Pure and Applied Chemistry. 87(9-10):1051–1069.



DOI: https://doi.org/10.22146/jrekpros.75633

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