Degradation of Ciprofloxacin (CIP) Antibiotic Waste using The Advanced Oxidation Process (AOP) Method with Ferrate (VI) from Extreme Base Electrosynthesis
DOI:
https://doi.org/10.48048/tis.2023.6639Keywords:
Ciprofloxacin, Antibiotic waste, Ferrate, Electrosynthesis, Waste degradationAbstract
Ciprofloxacin (CIP) antibiotic liquid waste is the most common waste found in hospital discharge waters. The accumulation of CIP can increase mutation, microbial resistance, and toxicity in the environment due to its low biodegradability and longevity in waters. Thus, methods for eliminating CIP are important. The Advanced Oxidation Process (AOP) method with ferrate (VI) has good redox potential in water disinfection, and degradation of organic and inorganic pollutants. Therefore, this study aims to degrade CIP waste with ferrate (VI). The ferrate (VI) used was synthesized from the electrolysis of transformer scrap metal plates under extremely alkaline conditions. The success of the synthesis was proven by the presence of FeO(OH) groups characterized using FTIR, XRF, and XRD. Then, the effect of time, pH, and CIP degradation was studied. The results showed that the maximum performance was obtained at pH 7 and 120 min with the addition of 1.1 mg ferrate at initial CIP concentration of 30 mg/L. The concentration of CIP decreased with increasing treatment time which was confirmed by UV-Vis Spectrophotometer. This condition is able to degrade 86.7 % of CIP. In addition, the LC-MS results show that degradation occurs due to a reaction between HFeO4-/H2FeO4 and the active site of piperazine ring antibiotics. This shows that Ferrate has a promising potential to reduce ciprofloxacin antibiotic pollution from hospital wastewater for a better environment.
HIGHLIGHTS
- Ciprofloxacin (CIP) antibiotic liquid waste is the most common waste found in hospital discharge waters. It can cause mutation, microbial resistance, and toxicity in the environment due to its low biodegradability and longevity in waters
- The Advanced Oxidation Process (AOP) method with ferrate (VI) has good redox potential in water disinfection, and degradation of organic and inorganic pollutants including antibiotic liquid waste
- Ferrate was able to degrade 86.7 % of ciprofloxacin antibiotic pollution from hospital wastewater through a reaction between HFeO4-/H2FeO4 and the active site of piperazine ring antibiotics
GRAPHICAL ABSTRACT
Downloads
Metrics
References
EY Klein, TPV Boeckel, EM Martinez, S Pant, S Gandra, SA Levin, H Goosens and R Laxminarayan. Global increase and geographic convergence in antibiotic consumption between 2000 and 2015. Proc. Natl. Acad. Sci. 2018; 15, 3463-70.
SI Polianciuc, AE Gurzău, B Kiss, MG Ștefan and F Loghin. Antibiotics in the environment: Causes and consequences. Med. Pharm. Rep. 2020; 3, 231.
P Guerra, M Kim, A Shah, M Alaee and SA Smyt. Occurrence and fate of antibiotic, analgesic/antiinflammatory, and antifungal compounds in five wastewater treatment processes. Sci. Total Environ. 2014; 1, 235-43.
B Nas, T Dolu and S Koyuncu. Behavior and removal of ciprofloxacin and sulfamethoxazole antibiotics in three different types of full-scale wastewater treatment plants: A comparative study. Water Air Soil Pollut. 2021; 4, 1-15.
L Huang, Y Mo, Z Wu, S Rad, X Song, H Zeng, S Bashir, B Kang and Z Chen. Occurrence, distribution, and health risk assessment of quinolone antibiotics in water, sediment, and fish species of Qingshitan reservoir, South China. Sci. Rep. 2020; 1, 1-18.
SW Hyung, J Lee, SY Baek, S Lee, J Han, B Kim, K Choi, S Ahn, DK Lim and H Lee. Method improvement for analysis of enrofloxacin and ciprofloxacin in chicken meat: Application of in-sample addition of trace ethylenediaminetetraacetic acid to isotope dilution ultra-performance liquid chromatography-mass spectrometry. Chromatographia 2022; 1, 35-45.
S Keerthanan, C Jayasinghe, JK Biswas and M Vithanage. Pharmaceutical and personal care products (PPCPs) in the environment: Plant uptake, translocation, bioaccumulation, and human health risks. Crit. Rev. Environ. Sci. Tech. 2021; 12, 1221-58.
IC Stanton, AK Murray, L Zhang, J Snape and WH Gaze. Evolution of antibiotic resistance at low antibiotic concentrations including selection below the minimal selective concentration. Commun. Biol. 2020; 1, 1-11.
LF Zhai, HY Guo, YY Chen, M Sun and S Wang. Structure-dependent degradation of pharmaceuticals and personal care products by electrocatalytic wet air oxidation: A study by computational and experimental approaches. Chem. Eng. J. 2021; 423, 130167.
EWES Shahrin, NAH Narudin, NNM Shahri, M Nur, JW Lim, MR Bilad, AH Mahadi, J Hobley and A Usman. A comparative study of adsorption behavior of rifampicin, streptomycin, and ibuprofen contaminants from aqueous solutions onto chitosan: Dynamic interactions, kinetics, diffusions, and mechanisms. Emerg. Contam. 2023; 9, 100199.
SB Verinda, M Muniroh, E Yulianto, N Maharani, G Gunawan, NF Amalia, J Hobley, A Usman and M Nur. Degradation of ciprofloxacin in aqueous solution using ozone microbubbles: Spectroscopic, kinetics, and antibacterial analysis. Heliyon 2022; 8, e10137.
N Li, J Zhang, Y Tian, J Zhao, J Zhang and W Zuo. Precisely controlled fabrication of magnetic 3D γFe2O3@ZnO core-shell photocatalyst with enhanced activity: Ciprofloxacin degradation and mechanism insight. Chem. Eng. J. 2017, 308, 377-85.
DB Miklos, C Remy, M Jekel, KG Linden, JE Drewes and U Hübner. Evaluation of advanced oxidation processes for water and wastewater treatment - A critical review. Water Res. 2018; 139, 118-31.
K Shang, R Morent, N Wang, Y Wang, B Peng, N Jiang, N Lu and J Li. Degradation of sulfamethoxazole (SMX) by water falling film DBD Plasma/Persulfate: Reactive species identification and their role in SMX degradation. Chem. Eng. J. 2022; 431, 133916.
RC Sanito, SJ You and YF Wang. Degradation of contaminants in plasma technology: An overview. J. Hazard. Mater. 2022; 424, 127390.
EM Cuerda-Correa, MF Alexandre-Franco and C Fernández-González. Advanced oxidation processes for the removal of antibiotics from water: An overview. Water 2019; 1, 102.
B Yang, GG Ying, JL Zhao, S Liu, LJ Zhou and F Chen. Removal of selected endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) during ferrate(VI) treatment of secondary wastewater effluents. Water Res. 2012; 7, 2194-204.
JQ Jiang. Advances in the development and application of ferrate(VI) for water and wastewater treatment. J. Chem. Tech. Biotechnol. 2014; 2, 165-77.
VK Sharma, R Zboril and RS Varma. Ferrates: Greener oxidants with multimodal action in water treatment technologies. Acc. Chem. Res. 2015; 2, 182-91.
Gunawan, NBA Prasetya, A Haris and F Febriliani. Synthesis of ferrate using NaOCl and Fe(OH)3 from electrolysis of used iron, and its application for metanil yellow degradation. J. Phys. Conf. Ser. 2021; 1943, 012181.
Gunawan, NBA Prasetya and RA Wijaya. Electrochemical synthesis of ferrate (FeO42–) in extreme alkaline medium and its application in dye degradation. Asian J. Chem. 2022; 34, 3361-68
G Gunawan, NBA Prasetya, A Haris and E Pratista. Ferrate synthesis using NaOCl and its application for dye removal. Open Chem. 2022; 20, 1142-54.
G Gunawan, A Haris, NBA Prasetya, E Pratista and A Amrullah. Ferrate(VI) synthesis using Fe(OH)3 from waste iron electrolysis and its application for the removal of metal ions and anions in water. Indones. J. Chem. 2021; 34, 3361-8.
W Gan, VK Sharma, X Zhang, L Yang and X Yang. Investigation of disinfection byproducts formation in ferrate(VI) pre-oxidation of NOM and its model compounds followed by chlorination. J. Hazard. Mater. 2015; 292, 197-204.
Y Jiang, JE Goodwill, JE Tobiason and DA Reckhow. Impacts of ferrate oxidation on natural organic matter and disinfection by product precursors. Water Res. 2016; 96, 114-25.
JQ Jiang, and B Lloyd. Progress in the development and use of ferrate (VI) salt as an oxidant and coagulant for water and wastewater treatment. Water Res. 2002; 6, 1397-408.
ZY Zhang, D Ji, W Mao, Y Cui, Q Wang, L Han and T Li. Dry chemistry of ferrate (VI): A solvent‐free mechanochemical way for versatile green oxidation. Angew. Chem. Int. Ed. 2018; 34, 10949-53.
Y Chen, Q Jin and Z Tang. Degradation of ofloxacin by potassium ferrate: Kinetics and degradation pathways. Environ. Sci. Pollut. Res. 2022; 29, 44504-12.
B Jebalbarezi, R Dehghanzadeh, S Sheikhi, N Shahmahdi, H Aslani and A Maryamabadi. Oxidative degradation of sulfamethoxazole from secondary treated effluent by ferrate (VI): Kinetics, by-products, degradation pathway and toxicity assessment. J. Environ. Health Sci. Eng. 2022; 1, 205-18.
Q Jin, D Ji, Y Chen, Z Tang and Y Fu. Kinetics and pathway of levofloxacin degradation by ferrate (VI) and reaction mechanism of catalytic degradation by copper sulfide. Sep. Purif. Tech. 2022; 282, 120104.
M Feng, X Wang, J Chen, R Qu, Y Sui, L Cizmas, Z Wang and VK Sharma. Degradation of fluoroquinolone antibiotics by ferrate(VI): Effects of water constituents and oxidized products. Water Res. 2016; 103, 48-57.
D Wang, Z Zeng, H Zhang, J Zhang and R Bai. How does pH influence ferrate(VI) oxidation of fluoroquinolone antibiotics? Chem. Eng. J. 2022; 431, 133381.
C Sarangapani, Y Dixit, V Milosavljevic, C Sullivan, P Bourke and P Cullen. Optimization of Atmospheric air plasma for degradation of organic dyes in wastewater. Water Sci. Tech. 2017; 75, 207-19.
A El Maghraoui, A Zerouale, M Ijjaali, M Sajieddine, M ben Abdellah and M Fes. Synthesis and characterization of Ferrate(VI) alkali metal by electrochemical method. Adv. Mater. Phys. Chem. 2013; 1, 83-7.
L Macera, G Taglieri, V Daniele, M Passacantando and F D’orazio. Nano-Sized Fe(III) Oxide Particles Starting from an Innovative and Eco-Friendly Synthesis Method. Nanomaterials 2020; 2, 323.
BS Zhu, Y Jia, Z Jin, B Sun, T Luo, LT Kong and JH Liu. A facile precipitation synthesis of mesoporous 2-line ferrihydrite with good fluoride removal properties. RSC Adv. 2015; 103, 84389-97.
MG Peleyeju, EH Umukoro, L Tshwenya, R Moutloali, JO Babalola and OA Arotiba. Photoelectrocatalytic water treatment systems: Degradation, kinetics and intermediate products studies of sulfamethoxazole on a TiO2-exfoliated graphite electrode. RSC Adv. 2017; 7, 40571-80.
S Bashir, RW McCabe, C Boxall, MS Leaver, and D Mobbs. Synthesis of α- and β-FeOOH iron oxide nanoparticles in non-ionic surfactant medium. J. Nanopart. Res. 2009; 3, 701-6.
B Yuan, J Xu, X Li and ML Fu. Preparation of Si-Al/α-FeOOH catalyst from an iron-containing waste and surface-catalytic oxidation of methylene blue at neutral pH value in the presence of H2O2. Chem. Eng. J. 2013; 226, 181-8.
A Munyengabe, C Zvinowanda, J Ramontja and JN Zvimba. Effective desalination of acid mine drainage using an advanced oxidation process: Sodium ferrate (VI) salt. Water 2021; 19, 2619.
A El Maghraoui, A Zerouale and M Ijjaali. Effect of degree of ClO‾ hypochlorite on the wet synthesis of ferrate (VI). Adv. Mater. Phys. Chem. 2015; 5, 133-9.
D Kowalczuk, M Miazga-Karska, A Gładysz, P Warda, A Barańska and B Drop. Characterization of ciprofloxacin-bismuth-loaded antibacterial wound dressing. Molecules 2020; 21, 5096.
A Woziwodzka, M Krychowiak-Maśnicka, G Gołuński, A Łosiewska, A Borowik, D Wyrzykowski and J Piosik. New life of an old drug: Caffeine as a modulator of antibacterial activity of commonly used antibiotics. Pharmaceuticals 2022; 7, 872.
F Eldin, O Suliman and SM Sultan. Sequential injection technique employed for stoichiometric studies, optimization and quantitative determination of some fluoroquinolone antibiotics complexed with iron (III) in sulfuric acid media. Talanta 1996; 4, 559-68.
K Basavaiah, P Nagegowda, BC Somashekar and V Ramakrishna. Spectrophotometric and titrimetric determination of ciprofloxacin based on reaction with cerium (IV) sulphate. ScienceAsia 2006; 4, 403-9.
MH Abdel‐Hay, EM Hassan, AA Gazy and TS Belal. Kinetic spectrophotometric analysis and spectrofluorimetric analysis of ciprofloxacin hydrochloride and norfloxacin in pharmaceutical preparations using 4‐chloro‐7‐nitrobenzo‐2‐oxa‐1, 3‐diazole (NBD‐Cl). J. Chin. Chem. Soc. 2008; 4, 818.
M Rizk, F Belal, F Ibrahim, S Ahmed and ZA Sheribah. Derivative spectrophotometric analysis of 4- quinolone antibacterials in formulations and spiked biological fluids by their Cu(II) complexes. J. AOAC Int. 2001; 2, 368-75.
M Thakur, S Pandey, A Mewada, V Patil, M Khade, E Goshi, and M Sharon. Antibiotic Conjugated Fluorescent Carbon Dots as a Theranostic Agent for Controlled Drug Release, Bioimaging, and Enhanced Antimicrobial Activity. J. Drug Deliv. 2014; 2014, 282193.
EA Serna-Galvis, F Ferraro, J Silva-Agredo and RA Torres-Palma. Degradation of highly consumed fluoroquinolones, penicillins and cephalosporins in distilled water and simulated hospital wastewater by UV254 and UV254/persulfate processes. Water Res. 2017; 122, 128-38.
T Ahamad, M Naushad and SM Alshehri. Analysis of degradation pathways and intermediates products for ciprofloxacin using a highly porous photocatalyst. Chem. Eng. J. 2021; 417, 127969.
J Deng, G Wu, S Yuan, X Zhan, W Wang and ZH Hu. Ciprofloxacin degradation in UV/chlorine advanced oxidation process: Influencing factors, mechanisms and degradation pathways. J. Photochem. Photobiol. A Chem. 2019; 371, 151-8.
HG Guo, NY Gao, WH Chu, L Li, YJ Zhang, JS Gu, and YL Gu. Photochemical degradation of ciprofloxacin in UV and UV/H2O2 process: Kinetics, parameters, and products. Environ. Sci. Pollut. Res. 2013; 5, 3202-13.
MER Jalil, M Baschini and K Sapag. Influence of pH and antibiotic solubility on the removal of ciprofloxacin from aqueous media using montmorillonite. Appl. Clay Sci. 2015; 114, 69-76.
M Zupančič, I Arčon, P Bukovec and A Kodre. A physico-chemical study of the interaction of cobalt (II) ion with ciprofloxacin. Croat. Chem. Acta 2002; 1, 1-12.
TA Gad-Allah, MEM Ali, and MI Badawy. Photocatalytic oxidation of ciprofloxacin under simulated sunlight. J. Hazard. Mater. 2011; 1, 751-5.
JC Durán-Álvarez. Synthesis and Characterization of the All Solid Z-Scheme Bi2WO6/Ag/AgBr for the photocatalytic degradation of ciprofloxacin in water. Top Catal. 2019; 12-16, 1011-25.
AS Giri and AK Golder. Ciprofloxacin degradation from aqueous solution by Fenton oxidation: Reaction kinetics and degradation mechanisms. RSC Adv. 2014; 13, 6738-45.
R Wajahat, A Yasar, AM Khan, AB Tabinda and SG Bhatti. Ozonation and Photo-Driven Oxidation of Ciprofloxacin in Pharmaceutical Wastewater: Degradation kinetics and energy requirements. Pol. J. Environ. Stud. 2019; 3, 1933-8.
S Badal, YF Her and LJ Maher. Nonantibiotic effects of fluoroquinolones in mammalian cells. J. Biol. Chem. 2015; 290, 22287-97.
CA Aggelopoulos, M Hatzisymeon, D Tataraki and G Rassias. Remediation of ciprofloxacin-contaminated soil by nanosecond pulsed dielectric barrier discharge plasma: Influencing factors and degradation mechanisms. Chem. Eng. J. 2020; 393, 124768.
HG Guo, NY Gao, WH Chu, L Li, YJ Zhang, JS Gu and YL Gu. Photo-chemical Degradation of Ciprofloxacin in UV and UV/H2O2 Process: Kinetics, Parameters, and Products. Environ. Sci. Pollut. Res. 2013; 5, 3202-13.
W Karl, J Schneider and HG Wetzstein. Outlines of an exploding network of metabolites generated from the fluoroquinolone enrofloxacin by the brown rot fungus gloeophyllum striatum. Appl. Microbiol. Biotechnol. 2006; 1, 101-13.
AS Giri and AK Golder. Ciprofloxacin degradation from aqueous solution by fen-ton oxidation: reaction kinetics and degradation mechanisms. RSC Adv. 2014; 13, 6738-45.
CL Amorim, IS Moreira, AS Maia, ME Tiri-tan and PM Castro. Biodegradation of ofloxacin, norfloxacin, and ciprofloxacin as single and mixed substrates by Labrys portucalensis F11. Appl. Microbiol. Biotechnol. 2014; 7, 3181-90.
VS Antonin, MC Santos, S Garcia-Segura and E Brillas. Electrochemical incineration of the antibiotic ciprofloxacin in sulfate medium and synthetic urine matrix. Water Res. 2015; 83, 31-41.
GE Ukpo, MA Owolabi, NOA Imaga, OO Oribayo and AJ Ejiroghene. Effect of Carica papaya (Linn) aqueous leaf extract on pharmacokinetic profile of ciprofloxacin in rabbits. Trop. J. Pharm. Res. 2017; 1, 127-34.
Downloads
Published
How to Cite
Issue
Section
License
Copyright (c) 2023 Walailak University
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.
