Simultaneous degradation of cephalexin, ciprofloxacin, and clarithromycin from medical laboratory wastewater by electro-Fenton process
Graphical abstract
Introduction
Health care facilities utilize a huge amount of water and generate wastewater including domestic wastes as well as medical and hazardous wastes based on the service provided by the facility [1]. Various laboratory services are provided in health care facilities depending on the class and extent of the establishment. The wastewater produced in these laboratories is rich in antibiotics, diagnostic materials, disinfectants, laboratory chemicals, and micropollutants [2,3]. Traditional treatment applications are usually not sufficient for the degradation of antibiotics present in the wastewater [4]. Therefore, they are released into the environment, which has become an emerging issue in the last decade [5]. The existence of antibiotics in the environment due to their persistence and stability may have toxic effects on human health [6]. Thus, novel technologies should be applied for the effective treatment of wastewaters containing antibiotics.
Numerous treatment techniques including coagulation, flocculation, filtration, sedimentation, adsorption, ultrasonication, and biological processes have been applied for the removal of emerging chemicals from water and wastewater [7]. Nonetheless, alternative methods are needed due to low removal efficiencies and high costs of some of these applications [8]. On the other hand, advanced oxidation processes (AOPs) which are effective to remove recalcitrant pollutants have gained increasing attention in antibiotic removal considering their strong oxidation capability and fast reaction rate [8]. AOPs such as Fenton, ozonation, photocatalytic oxidation, and electrooxidation have been used for the removal of antibiotics from water or wastewater [8,9].
Various types of antibiotics including fluoroquinolones, macrolides, and cephalosporin have been detected in wastewater globally [10]. Among these groups, Ciprofloxacin (CIP) and Clarithromycin (CLA) were implemented in the priority substances list and watch list for water bodies in the Directive 2013/39/EU [11] and Decision 2015/495/EU [12] while Cephalexin (CEX) is one of the most frequently prescribed antibiotics [13]. Biological treatment [14,15], adsorption [[16], [17], [18]], Fenton process [19,20], photochemical degradation [21], membrane biological reactor [22], and sonochemical treatment [23] are among the applied methods for the removal of CIP, CLA, and CEX from aqueous media. Besides, to the best of authors’ knowledge, there were no studies on the removal of CEX, CIP, and CLA by the EF process from hospital wastewater or wastewater from health care facilities. Thus, there is a need for researches considering alternative treatment methods including EF for antibiotic removal from such kind of wastewater.
The traditional approach for the optimization of process variables is performing the experiments by changing one parameter at each time. However, this causes a loss of materials, time, and human labor. Thus, using a statistical tool such as response surface methodology (RSM) has gain importance since it provides the optimization of process variables with a minimum number of experiments. RSM has been applied for the optimization of process variables in antibiotic removal from various wastewaters [[24], [25], [26], [27]]. Besides, it was applied for the optimization of CEX removal by sono-Fenton [28] and CIP removal by the EF [29] from synthetic water. However, there is a lack of a study on the removal and process optimization of CEX, CIP, and CLA from real medical laboratory wastewater by the EF process.
The electro-Fenton (EF) process, which is a combination of electrocoagulation, and traditional Fenton process is an effective oxidation method, especially in high strength wastewaters. During the EF process, Fe2+ ions are provided from sacrificial iron anodes [30,31] and more OH· radicals are generated which provides an advantage of both electrocoagulation and Fenton processes [[30], [31], [32], [33], [34]]. EF has been used for the degradation of various antibiotics in water [[35], [36], [37], [38]]. On the other hand, there were only a few studies concerning the removal of CEX [39], CIP [[40], [41], [42]], and CLA [43] by electro-Fenton or Fenton based treatments. The encountered studies were conducted by synthetic water and to the best of authors’ knowledge; there were no studies on CEX, CIP, and CLA removal from hospital wastewater or such a kind of wastewater by the EF process. The present study is among the first attempts to remove CEX, CIP, and CLA from medical laboratory wastewater by the EF process. The EF process becomes prominent in terms of ease of application, high pollutant removal efficiency, and comparatively moderate cost at optimized conditions. The present study will provide an insight into the usage of the EF process for the removal of CEX and CLA as well as contribute to the limited researches on CIP removal by the EF process. In this study, removal of Cephalexin, Ciprofloxacin, and Clarithromycin from medical laboratory wastewater by the electro-Fenton process was investigated. This study provides both the application of the EF process for CEX, CIP and CLA removal in wastewater with high toxic strength and optimization of process parameters. The process variables were optimized with central composite design and the optimum conditions for antibiotics removal by the electro-Fenton process were determined.
Section snippets
Wastewater characterization
The wastewater used in this study was taken from a medical laboratory's wastewater tank in İstanbul, Turkey. The medical laboratory serves 11 different health care facilities. Approximately 4−5 m3 day−1 of wastewater is generated in the laboratory which is collected in a 25 m3 capacity tank and no domestic wastewater is mixed in this wastewater tank. The wastewater used in the present study was taken when the volume of wastewater in the tank was about 10 m3, which represents a composite sample
Results and discussion
The suitability of the experimental data to the polynomial model representing Cephalexin, Ciprofloxacin, and Clarithromycin removal efficiencies (%) (response Y) as a function of pH, current, reaction time, and H2O2/COD ratio were analyzed using the Statgraphics Centurion XVI.I software and the model equations are given below.
Conclusions
In this study, wastewater occurring in a medical laboratory serving 11 different health care facilities was treated with the EF process. The removal performance of antibiotics was evaluated and process parameters were optimized applying central composite design. The optimized process variables were pH 2.99, current 3.93 A, reaction time 35.3 min, and H2O2/COD ratio 1.09. Among the linear parameters, the H2O2/COD ratio has the highest effect on CEX, CIP, and CLA removal by the EF process. The
CRediT authorship contribution statement
Irfan Basturk: Methodology, Validation, Investigation. Gamze Varank: Conceptualization, Investigation, Methodology, Supervision, Writing - original draft. Selda Murat-Hocaoglu: Conceptualization, Investigation, Methodology, Supervision. Senem Yazici-Guvenc: Software, Formal analysis, Visualization. Emine Can-Güven: Investigation, Writing - original draft. Elmas Eva Oktem-Olgun: Methodology, Validation. Oltan Canli: Methodology, Validation.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This research was supported by the Ministry of Environment and Urbanization with the project entitled “Treatment and Management of Liquid Wastes and Wastewater from Healthcare Facilities” and by Yildiz Technical University-The Scientific Research Projects Coordinatorshipwith the research project number of FDK-2018-3426.
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2023, Inorganic Chemistry CommunicationsCitation Excerpt :Various methods have been investigated for the removal of CFX. For the specific case of CFX, technologies such as adsorption [5], biological technique [6], membrane separation [7], electro-Fenton oxidation [8,9], and photocatalytic degradation [10] have been commonly used. Gashtasbi et al., synthesized an activated carbon-impregnated magnetite composite and used it for the removal of CFX from an aqueous solution via the UV system [11].