JSEHR 1(1)-4

JSEHR 1(1)-4

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  Investigation of Photo–Fenton–LikeProcess Efficiency in Diazinon Pesti- cide Removal from Aqueous Solutions Leila Kazemizad1 , Yasaman Ghaffari1 , Majid Kermani2* , Mahdi Farzadkia2 , Ayoub Hajizadeh1 , 1 Department of Environmental Health Engineering, School of Public Health, Tehran University of Medical Sciences, Tehran, Iran. 2 Department of Environmental Health Engineering, School of Public Health, Iran University of Medical Sciences, Tehran, Iran. Received 12 October 2016; Revised 10 November 2016; Accepted 24 November 2016; Available online 27 December 2016 ABSTRACT: Diazinon pesticide and its metabolites have been identified in aquatic systems worldwide. It was related to toxicity for aquatic organisms, animals, and humans. Waters contaminated with such persistent insecticides should be treated with suitable treatment processes. In this research, Diazinon removal from aqueous solutions by the photo–Fenton–like process (UV/H2 O2 /Fe0 ) was investigated. This experimen- tal laboratory scale study was performed on synthetic wastewater in a batch system. The reaction was done in the cylindrical UV irradiation photo–reactor with 2.5 L useful volume at 25 ±2 °C. The effects of H2 O2 , pH, ZVI, retention time and initial Diazinon concentration on removal efficiency were studied. The results showed that the optimal parameters for this process were as follows: [Fe0 ]/[H2 O2 ] molar ratio of 1:1, pH 4, the reaction time of 30 min, and initial concentration of 10 mg/L. Diazinon removal and COD reduction in this condition were achieved 83.05% and 71.34%, respectively. Photo–Fenton like process can be suggested as a pretreatment step for the biological removal or post treatment of Diazinon and other pesticides with a similar structure in the aqueous environments. Also, considering the high potential of the photo–Fenton– like process in the reaction with pollutants, a modifying pilot system to ensure concurrent proper rotation speed and UV radiation seem to be necessary. KEYWORDS: Diazinon, Photo–Fenton Like Process, AOPs, ZVI, Organophosphate Pesticide Introduction One of the organophosphate pesticides that is vastly used to treat a variety of insects in different regions is Diazinon [1]. Despite Diazinon has low persistence in the environment compare to the organochlorine pesticides, it is a non–specific insecticide and highly toxic to animals and humans. The main toxic action of Diazinon is inhibition of acetylcholinesterase activity [2]. Diazinon (O, O–diethyl O–[2–isopropyl–6–meth- ylpyrimidin–4–yl] thiophosphate) is classified by the World Health Organization as “moderately hazardous” class II. It was related to toxicity for aquatic organisms in the concentration of 350 ng/L, with an LC50 in killifish (48 h) of 4.4 mg/L. Fatal human doses were found to be in the range from 90 to 444 mg/kg. Diazinon is relatively water soluble (40 mg/L at 25 °C), non–polar, moderately mobile and persistent in soil. Hence, it is of concern for groundwater and surface resources derived drinking water [3–5]. Diazinon and its metabolites have been identified in aquatic systems worldwide [4]. Therefore, wa- ters contaminated with such persistent insecticides should be treated with suitable treatment processes [6, 7]. Conventional water treatment processes have no enough efficacy for the degradation and removal of emerging water micro–pollutants including Diazinon [8]. In recent years, dif- ferent methods have been developed and studied for removal of Diazinon such as biodegradation [9], sonochemical degra- dation [10], photodegradation [11], Fenton reagents and its derivatives [12–14], adsorption [15], electrocoagulation [4], and photocatalytic degradation [7]. A number of studies have *Corresponding Author Email: [email protected] Tel.: +98 2186 704 627; Fax: +98 2188 622 707 Note. Discussion period for this manuscript open until January 31, 2017 on JSEHR website at the “Show Article” http://dx.doi.org/10.22053/jsehr.2016.33383 J. Saf. Environ. Health Res. 1(1): 17–22, Autumn 2016 DOI: 10.22053/jsehr.2016.33383 ORIGINAL RESEARCH PAPER indicated the potential for using advanced oxidation process- es (AOPs) to destroy micro–pollutants completely such as pes- ticides. AOPs use combinations of oxidants, catalysts, and ultravio- let irradiation to produce hydroxyl radicals (OH• ) in solutions and have offered interest for the degradation of non–biode- gradable or hazardous organic pollutants in wastewater. The organic compounds are oxidized and mineralized by free rad- icals to carbon dioxide, water, and mineral salts. The Fenton reaction (Fe2+ /H2 O2 ), and Fenton–like reactions (Fe0 /H2 O2 or Fe3+ /H2 O2 ) have been widely applied in the treatment of biore- fractory wastewater in the field of AOPs [13]. The main advan- tage of Fenton processes can be linked to the fact that the re- action occurs at room conditions of temperature and pressure which results a less expensive treatment. furthermore, a short time is necessary for the reaction [16]. However, Fenton sys- tems have two major limitations: (a) more iron sludge produc- tion and (b) slow Fe+3 ions reduction by H2 O2 [13, 17]. Hence, ultraviolet (UV) irradiation is offered for dominance on the system limitations. The use of UV irradiation causes ferric iron (Fe+3 ) that had poor efficiency in Fenton process, returned to activity segment and transformed to ferrous iron ion in which enhance process efficiency. Moreover, UV irradiation affords hydroxyl radicals gain [13]. Thus, Fenton systems plus UV irradiation considering ad- vantages such as favorite health and environmental aspects, high efficiency for various pollutants removal from water and wastewater, and other advantages have a very desirable pros- pect in water and wastewater industries. The presence of high concentrations of chemical, synthetic, and toxic pollutants, which have an inhibitory effect on microorganism’s biologi- cal activity, have made frequent use of these systems in treat- ing industrial wastewater. Although, great studies have been performed heretofore about AOPs application sake pesticides
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  Leila Kazemizad etal. / J. Saf. Environ. Health Res. 1(1): 17–22, Autumn 201618 elimination from aquatic environments; anyone has been paid to evaluate and survey pesticides removal via Fenton–like processes plus UV irradiation especially using zero–valent iron (Fe0 ) in Diazinon removal. Moreover, optimal values of affecting parameters in this process have been implied less. Thus, the objectives of this study were: (a) investigation of photo–Fenton–like (UV/H2 O2 /Fe0 ) process efficiency in Dia- zinon removal from aqueous solutions and (b) optimization of affecting parameters on the process at different concentra- tions of proposed toxin. Materials and methods Materials and equipment In this laboratory experimental study, Diazinon primary matter for preparing different initial concentrations was applied from Merck. Ferrous sulfate (FeSO4 .7H2 O) and zero–valent iron (ZVI) powder for activation of producing OH• ; hydrogen peroxide solution (30% w/w) as oxidant; potassium hydrogen phthalate (KHP), Fe(NH4 )2 (SO4 )2 .6H2 O (FAS), K2 Cr2 O7 , HgSO4 and AgSO4 for COD test; H2 SO4 and NaOH for proper pH adjustment; and sodium thiosulfate for samples maintenance were also purchased from Merck. Methanol as the mobile phase of HPLC (high–performance liquid chromatography) was obtained from Caledon Com- pany. The Diazinon concentrations were measured using a CECIL HPLC with a UV detector (CECIL, England, CE4100 model) and column: C18 (250 mm× 4.6 mm I.D.) and elu- tion process were done using gradient mode. The chemi- cal oxygen demand (COD) was determined by COD reactor HACH DRB200 and CECIL Aquarius spectrophotometer [18]. The pH meter used for pH adjustment was HACH HQ40d model. Photo–reactor characteristic The schematic of photoreactor is shown in Fig. 1. The cy- lindrical UV irradiation photo–reactor with 2.5 L useful volume was made from very slick and smooth steel for maximum rays repercussion inside of the reactor. UV rays were supplied by using low–pressure mercury vapor UV lamp about the power of 55 W (Netherland product). The lamp was put as the central inside of a transparent quartz shield with 3 cm diameter along the reactor. The photore- actor was connected to a storage vessel by 2.5 L volume for sample loading and sampling. A jar test set at 200 rpm was used for mixing. A peristaltic pump was applied for contin- uous flow of reactor contents. The UV lamp and photo–re- actor characteristics used in this research are presented in Table 1. Fig. 1. Schematic of photo–reactor Experimental procedure This experimental laboratory scale study was performed on synthetic wastewater in a batch system. Reaction on the sam- ple was done in the space through UV lamp and steel cover (Fig. 1) at 25 ±2 °C. Degradation of Diazinon during photo– Fenton–like oxidation was performed under experimental conditions including: H2 O2 (in 0.3, 0.6, 1, and 2.5 mM), pH (the values of 4, 5.37, 7, and 10), ZVI (in 0.3, 0.6, 1, and 2.5 mM) and initial Diazinon concentration (in 10, 20, 40, and 50 mg/L). Reaction time was uncertain up to 30 minutes (1, 2, 4, 7, 15, and 30 min). Experiments were done at five discrete steps including determination of optimum values of H2 O2 , pH, ZVI, reaction time, and effect of initial Diazinon concentration on removal efficiency. In each step, the optimum value for con- sidered parameter was determined via poising all variables and changing one variable. Diazinon standard solution with a concentration of 50 mg/L was used at the first because of detecting the maximum concentration of this toxin in environ- mental wastewaters. Final assessment of process was based on evaluating Diazinon ultimate concentration using HPLC set. The samples were taken at selected reaction times and analyzed by HPLC. Diazinon mineralization quantity was also appointed. Table 1. Characteristics of UV lamp and photo–reactor Conclusively, the COD reduction was considered under op- timal conditions (according to 5220B method)[18]. All exper- iments were run in duplicate. After experiments completion, results were analyzed and related diagrams were depicted using Excel software. Results and discussion Effect of H2 O2 The effect of H2 O2 dosage changes on Diazinon removal ef- ficiency is illustrated in Fig. 2. Adequate dosages of H2 O2 extremely affect the reaction rate. As it is obvious, Diazinon removal efficiency firstly enhanced to 76.45% with H2 O2 increasing from 0.3 mM to 0.6 mM at aconstant dose of Fe0 . Then, it reduced with more H2 O2 adding from 0.6 mM to 2.5 mM. The use of H2 O2 mid iron ion results in producing a large number of OH• causes a rapid reduction of organic compounds (Eq.1) [19, 20]. Hence, removal efficiency enhanced at the first, but addi- tional amounts of H2 O2 reacted with produced OH• in the pro- cess (Eq. 2) and redounded upon weaker radicals output that
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  Leila Kazemizad etal. / J. Saf. Environ. Health Res. 1(1): 17–22, Autumn 2016 19 had lower activity rather than OH• [20]. Another reason for the decline in the efficiency of the process can be spontaneous decomposition of H2 O2 to water and oxygen (Eq. 3). Produced O2 trapped in the sludge matrix and led to its flotation [21]. Excess H2 O2 in wastewater causes the COD rise [22]. Fig. 2. Effect of different concentrations of H2 O2 on Diazinon re- moval: [H2 O2 ]= varying, [Fe0 ]= 0.6 mM, pH= 5.37(neutral), reaction time= 30 min, Diazinon: 50 mg/L. The standard deviation of all data samples was below 5. With the above, determination of the optimum value for the maximum economy and efficiency OH• production is im- portant. So, it seems that in this study, the maximum removal efficiency among the four studied concentrations of Diazinon in the process (0.3, 0.6, 1, and 2.5 mM) belonged to the 0.6 mM. Therefore, the optimal value was used in subsequent experiments. Murray and Parsons (2004) demonstrated that organic matter removal efficiency enhanced at a fixed concen- tration of Fe (II) with increasing H2 O2 and then decreased with further increasing the H2 O2 concentration [23]. Also, Wu et al. (2010) believe that this is due to the combination of OH• in- duced proliferation of H2 O2 and addition production of OOH• which is OH• consumer [24]. Effect of pH The effect of pH values in four ranges of acidic, alkaline, neu- tral and natural (values of 4, 7, 10, and 5.37) with an optimal concentration of hydrogen peroxide (0.6 mM) and certain iron concentration (0.6 mM) for Diazinon removal was examined. As shown in Fig. 3, the maximum removal efficiency equaled to 81.46% which was considered at pH= 4. Studies have shown that the best range of pH for the Fenton reaction is 3 to 4 and the process reactions are pH–dependent [25]. Research- es have also shown that pH declining to a value of 2 and lower causes decreasing the process efficiency due to OH+2 forma- tion and consequently Fe+3 and OH• production also decrease [26]. Wu et al. (2010) remarked that the removal efficiency decline at pH= 2 is related to complex species formation that have less reactivity with H2 O2 [24]. At pH= 4, Fe(OH)+ ion is formed which have activity more than Fe+2 in the Fenton pro- cess [27]. Another reason could be that the soluble part of the iron ion and the hydroxyl radical oxidation potential are more at the acidic pH [19] and hydrogen peroxide is also decom- posed easily into hydroxyl radical [27]. Fig. 3. Effect of pH on Diazinon removal: [H2 O2 ]= 0.6 mM, [Fe0 ]= 0.6 mM, pH= varying, reaction time= 30 min, Diazinon: 50 mg/L. The standard deviation of all data samples was below 5. As was observed, removal efficiency decreased with in- creasing pH in the studied concentration of Diazinon. At pH above 4, Fe+3 precipitates as Fe(OH)3 causing decomposition of hydrogen peroxide into water and oxygen [25]. Moreover, H2 O2 in presence of H+ at acidic pH transforms to peroxone ion that affords H2 O2 persistence and prohibits from H2 O2 with iron ions reaction [28]. In this study, pH= 4 was selected as op- timal pH in order to provide a favorite condition for Diazinon removal which is consistent with most studies. Effect of ZVI Given the dominant role of iron in the reaction with hydro- gen peroxide which causes increasing production of OH• , it is very important to determine the optimum dose. Iron ions are as ferrous ion (Fe+2 ), ferric ion (Fe+3 ), and zero–valent iron (Fe0 ) forms. ZVI powder was used in the photo–Fenton–like process. The effect of different concentrations of ZVI on the photo–Fenton–like process in Diazinon removal is specified in Fig. 4. ZVI powder addition to 0.6 mM (33.6 mg/L) increased the toxin removal efficiency to 81.46%. More amounts of ZVI decreased the process efficiency. With increasing the concen- tration of Fe+2 , more OH• produced and removal rate and effi- ciency of various pollutants enhanced. Other studies have also shown that excessive concentrations of iron (Fe+2 ) have been an inhibitory effect on the production of hydroxyl radicals and reduced the rate and efficiency of the chemicals destruction [29]. The use of iron ions with hydrogen peroxide for produc- ing large amounts of OH• and thereby increasing oxidizing po- tential of H2 O2 suddenly decrease the concentration of organic compounds [21]. This causes the removal efficiency firstly enhanced with increasing concentration of the reactants. But with increasing iron concentration (higher than optimal val- ue), the metal ion is combined with OH• and it makes the reac- tion environment [20]. Effect of [Fe0 ]/[H2 O2 ] molar ratio Perusing relationship between changes in Diazinon removal efficiency and changes in [Fe0 ]/[H2 O2 ] molar ratio in the reac- tion showed that increasing the [Fe0 ]/[H2 O2 ] molar ratio from 0.5 to 1 in the process led to increase efficiency and achieve removal efficiency of 83.46%. It is also revealed that increase in the ratio from 1 to 4.17 and higher is conducive to decline efficiency. This means that hydrogen peroxide in higher pro- portion than optimal value had an inhibition role for the pro- duction of hydroxyl radicals and decreased the process effi- ciency [21, 22].
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  Leila Kazemizad etal. / J. Saf. Environ. Health Res. 1(1): 17–22, Autumn 201620 Fig. 4. Effect of different concentrations of ZVI on Diazinon remov- al: [H2 O2 ]= 0.6 mM, [Fe0 ]= varying, pH= 4, reaction time= 30 min, Diazinon: 50 mg/L. The standard deviation of all data samples was below 5. The optimal molar ratio of [Fe0 ]/[H2 O2 ] is important not only in terms of achieving effective degradation of Diazinon but also minimizing chemicals consumption and residuals re- sulting from the completion of the reaction . Hence, in order to achieve higher efficiency in Diazinon removal, according to the molar ratio of [Fe0 ]/[H2 O2 ] in the photo–Fenton–like pro- cess was chosen 1:1. Effect of retention time Diazinon removal rate in various retention times (1, 2, 4, 7, 15, and 30 min) was investigated. Results demonstrated that removal efficiency enhanced with varying retention time from 0 to 30 min. Maximum removal efficiency (83.05%) was achieved at a reaction time of 30 min under optimal condi- tion (Table 2). Also, the maximum removal in all steps was observed after 30 min that was used in the determination of optimum values. It should be noted that short treatment time may need higher chemicals consumption. Moreover, the long treatment time can enhance the reactor volume and construc- tion costs [14]. Considering the results, 30 min was selected as appropriate reaction time in this study. Table 2. Optimal parameters of photo–Fenton–like process for Diaz- inon removal Effect of initial Diazinon concentration Diazinon oxidation procedure by using a photo–Fenton–like process in different initial concentrations of the toxin (10, 20, 40, and 50 mg/L) at the optimal values of the studied vari- ables was performed. The effect of the initial Diazinon con- centration on removal efficiency is presented in Fig. 5. The maximum removal efficiency for the concentration of 10 mg/L using optimized condition was achieved 83.05%. The process efficiency for concentrations of 20, 40, and 50 mg/L were 82.33, 81.62, and 81.46 percent, respectively. Thus, the removal efficiency was declined by increasing the concentra- tion of the toxin. Increase in concentration of the toxin caused a reduction in the reaction rate (Table 3). The reaction rate in the process for the concentration of 10 mg/L (k= 0.533 1/ min) was more than the reaction rate of 50 mg/L (k= 0.097 1/min). Because of increasing concentration of Diazinon, the numbers of pesticide molecules in an aqueous environment enhanced and competition between these molecules on the hydroxyl ions increased [30]. Another cause of declined de- toxification efficiency in higher concentrations in photolysis processes (such as photo–Fenton–like) is that with increas- ing concentrations of toxin, UV photons penetration into the solution becomes less and seek to reduce the influence of the photons. Hence, the decomposition of H2 O2 to OH• is reduced. Thus, whatever the level of toxin concentration increases, penetration of UV photons and subsequently production of hydroxyl radicals and removal efficiency will be reduced [31]. In its decomposition procedure, organic matter creates com- pounds which cause the breakdown of aromatic rings and ef- fectively promote the removal efficiency by H2 O2 over the time [30]. Fig. 5. Effect of different initial concentrations of Diazinon on re- moval efficiency: [H2 O2 ]= 0.6 mM, [Fe0 ]= 0.6, pH= 4, reaction time= 30 min. The standard deviation of all data samples was below 5. Table 3. The reaction rate in different initial concentrations of Dia- zinon (t/Ct changes versus time): [H2 O2 ]= 0.6 mM, [Fe0 ]= 0.6, pH= 4, reaction time= 30 min. Conclusion In this study, degradation of Diazinon by photo–Fenton–like process was investigated and optimal values of affecting pa- rameters on the process were explained. The results showed that this process could successfully degrade Diazinon under optimal conditions (83.05% at 10 mg/L initial concentration, 30 min UV irradiation time, [Fe0 ]/[H2 O2 ] molar ratio of 1:1, and pH4 ). The rate of mineralization was surveyed and 71.34% COD reduction on optimal conditions was observed. Also, Di- azinon removal in the concentration of 50 mg/L that was de- tected as the maximum level of the toxin in the environmental wastewaters was achieved up to 81.46%. Photo–Fenton like process (UV/H2 O2 /Fe0 ) can be suggested as a pretreatment step for the biological removal or post treatment of Diazinon and other pesticides with a similar structure in the aqueous environments. However, due to the influence of other com- pounds in the wastewater of industries producing pesticides, it is recommended that a pilot–scale study on real wastewater from industries that have the problem of toxic effluents dis- charge into the environment be implemented. Also consider-
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  Leila Kazemizad etal. / J. Saf. Environ. Health Res. 1(1): 17–22, Autumn 2016 21 ing the high potential of the photo–Fenton–like process in the reaction with pollutants, modifying the pilot system to ensure concurrent proper rotation speed and UV irradiation seems to be necessary. Acknowledgements This study was part of a M.S. dissertation supported by Tehran University of Medical Sciences (TUMS); (Grant No: 240/3134). References [1] H. Hossaini, G. Moussavi, M. Farrokhi, The investigation of the LED–activated FeFNS–TiO2 nanocatalyst for photocatalytic deg- radation and mineralization of organophosphate pesticides in water, Water research, 59 (2014) 130–144. [2] M. Čolović, D. Krstić, S. Petrović, A. Leskovac, G. Joksić, J. Savić, M. Franko, P. Trebše, V. Vasić, Toxic effects of Diazinon and its photo- degradation products, Toxicology letters, 193 (2010) 9–18. [3] R.R. Kalantary, Y. Dadban Shahamat, M. Farzadkia, A. Esrafili, H. 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  Leila Kazemizad etal. / J. Saf. Environ. Health Res. 1(1): 17–22, Autumn 201622 AUTHOR(S) BIOSKETCHES Kazemizad, L., MSc, Department of Environmental Health Engineering, School of Public Health, Tehran University of Medical Sciences, Tehran, Iran. Email: [email protected] Ghaffari, Y., MSc, Department of Environmental Health Engineering, School of Public Health, Tehran University of Medical Sciences, Tehran, Iran. Email: [email protected] Kermani, M., Ph.D., Associate Professor, Department of Environmental Health Engineering, School of Public Health, Iran University of Medical Sciences, Tehran, Iran. Email: [email protected] Farzadkia, M., Ph.D., Professor, Department of Environmental Health Engineering, School of Public Health, Iran University of Medical Sciences, Tehran, Iran. Email: [email protected] Hajizadeh, A., MSc, Department of Environmental Health Engineering, School of Public Health, Tehran University of Medical Sciences, Tehran, Iran. Email: [email protected] COPYRIGHTS copyright for this article is retained by the author(s), with publication rights granted to the journal. this is an open–access article distributed under the terms and conditions of the Creative Commons Attribiotion Licsense (https://creativecommons.org/licenses/by/4.0/) HOW TO CITE THIS ARTICLE L. Kazemizad, Y. Ghaffari, M. Kermani, M. Farzadkia, A. Hajizadeh, Investigation of Photo-Fenton-Like Process Efficiency in Diaz- inon Pesticide Removal from Aqueous Solutions, Journal of Safety, Environment, and Health Research, (2016) 19-24. DOI: 10.22053/jsehr.2016.33383 URL: http://jsehr.net/article_33383.html