Degradation of Cefixime Antibiotic by Heterogeneous Catalytic Ozonation Process using novel LDH/zeolite nano-composite:Modeling and Optimization Process

Degradation of Cefixime Antibiotic by Heterogeneous Catalytic Ozonation Process using novel LDH/zeolite nano-composite:Modeling and Optimization Process | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Degradation of Cefixime Antibiotic by Heterogeneous Catalytic Ozonation Process using novel LDH/zeolite nano-composite:Modeling and Optimization Process Yalda Sheikh, Elham Tazikeh-Lemeski, Yousef Dadban Shahamat, Mohammad Taghi Baei, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4388377/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 27 May, 2025 Read the published version in Journal of Environmental Health Science and Engineering → Version 1 posted 4 You are reading this latest preprint version Abstract In recent decades, the indiscriminate use of antibiotics and their discharge into the environment have caused serious consequences for aquatic and terrestrial organisms. In the present study, the optimization of cefixime antibiotic decomposition by a powerful catalytic ozonation process has been investigated. In this study, MgAl-LDH /zeolite nanocomposite was synthesized and use as an ozonation-adsorption catalyst for the degradation of Cefixime antibiotic from aqueous solution. XRD, FE-SEM, and FTIR analyzes were scrutinized to reveal the main characteristics of the as-prepared nanocomposite, showing that it was well-synthesized. The investigated variables in the catalytic ozonation of Cefixime by the mentioned nanocomposite included solution pH level (5–9), nanocatalyst dose (0.5–2.5 g/L), Cefixime concentration (5–25 mg/L) and reaction time (5–60 min) which they were optimized by adopting RSM-CCD. The results showred that all variables had a positive effect on the efficiency of the catalytic ozonation process. Nonetheless, the lowest effect of operational factor pH, the degradation of Cefixime was subjected to the initial content of Cefixime in this treatment system. The optimal conditions for cefixime removal by catalytic ozonation process were determined at pH of 7.72, nanocatalyst dosage of 1 g/L, cefixime concentration of 23 mg/L, and reaction time of 55 min. In the optimized operating conditions, the removal efficiency of Cefixime by MgAl-LDH /zeolite nanocomposite was high up to 98.37%. Cefixime LDH Nanocomposites Ozonation Wastewater Zeolite Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Introduction Recently, emerging pollutants, such as synthetic organic chemicals, have been large identified in the natural environment. These substances are considered a new group of micropollutant compounds that have harmful effects on human health and ecology [ 1 ]. Also, these unknown substances have been frequently diagnosed in diverse effluents from urban sludge, daily household products, drug production units, hospital wastewater, sanitary landfills, and aquatic environments. It had been noted that the concentration of emerging pollutants was in the range of ng/L-mg/L. The large identified concentration of such compounds in water medium can potentially cause microbial large present in pharmaceutical organic pollutants, personal care products (PCPs), endocrine-disrupting compounds (EDCs), surfactants, insecticides, and industrial additives [ 2 ]. Among medicinal compounds, antibiotics are highly prescribed and consumed in the medical field. These drugs are still a hot topic about worldwide environmental health because creating resistance to bacterial species [ 3 ]. The consumption of antibiotics is pointed to be between 200000 − 100000 tons per year worldwide. These compounds are considered dangerous substances for the environment as they show varied genetic behaviors bringing substantial changes in different ecosystems. Over the last decades, various antibiotic residues have been recognized in surface water, underground water, and sewage treatment plants [ 4 , 5 ]. The identification of these compounds in water mediums are mainly subjected to complex chemical structure, polarity, low volatility, hydrophilic, high stability, and antimicrobial properties in aquatic environments [ 6 ]. Antibiotics are divided into several categories—penicillin, cephalosporin, tetracycline, aminoglycosides, fluoroquinolones, macrolides, and sulfonamides. Among them, cephalosporins are classified into three generations [ 7 ]. Cefixime is one of the third-generation cephalosporins group, which is used in the treatment of infectious diseases under the brand name Suprax [ 8 ]. Cefixime is a semi-synthetic antibiotic, Cefixime is the first member of the third-generation cephalosporin class use for oral administration, a wide range of Gram-negative bacteria, and some Gram-positive aerobic bacteria [ 9 ]. This antibiotic effectively applied against various bacterial organisms and infections, including staphylococcus, hemophilic influenza, Escherichia coli, streptococcus fever, tonsillitis, and throat infections [ 10 ]. Cefixime is one of the most widely used antibiotics, with e half-life of around 3 and 4 hr, which is longer than other cephalosporins classes. The threshold risk level of Cefixime in water sources as an organic pollutant is 5 µg/L [ 11 ]. The enforcing Environmental laws and public health concerns have resulted in all institutions. The organizations should purify their wastewater before discharging their effluents into surface water or reusing based on the current environmental health standards [ 12 ]. Since the concentration of antibiotics in surface water, underground water, sewage, and drinking water has been detected in ng/L to µg/L, an advanced system is needed to remove these compounds from aqueous environments. Therefore, conventional water and wastewater treatment processes cannot analyze and remove these compounds [ 3 ]. Thus, various technologies have been applied to remove pharmaceutical compounds from wastewater, such as adsorption with activated carbon, reverse osmosis, stripping with air, and biologic methods. The mentioned procedures not only do not remove the pollutant but also transfer it from one phase to another [ 13 ]. In the last decade, the application of advanced oxidation processes (AOPs) has been expanded to reduce the pollution caused by pharmaceutical residues in water. These processes are based on the formation of active hydroxyl radicals (˙OH) that react with organic substances to eradicate their structures [ 14 ]. The typical AOPs in the purification of drugs include photolysis, catalytic ozonation, Fenton oxidation, heterogeneous photocatalyst, electrochemical oxidation, ultrasonic radiation, and wet air oxidation. Depending on the characteristics of wastewater under treatment, AOP S processes can be used alone or with other physical, chemical, and biologic processes [ 15 – 18 ]. Oxidation is a method used in recent years to decompose non-biodegradable pollutants. In oxidation reactions, electrons are transferred from an oxidizing substance to another substance [ 19 ]. Ozone is one of the strong oxidants that directly and indirectly oxidize and decomposes the target pollutant. In the direct mechanism, the ozone molecule directly reacts with the aimed pollutant, and in indirect ozonation, the ozone molecule is decomposed and converted into hydroxyl radicals [ 14 ]. Then, the hydroxyl radical reacts with the pollutant and eradicates it. However, ozone has limitations such as low oxidation rate, high energy consumption, and pollutant selectivity [ 20 , 21 ]. One of the advanced oxidation processes is the catalytic ozonation process (COP). Adding a catalyst to the ozonation process leads to an increase in the amount of oxidation, a decrease in reaction time and production of toxic and by-products, and consequently an increase in usability as a complete treatment process or cheap pre-treatment [ 22 ]. The catalytic ozonation process can be used in both homogeneous and heterogeneous ways. Among these two methods, the heterogeneous catalytic ozonation process is suitable for wastewater treatment due to its low cost, the potential to regenerate the catalyst, and not cause secondary pollution. Some of the frequent catalysts proposed and used in this method are metal oxides (TiO 2 , MnO 2 , Al 2 O 3 , etc.), reinforced metals, or metal oxides such as CuTiO 2 , CU/Al 2 O 3 , Fe 2 O 3 /Al 2 O 3 , TiO 2 /Al 2 O 3 , Co/SiO 2 , Ru/CeO 2 [ 19 , 23 ]. Recently, another interesting catalyst has been layered double hydroxides (LDH), part of the family of synthetic and natural clay compounds. These minerals have a two-dimensional and layered structure consisting of positively charged cationic hydroxide layers with interlayers containing anions and water, such as clay minerals. Many divalent ions such as nickel, cobalt, copper, and zinc can create different forms of LDH with trivalent ions such as aluminum, chromium, iron, and gallium and produce large structural compounds. The mineral form of LDH of calcium with aluminum is known as hydrocalumite, and LDH of magnesium with aluminum is known as hydrotalcite (double-layer hydroxide). In general, the formula of LDHs is expressed as [M 2 + 1−x M 3 + x (OH) 2 ] (A n− ) x/n .mH 2 O, where M 2+ and M 3+ are divalent and trivalent cations, respectively. Also, A n− represents the interlayer anions, and x is equal to the molar ratio of M 3+ / (M 2+ + M 3+ ). The layered structure, active interlayer space, high anion exchange, chemical and physical stability, and colloidal properties are prominent features of this nanocatalyst, causing much attention among advanced oxidation processes [ 24 , 25 ]. The simultaneous application of adsorbent catalysts along with oxidation is called the adsorption-catalyst process (ACP). ACP processes are one of the AOP processes in which adsorption and reaction on the porous catalyst surface coincide [ 25 ]. In ACP processes, porous materials are used, showing a dual function as adsorbents and catalysts in ozonation. These catalysts are different from non-porous catalysts that are usually used in ozonation processes as metal oxides or natural minerals. Among the porous adsorbents used are zeolite and activated carbon. One of the most common and cheapest natural zeolites is Clinoptilolite, whose features include environmental compatibility, heat resistance (up to 800 ℃), and oxidation by ozone [ 26 ]. In the present study, the optimization of cefixime antibiotic decomposition by a powerful catalytic ozonation process with MgAl-layered double hydroxide nanocomposite placed on clinoptilolite zeolite (MgAl-LDH) under different conditions has been investigated, with RSM-CCD method. According to the authors' review, no study has been conducted on using ACP process with natural zeolite as a porous adsorbent. Material and methods Materials Cefixime antibiotic powder used in this study was 98% pure (provided from Sigma Aldrich Company). Some characteristics of this antibiotic are shown in Table 1 [ 27 , 28 ]. The H 2 SO 4 and NaOH solutions (1%) were consumed to adjust the pH level. Also, the ozone output from the reactor was decomposed in an impinger containing KI with a concentration of 20%. Other chemicals used in this study include MgCl 2 (H 2 O) 6 , AlCl 3 (H 2 O) 6 , Na 2 SO 3 , KH 2 PO 4 , Na 2 SO 3 , Na 2 SO 3, CH 3 OH, H 3 PO 4 and HCl. All chemicals were obtained from Merck, Germany. Table 1 Some characteristics of Cefixime medicine name Cefixime Structure Molecular formula C 6 H 15 N 5 O 7 S 2 Group Third-generation cephalosporin Molecular Weight (g/mol) 453.452 λmax 290 nm Dissolvability Low Color light yellow Average half-life 3–4 hours pK a1 (COOH group of cefixime nucleus) 2.1 pK a2 (aminothiazole group) 2.92 pK a3 (chain-COOH group) 3.45 Table 1 Some characteristics of Cefixime MgAl-LDH synthesis coated on Zeolite The MgAL-LDH Nanocatalyst was synthesized by co-precipitation method at room temperature [ 29 ]. To prepare LDH coated on Zeolite, the 50 ml of 4 M sodium hydroxide was dropped wisely poured into an Erlenmeyer flask containing 50 ml of a solution containing 10.165 g of magnesium chloride hexahydrate and 9.63 g of aluminum chloride hexahydrate and 10 g of zeolite powder with constant magnetic stirring. After finishing the NaOH, it was sonicated for 30 minutes by BANDELIN machine (Bandelin Company, SONOREX DIGITEC model, made in Germany) with power of 165 W and 30 Hz frequency. Then, the suspension was located in the autoclave tank (Reyhan teb, RT-2 model, Made in Iran) and placed in the oven (FINE TECH Company, SHINSAENG model, made in Korea) at a temperature of 180 ℃ for 24 hr. After the completed the determination time, it was washed 5 times with double distilled water. Finally, it was dried in the oven at 60 ℃ within a day. The physical and structural characteristics of the obtained catalyst were determined by an X-Ray scattering device (PHILIPS Company, PW1730 model, made in the Netherlands). Also, to determine the crystal structure of the catalyst, the size of the catalyst was examined by electron microscopy (FESEM-EDAX; TESCAN mira3, Czech Republic). Moreover, the functional groups of the as-synthesized nanocomposite were investigated through infrared spectroscopy and FTIR (Thermo Company, AVATAR model, made in USA). pH ZPC analysis was performed to determine the surface charge of MgAl-LDH nanocatalyst. The procedure for the determination of the pH ZPC of catalyst To determine the state of electric charge dispersion on the surface of the synthesized catalyst, the value of pH pzc was measured [ 19 ]. This parameter of catalysts is an index to evaluate and interpret the mechanism of the catalytic ozonation process. NaCl solution (0.01 M), hydrochloric acid (0.1 M), and soda (0.1 M) were used to determine pHpzc. In this process, 30 mL of NaCl electrolyte solution in distilled water was poured into 6 Erlenmeyer flasks with a volume of 50 mL. The pH of the solutions was adjusted in the range of 2 to 12 using the acid mentioned above and base chemicals. Then 1 g of catalyst was added to each flask and placed on a shaker at 200 rpm for 48 hr. After passing the mentioned time, the final pH of the filtered solution was measured with a pH meter (HACH Company, Sension156 model, made in USA). Eventually, the value of pHpzc was calculated by drawing the curve of pH changes against the initial pH. Synthetic wastewater The wastewater used in the reactor contained different concentrations of Cefixime, which was prepared synthetically. For this purpose, a standard solution of 1000 ppm antibiotic was prepared by dissolving 1 g of laboratory-grade antibiotic in 1 L of water. Other desired concentrations were prepared from this solution. Apparatus and Analytical Procedures An ozone generator made in Iran with a 6 g/hr nominal capacity was used to supply ozone. The ozone flow rate was set to 1.5 L/min by the rotameter installed at the end of the reactor so that the ozone concentration entering the reactor was about 35 mgL − 1 min − 1 using the iodometric titration method [ 30 ]. The measurement of the residual concentration of cefixime antibiotic was performed by a high-performance liquid chromatography device (HPLC, Waters 1525 made in USA) equipped with a UV absorption detector at a wavelength of 290 nm and a C18 column (Restek company, 5-mm particle size, 250 d 4.6 mm). The mobile phase consisted of methanol and 25 mM phosphate buffer 40:60% (v/v) and orthophosphoric acid to adjust the pH to 5.5, with a wavelength of 290 nm and a flow rate of 1.2 mL/min. The reactor used in this process was a Plexiglas cylinder with a diameter of 5 cm and a height of 1 m (Fig. 1 ), and the reactor system was designed as a semi-batch. Ozone gas was injected into the effluent through the air stone at the reactor's bottom. Figure 1 . Schematic of catalytic ozonation reactor for cefixime degradation In each experimental run, 200 ml of synthetic wastewater containing a specific concentration of Cefixime was transferred to the reactor and subjected to the ACP process. The nanocatalyst used along with ozone consisted of MgAl-layered double hydroxide (MgAl-LDH), which was placed on a zeolite substrate. The parameters of this study included pH (9 − 5), nanocomposite concentration (0.5–25 g/L), cefixime initial concentration (5–25 mg/L), and reaction time (5–60 min). Experiment design This work investigated the removal of the Cefixime antibiotic by MgAl-LDH catalyst. The variables used in the current study were 4, which respectively include the initial concentration of cefixime (5–25) mg/L, the contact time (5–60) min, the pH (5–9), and the adsorbent dosage (0.5–2.5) g/L. This study was based on employing the RSM method (response surface method) and the Central Composite Design (CCD) test design using design expert version 11.0.3.0 software. The test design table, relevant variables, and results are presented in Table 2 . Paying attention to Table 2 , variable A is the initial concentration range, variable B is the pH range, C is the amount of catalyst, and D is the contact time. The response variable shows the removal efficiency. Also, the predicted removal values ​​are given in the last column of Table 2 . The coefficients using Analysis of Variance (ANOVA) were analyzed, and p-value ≥ 0.05 was determined as a significant level. Table 2 The scope of the investigated variables in the design of the Catalytic ozonation process Main independent variables Unit symbol level of variables -α -1 0 + 1 +α pH - B 5 6 7 8 9 Dose of catalyst g/L C 0.5 1 1.5 2 2.5 Reaction time min D 5 18.75 32.5 46.25 60 Cefixime concentration mg/L A 5 10 15 20 25 Table 2 The scope of the investigated variables in the design of the Catalytic ozonation process The CCD-RSM method uses variance analysis and response surface regression analysis to determine the fit of the test results with the multivariate quadratic model as follows: $$\text{Y}= {\text{a}}_{0}+\sum _{\text{i}=1}^{\text{k}}{\text{a}}_{\text{i} }{\text{x}}_{\text{i}}+ \sum _{\text{i}=1}^{\text{k}}{\text{a}}_{\text{i}\text{i} }{\text{x}}_{\text{i}}^{2} + \sum _{\text{i}\ne 1}^{\text{n}}{\text{a}}_{\text{i}\text{j}}{\text{x}}_{\text{i}}{\text{x}}_{\text{j}}+{\epsilon } \left(1\right)$$ Where y is assigned to the predicted removal efficiency (percentage), a 0 is the constant coefficient, a i , a ii , a ij are the estimated coefficients for the main, quadratic, and reciprocal effects, respectively, and xi and x j are the input variables in actual values. n, specifies the number of input variables, and e is assigned to the model error [ 31 ]. The CCD method, according to the prediction model, can exhibit the impacts of operating variables on the performance of the cefixime antibiotic removal process. The variables were optimized to achieve the maximum removal efficiency of Cefixime based on the desired performance in the CCD method. The runs determined by the software are shown in Table 3 . Table 3 The 4-factor CCD matrix with actual factor levels for Cefixime removal based on RSM method Std A:C 0 B:pH C:Catalyst dosage D:Time reaction Y:Cefixime degradation efficiency Actual Value Predicted Value mg/L g/L min (%) (%) 1 10 6 1 18.75 75.00 75.33 2 20 6 1 18.75 82.00 82.1 3 10 8 1 18.75 80.00 80.42 4 20 8 1 18.75 84.00 84.05 5 10 6 2 18.75 83.00 82.94 6 20 6 2 18.75 87.45 88.07 7 10 8 2 18.75 91.00 90.89 8 20 8 2 18.75 93.10 92.88 9 10 6 1 46.25 92.00 92.18 10 20 6 1 46.25 97.00 97.19 11 10 8 1 46.25 93.70 93.15 12 20 8 1 46.25 95.00 95.03 13 10 6 2 46.25 93.00 93.02 14 20 6 2 46.25 96.85 96.39 15 10 8 2 46.25 97.00 96.86 16 20 8 2 46.25 97.35 97.09 17 5 7 1.5 32.5 89.00 88.98 18 25 7 1.5 32.5 96.00 95.99 19 15 5 1.5 32.5 87.00 86.56 20 15 9 1.5 32.5 91.93 92.34 21 15 7 0.5 32.5 85.00 84.65 22 15 7 2.5 32.5 94.00 94.32 23 15 7 1.5 5 78.00 77.45 24 15 7 1.5 60 98.00 98.51 25 15 7 1.5 32.5 91.47 91.9 26 15 7 1.5 32.5 92.07 91.9 27 15 7 1.5 32.5 91.80 91.9 28 15 7 1.5 32.5 92.20 91.9 29 15 7 1.5 32.5 91.93 91.9 30 15 7 1.5 32.5 91.93 91.9 31 15 7 1.5 32.5 91.90 91.9 32 15 7 1.5 32.5 91.95 91.9 33 15 7 1.5 32.5 91.93 91.9 34 15 7 1.5 32.5 91.93 91.9 35 15 7 1.5 32.5 91.89 91.9 36 15 7 1.5 32.5 91.83 91.9 Results and discussion Nano-composite properties X-ray diffraction (XRD) This analysis is done to scrutinize the crystallinity or crystal size. The diffraction pattern of the samples is shown in Fig. 2 . The samples were obtained using a diffractometer of 40 kV and 30 mA at a diffraction angle between 5 and 70°C at room temperature with a radiation source (Cu-α = 1.54). Scherer equation Eq. 2 ., was computed to estimate the crystallite size [ 32 ]: $$d= \frac{K\lambda }{\beta COS \theta }$$ 2 In the above equation, d is the crystal size, λ is the X-ray wavelength, β is the peak width (width at half maximum value (FWHM), θ is the Bragg angle, and K is Scherer's constant (equal to 0.9). According to the crystal structure data of Clinoptilolite in JCPDS (instrument library number 1349-0025-00), the observed pattern of the clinoptilolite zeolite sample demonstrates characteristic peaks at 9.85°, 11.18°, 17.3° and 19.1°, 22.34°, 22.7°, 25°, 26.04°, 28.15°, 30°, and 32°, which is consistent with the results reported by other researchers [ 33 , 34 , 35 ]. The spectrum of zeolite-LDH revealed characteristic diffractions for zeolite is lower intensity with specific shifted, which could be due to overlap with LDH peaks. Also, some other peaks at 45.6°, 56.6°, and 66.5° were also observed in zeolite-LDH with higher intensity, indicating a higher degree of crystallization for LDH crystals [ 36 ]. Therefore, the XRD (TESCAN Company, Mira3, Czech Republic) pattern of zeolite-LDH shows that peaks related to zeolite and LDH, which demonstrate the successful and effective growth of LDH crystals on zeolite components. By Scherer's equation, the crystallite size of zeolite and zeolite-LDH was estimated to be around 11 nm and 20 nm, respectively. Figure 2 XRD pattern of as-synthesized MgAl-LDH nanocomposite Scanning electron microscope (FE-SEM) As shown in Fig. 3 (a), the synthesized catalyst has a uniform and layered structure with specific nanometer dimensions. As a result, this indicates the proper synthesis conditions. Figure 3 a) Electron Microscopy Analysis (SEM) (200KX, 5KX); b) Energy-dispersive X-ray spectroscopy (EDS) Spectrum analysis of MgAl-LDH nanocomposite Figure 3 (b) shows the Weight and atomic percentage of the elements toward the synthesized catalyst. Additionally, element mapping analysis by element including O, Na, Mg, Al, Si, Cl, K, and color and overall composition of elements can be seen in Fig. 3 . Infrared spectroscopic analysis (FTIR) Fourier transform infrared (FTIR) spectroscopic analysis was used to present the chemical structure of the functional groups of zeolite (Zeo) and zeolite modified with layered double hydroxide (Zeo-LDH). The FTIR spectra of the above samples in the range of 400 to 4000 cm − 1 are presented in Fig. 4 . Regarding the spectrum of zeolite (Clinoptilolite), the vibrations around 1600–3700 cm − 1 can be attributed to the water absorbed by the zeolite. For example, The peak at 3622 cm − 1 is related to the interaction of the hydroxyl of water with cations, and the other bands are attributed to the hydrogen bond of the water molecule to the surface oxygen (3451 cm − 1 ) and the bending vibration mode of water (1635 cm − 1 ). The peak at 1067cm − 1 is responsible for the asymmetric stretching vibrations of the T-O bonds in the TO4 tetrahedron (T equals Si and Al). Furthermore, peaks at 796 and 469 cm − 1 can be observed, which are respectively assigned to the stretching vibrations of the O-T-O groups and the bending stretching of the T-O bonds, these results are similar to the results obtained by other authors [ 37 , 38 ]. The functional groups observed for the zeolite-LDH spectrum were analogous to the zeolite spectrum, which were slightly different only in the detection frequency and wavelength of the functional groups. Compared to zeolite, zeolite-LDH showed a broad peak at 3477 cm − 1 , corresponding to the formation of hydrogen bonds in the stretching bands of hydroxyl groups and H 2 O from the surface and interlayer [ 39 , 40 ]. The spectrum of zeolite-LDH has a weak absorption peak due to the absorption of CO 3 2− at 1384 cm − 1 , this finding is consistent with the study of other researcher[ 39 ]. Figure 4 FTIR spectrum of zeolite and zeolite-LDH Development of regression model In the current work, the efficiency of the catalytic ozonation process with MgAl-LDH nanocomposite based on zeolite in the removal of cefixime antibiotic using CCD to optimize four variables was investigated, and the findings are shown in Table 3 . Table 3 The 4-factor CCD matrix with actual factor levels for Cefixime removal based on RSM method The compatibility of Linear, 2FI, Quadratic, and Cubic models related to the obtained experimental results was investigated (Table 4 ). Based on the value of Adjusted R² , the proposed model was Quadratic model with 0.99 R². The value of Predicted R² for this model was equal to 0.98, which is in good agreement with Adjusted R² as the difference between them is less than 0.2. Table 4 The results of investigating cefixime removal models by RSM-CCD method Source Sequential p-value Lack of Fit P-value Adjusted R² Predicted R² Linear < 0.0001 < 0.0001 0.8481 0.8029 2FI 0.0004 < 0.0001 0.9243 0.8943 Quadratic < 0.0001 0.0007 0.9955 0.9859 Suggested Cubic < 0.0001 0.7658 0.9991 0.9975 Aliased Table 4 The results of investigating cefixime removal models by RSM-CCD method According to the results, for all the investigated parameters, the p-value is less than 0.0001, and all 4 variables are significant. means that the studied model can describe the catalyst's investigation of cefixime antibiotic removal. The F-value for the variables indicates the most significant effect of the reaction time variable on the efficiency of cefixime decomposition by the process. .Based on the results of analysis of Variance from Table 5 , the selected model was significant. The variables of pH, catalyst dose, cefixime initial concentration and contact time had a significant effect on the reaction rate. Using the response-level statistical method, the predicted model of the quadratic type and the coded relationship below Eq. 3. expresses the empirical relationship between the test experiences and the removal efficiency. Table 5 The results of analysis of variance of the quadratic model of cefixime antibiotic removal Source Sum of Squares df Mean Square F-value p-value Model 1071.13 14 76.51 556.15 < 0.0001 significant A-C 0 73.68 1 73.68 535.55 < 0.0001 B-pH 50.22 1 50.22 365.04 < 0.0001 C-Catalyst 140.41 1 140.41 1020.64 < 0.0001 D-time 665.18 1 665.18 4835.24 < 0.0001 AB 9.84 1 9.84 71.56 < 0.0001 AC 2.68 1 2.68 19.49 0.0002 AD 3.11 1 3.11 22.58 0.0001 BC 8.19 1 8.19 59.56 < 0.0001 BD 16.91 1 16.91 122.94 < 0.0001 CD 45.73 1 45.73 332.42 < 0.0001 A² 0.6712 1 0.6712 4.88 0.0384 B² 12.04 1 12.04 87.55 < 0.0001 C² 11.72 1 11.72 85.19 < 0.0001 D² 30.74 1 30.74 223.48 < 0.0001 Residual 2.89 21 0.1376 Lack of Fit 2.56 10 0.2562 8.61 0.0007 significant Pure Error 0.3273 11 0.0298 Cor Total 1074.02 35 Cefixime removal (%)= -20.11081 + 1.72867A + 12.67199B + 12.52913C + 1.70827D-0.156875 AB-0.163750 AC-0.006409 AD + 1.43125 BC-0.074773 BD-0.245909 CD + 0.005793A 2 -0.613507B 2 -2.42069C 2 -0.005184D 2 (3) Table 5 The results of analysis of variance of the quadratic model of cefixime antibiotic removal Figure 5 (a) Correlation between predicted vs. actual values, (b) Normal plot of residuals values In Fig. 5 . (a), the relationship between the predicted and actual values is plotted against each other, and the placement of points near the common line indicates the appropriate results from the experiments. Moreover, in Fig. 5 (b), the Normal plot of residuals values obtained from the experiments which indicates the normality of the data and the Predictive model expresses a quantitative amount, exhibiting the appropriate accuracy of the results. The influence of operational variables on Degredation efficiency The initial pH of the solution is a main parameter affecting the catalytic ozonation process [ 30 ]. Therefore, the effect of initial pH on the removal efficiency of Cefixime by catalytic ozonation process with LDH nanocatalyst is scrutinized and is shown in 3D response surfaces in the central point values of other parameters in Fig. 6 . What is more, the graph of pH changes to determine the pHzpc of the catalyst surface is observed in Fig. 7 . Figure 6 . The contours of 3D for cefixime removal by catalytic ozonation process with MgAl-LDH nanocatalyst; Catalyst dosage 1.5 g/L, C 0 _cefexime: 15mg/L, pH 7 and reaction time 32.5 min. According to the findings, increasing the pH level from 5 to 9 improves the removal efficiency from 70 to 90%. Altering the pH of the solution affects the amounts of dissolved ions, the properties of the catalyst surface, and the rate of ionization of the compounds. These changes can be related to the pH ZPC of the catalyst surface and the pKa of the target pollutant. The results of mass titration of acid and base of MgAl-LDH catalyst in Fig .7. show the value of pHzpc equal to 8.7. MgAl-LDH nanocatalyst was determined to be 8.7 by the solid addition method. At pH > pH ZPC , the catalyst surface is negatively charged, while at pH < pH ZPC is positively charged, at pH ≈ pH ZPC is neutral. Since the pKa for Cefixime has been recorded to be 3.73, at higher pH levels, cefixime molecules are ionized as negative ions in solution [ 41 , 42 ]. Thus, the influence of pH on catalytic ozonation can be attributed to the electrostatic interaction between the surface of nanoparticles and target pollutants. On the other hand, as mentioned in the introduction section, the mechanism of oxidation by ozone is direct and indirect. The ozone molecule directly oxidizes the target pollutant in acidic pH through selectivity reactions. Consequently, this restriction prevents the oxidation of all pollutants [ 43 , 44 ]. However, indirect oxidation occurs at alkaline pH, leading to ozone decomposed and powerful hydroxyl radicals being produced, which in the presence of MgAl-LDH nanocatalyst, improves ozone molecule decomposition and hydroxyl radical production [ 42 ]. Unlike the ozone molecule, hydroxyl radicals act non-selectively in addition to their higher destructive power. In this regard, other studies also reached similar results [ 27 , 43 , 45 , 46 ]. Figure 7 The graph of pH variation to determine the pHzpc of the catalyst surface The catalyst dose used in the process is one of the effective factors in increasing the efficiency of cefixime pollutant degradation. As can be seen in the 2D and 3D contours, with the increase of the catalyst dose from 0.5 to 2.5 gr, the cefixime removal efficiency has increased from less than 50% to about 90%. In general, based on other literature, the following mechanisms are suggested for the degradation of cefixime antibiotic by ACP process with MgAl-LDH nanocatalyst supported on zeolite: (a) Adsorption of ozone molecules on zeolite and LDH, its decomposition into active radicals, and then the destruction of Cefixime by these active radicals (b) Cefixime molecules adsorbed on the surface of zeolite, and LDH are decomposed and destroyed by ozone molecules and hydroxyl radicals produced. (c) Ozone and cefixime molecules are simultaneously adsorbed on the surface of zeolite and LDH and react [ 29 , 47 ]. In overall, ozone destruction and hydroxyl radical production during the ACP process are according to (4–10) reactions [ 46 ]: M n+ + O 3 + H + → M (n+1)+ + HOֺ + O 2 (4) O 3 + HOֺ → O 2 + HO. − 2 (5) M (n+1)+ + HO. − 2 + HO − → M n+ + H 2 O + O 2 (6) Mn + + HOֺ → M (n+1)+ + HO − (7) Mn + + O 3 → M (n+1)+ + O. − 3 (8) O. − 3 + H+ → HOֺ 3 (9) HOֺ 3 + O 2 → HOֺ (10) In these reactions, M represents cations such as Al and Mg, and n represents the charge of the ion. As mentioned, LDH nanoparticles have a layered and 2D structure, and these layers include positively charged cationic hydroxides and layers containing anions and water. Since Al 3+ and Mg 2+ cations are placed in the center of the octahedral structure of LDH and hydroxyls are placed at the edges, the water molecules adsorbed on these surfaces are ionized to OH − and H + ions and form surface hydroxyl groups, which result in ozone reacts with these molecules and produces hydroxyl radicals, and finally, these radicals destroy the Cefixime adsorbed in the pores of the MgAl-LDH nanocatalyst placed on the zeolite base, which has an adsorption-catalytic effect[ 46 ]. Therefore, increasing the dose of the catalyst can lead to an increase in the removal efficiency of Cefixime. To date, MgAl-LDH nanocomposite has been used as a catalyst in several studies, and similar results have been obtained. Pourfaraj et al. (2017) investigated the efficiency of MgAl-LDH nanoplates for absorbing Brilliant Yellow dye from aqueous medium. The results of this study indicate an increase in the efficiency of the absorption process by increasing the dose of MgAl-LDH nanoplates, which indicates the direct effect of the nanocomposite dose on the pollutant absorption capacity [ 24 ]. In another study, the decomposition of p-nitroaniline by catalytic ozonation process with MgAl-LDH nanocatalyst has been tested, and the results obtained regarding the catalyst dosage are in line with the results of the present study. In fact, with the increase in the dose of this nanocomposite, the production of OHֺ radicals increased, which leads to an increase in the rate of decomposition of the target pollutant [ 46 ]. The initial concentration range of Cefixime was considered to be 5–25 mg/L by studying other similar literature, and its effect on the efficiency of the catalytic ozonation process was investigated. The results are shown in 2D and 3D response surface plots (Fig. 6 ). The results showed that in this range of Cefixime concentration, with increased Cefixime concentration, its removal efficiency also increased. Increasing the concentration of the target pollutant leads to the enhancement in the catalyst dosage and reaction time. According to the result of the modeling analysis (Fig. 7 ) and the effect of the reaction on the pH of the sample, we see a different removal percentage of the cefixime drug from the samples. In general, the effect of the initial concentration is smaller than the contact time and the catalyst dose. The application of MgAl-LDH nanoparticles based on zeolite along with ozone molecules, in addition to the role of a catalyst and the production of hydroxyl radicals, has also improved the absorption capacity, which in the mentioned concentration range of Cefixime, increasing the initial concentration did not have an inhibitory effect on the efficiency of the process [ 48 ]. Meanwhile, regarding other AOPS studies to remove Cefixime, different results have been obtained. including the study of Salimi et al. (2019), in which the photocatalytic decomposition of Cefixime with MIL125ML/g CN-20 nanocomposite has been investigated, and according to the results, it has been reported that by increasing the initial concentration of Cefixime from 15 to 25 mg/L, the degradation rate of the target contaminant has been declined because of covering the nanocomposite with intermediate molecules and reducing the absorption of light by the nanocomposite [ 9 ]. In another study, cefixime degradation was done by photocatalytic ozonation process with N-TiO 2 /graphene oxide/titanium nanosheets at concentrations of 5–20 mg/L by Sheydaei et al. The results show that with increasing the initial concentration of Cefixime, the reaction rate constant has decreased, and the reason for that is the limitation in the number of active sites of the nanocomposite, which are saturated by absorbing a certain concentration of Cefixime [ 49 ]. The treatment of wastewater containing diazinon pesticide was conducted by catalytic ozone process with MgAl-LDH nanoparticles. The achieved results are similar to the current. However, in the present study, modification of this nanocomposite with zeolite base and ACP process did not decrease the removal efficiency of higher concentrations, which is one of the strengths of this process [ 43 ]. According to the analysis of variance and the contact time of the cefixime reaction and the catalytic ozonation process that took place in the time range of 5–60 min, it shows that the contact time has the most important effect among the variables and we see an increase in the removal efficiency of Cefixime up to 98%. Optimization According to the results of the model and using the optimization part of the Design Expert software, the optimal conditions of the process were determined. For the antibiotic Cefixime, the optimal removal conditions by the catalyst were determined at a pH of 7.72, an adsorbent dose of 0.997g/L, with a reaction time of 55.23 min and an initial concentration of 22.8 mg/L. The presence of toxic compounds in the environment creates potential hazards for aquatic and terrestrial organisms, and the provision of healthy water is a necessity for the continuation of life. sample in this study was real, the results can be used directly in wastewater treatment produced in the poison manufacturing industry and similar industries. Conclusion This study investigated the efficiency of the catalytic ozonation process using MgAl-LDH nanoparticles to cefixime elimination from aqueous solutions. The synthesized MgAl-LDH nanocomposite supported on zeolite was proved to be a potential catalyst for degrading Cefixime by the catalytic ozonation process. In this process, the effect of parameters of initial pH, cefixime concentration, catalyst dose, and contact time for cefixime removal was evaluated. In the optimal conditions obtained by the CCD method for the COP process, the removal efficiency of Cefixime at pH of 7.72, nanocatalyst dosage of 0.997 g/L, cefixime concentration of 22.8 mg/L, and reaction time of 55.23 min was stood at 98.37%. The presence of MgAl-LDH nanocatalyst placed on zeolite with ozone, in addition to absorbing the target pollutant, absorbs and decomposes the ozone molecule and produces hydroxyl radicals. The production of more hydroxyl radicals leads to an increase in the removal efficiency of Cefixime. Therefore, the use of this process is suggested for wastewater containing antibiotics. Declarations Acknowledgements This research is a part of the doctoral thesis titled " Investigating the removal of cefixime by Catalytic Ozonation in the presence of LDH nano composite placed on a Zeolite substrate by the central composite design(CCD) method ". Thanks are hereby given to the support of Islamic Azad University of Gorgan branch and Golestan University of Medical Sciences for conducting this research. Authors’ contributions Conceptualization: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Data curation: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Formal analysis: Yalda Sheikh. Funding acquisition: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Investigation: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Methodology: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Project administration: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Resources: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Software: Yalda Sheikh. Supervision: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Validation: Mohammad Taghi Baei, Hamidreza Jaliliane Visualization: Elham Tazikeh-Lemeski , Yousef Dadban-Shahamat. Writing–original draft: Yalda Sheikh. 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Preparation of nano N-TiO 2 /graphene oxide/titan grid sheets for visible light assisted photocatalytic ozonation of cefixime. J Chem Eng. 2018;353:138–46. Supplementary Files graphicalabs.jpg Cite Share Download PDF Status: Published Journal Publication published 27 May, 2025 Read the published version in Journal of Environmental Health Science and Engineering → Version 1 posted Reviewers agreed at journal 07 Jun, 2024 Reviewers invited by journal 07 Jun, 2024 Editor assigned by journal 08 May, 2024 First submitted to journal 08 May, 2024 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4388377","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":311631774,"identity":"4cfd4f05-dad1-4195-9e00-99801130e87a","order_by":0,"name":"Yalda Sheikh","email":"","orcid":"","institution":"Islamic Azad University Gorgan Branch","correspondingAuthor":false,"prefix":"","firstName":"Yalda","middleName":"","lastName":"Sheikh","suffix":""},{"id":311631775,"identity":"e60b2849-0621-4b8f-a098-701e68b95651","order_by":1,"name":"Elham Tazikeh-Lemeski","email":"","orcid":"","institution":"Islamic Azad University Gorgan Branch","correspondingAuthor":false,"prefix":"","firstName":"Elham","middleName":"","lastName":"Tazikeh-Lemeski","suffix":""},{"id":311631776,"identity":"6d47cce3-2b9b-4ab7-8749-5841117c03c4","order_by":2,"name":"Yousef Dadban Shahamat","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA8ElEQVRIiWNgGAWjYDCCA0DMw8CcwMDAfAAhmkCcFjYkdURq4TEgzl18tw+wSbypsc7jn93z+cXHtm32DOyHHzA83INbi+S5BDbJOcfSiyXunN1mObPtdmIDT5oBQ8Iz3FoMzjCwSfOwHU5suJG7zZi37TbQhTlAvxwgpOXf4cT5N3KegbTYM/C/IUILb9vhxA03cpgfA7UwNkgQsEXyDGOz5dy+9GLDG2lmjDPO3U5sk3hmcACfFr4zzAdvvPlmnSd3I/nxhw9lt+35+ZMfPvyBRwsDA2MDjMUmASYZIJFFFGD+QKzKUTAKRsEoGFkAABWZVZL9+RhVAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0002-6040-0562","institution":"Golestan University of Medical Sciences and Health Services","correspondingAuthor":true,"prefix":"","firstName":"Yousef","middleName":"Dadban","lastName":"Shahamat","suffix":""},{"id":311631777,"identity":"fccfafd4-40d7-4996-8db4-f27b46270888","order_by":3,"name":"Mohammad Taghi Baei","email":"","orcid":"","institution":"Islamic Azad University Azadshahr Branch","correspondingAuthor":false,"prefix":"","firstName":"Mohammad","middleName":"Taghi","lastName":"Baei","suffix":""},{"id":311631778,"identity":"7f5dfd40-803c-40c4-a6d3-cbd8247ead36","order_by":4,"name":"Hamidreza Jalilian","email":"","orcid":"","institution":"Islamic Azad University Gorgan Branch","correspondingAuthor":false,"prefix":"","firstName":"Hamidreza","middleName":"","lastName":"Jalilian","suffix":""}],"badges":[],"createdAt":"2024-05-08 10:05:30","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4388377/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4388377/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s40201-025-00941-5","type":"published","date":"2025-05-27T15:57:50+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":58836590,"identity":"93b9c241-0275-47b3-8d8e-d7cb9dc1c53b","added_by":"auto","created_at":"2024-06-21 20:04:43","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":15746,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic of catalytic ozonation reactor for cefixime degradation\u003c/p\u003e","description":"","filename":"Picture1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/26a1e75c84ad75c6affd6813.jpg"},{"id":58836589,"identity":"7383b048-f56f-4e87-a00b-03035e2e411f","added_by":"auto","created_at":"2024-06-21 20:04:43","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":89926,"visible":true,"origin":"","legend":"\u003cp\u003eXRD pattern of as-synthesized MgAl-LDH nanocomposite\u003c/p\u003e","description":"","filename":"Picture2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/d304098cef2ff7bcad15eb00.jpg"},{"id":58836594,"identity":"a733ec6e-5f13-41a5-ba28-156e2795faa6","added_by":"auto","created_at":"2024-06-21 20:04:43","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":111034,"visible":true,"origin":"","legend":"\u003cp\u003ea)Electron Microscopy Analysis (SEM) (200KX, 5KX); b) Energy-dispersive X-ray spectroscopy (EDS) Spectrum analysis of MgAl-LDH nanocomposite\u003c/p\u003e","description":"","filename":"Picture3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/e7fd26416f94269024c80eb6.jpg"},{"id":58836593,"identity":"7a7dbfc0-7530-4e02-9bc3-70fdbf5e77c7","added_by":"auto","created_at":"2024-06-21 20:04:43","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":123143,"visible":true,"origin":"","legend":"\u003cp\u003eFTIR spectrum of zeolite and zeolite-LDH\u003c/p\u003e","description":"","filename":"Picture4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/2f95dce8f97e7968356017f3.jpg"},{"id":58836832,"identity":"8c087a13-b083-4ccf-ba1a-857442dc8ab8","added_by":"auto","created_at":"2024-06-21 20:12:43","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":24714,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Correlation between predicted vs. actual values, (b) Normal plot of residuals value\u003c/p\u003e","description":"","filename":"Picture5.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/5be787d9117bc6794020a5c7.jpg"},{"id":58836833,"identity":"cc8173c2-4bbc-48b2-99ef-49787cc8ea74","added_by":"auto","created_at":"2024-06-21 20:12:43","extension":"jpg","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":167403,"visible":true,"origin":"","legend":"\u003cp\u003eThe contours of 3D for cefixime removal by catalytic ozonation process with MgAl-LDH nanocatalyst; Catalyst dosage 1.5 g/L, C\u003csub\u003e0\u003c/sub\u003e_cefexime: 15mg/L, pH 7 and reaction time 32.5 min.\u003c/p\u003e","description":"","filename":"Picture6.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/ebbf2575508a4cbc28917c99.jpg"},{"id":58836591,"identity":"e53cc520-07d8-4ee1-8be2-2af1d2b9324f","added_by":"auto","created_at":"2024-06-21 20:04:43","extension":"jpg","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":87130,"visible":true,"origin":"","legend":"\u003cp\u003eThe graph of pH variation to determine the pHzpc of the catalyst surface\u003c/p\u003e","description":"","filename":"Picture7.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/da96de34265a7eef901b1e91.jpg"},{"id":83783647,"identity":"927cd9eb-b7ea-48d2-bead-88a1f3fc3597","added_by":"auto","created_at":"2025-06-02 16:12:21","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1937882,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/6d599b7a-21fb-4030-aa52-25a441216d7b.pdf"},{"id":58836834,"identity":"59583332-10f7-4b5f-8e9c-f4f292abae6b","added_by":"auto","created_at":"2024-06-21 20:12:43","extension":"jpg","order_by":6,"title":"","display":"","copyAsset":false,"role":"supplement","size":279304,"visible":true,"origin":"","legend":"","description":"","filename":"graphicalabs.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4388377/v1/0c40728264a32e0c3de9adb5.jpg"}],"financialInterests":"","formattedTitle":"Degradation of Cefixime Antibiotic by Heterogeneous Catalytic Ozonation Process using novel LDH/zeolite nano-composite:Modeling and Optimization Process","fulltext":[{"header":"Introduction","content":"\u003cp\u003eRecently, emerging pollutants, such as synthetic organic chemicals, have been large identified in the natural environment. These substances are considered a new group of micropollutant compounds that have harmful effects on human health and ecology [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e]. Also, these unknown substances have been frequently diagnosed in diverse effluents from urban sludge, daily household products, drug production units, hospital wastewater, sanitary landfills, and aquatic environments. It had been noted that the concentration of emerging pollutants was in the range of ng/L-mg/L. The large identified concentration of such compounds in water medium can potentially cause microbial large present in pharmaceutical organic pollutants, personal care products (PCPs), endocrine-disrupting compounds (EDCs), surfactants, insecticides, and industrial additives [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eAmong medicinal compounds, antibiotics are highly prescribed and consumed in the medical field. These drugs are still a hot topic about worldwide environmental health because creating resistance to bacterial species [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]. The consumption of antibiotics is pointed to be between 200000\u0026thinsp;\u0026minus;\u0026thinsp;100000 tons per year worldwide. These compounds are considered dangerous substances for the environment as they show varied genetic behaviors bringing substantial changes in different ecosystems. Over the last decades, various antibiotic residues have been recognized in surface water, underground water, and sewage treatment plants [\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]. The identification of these compounds in water mediums are mainly subjected to complex chemical structure, polarity, low volatility, hydrophilic, high stability, and antimicrobial properties in aquatic environments [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. Antibiotics are divided into several categories\u0026mdash;penicillin, cephalosporin, tetracycline, aminoglycosides, fluoroquinolones, macrolides, and sulfonamides. Among them, cephalosporins are classified into three generations [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]. Cefixime is one of the third-generation cephalosporins group, which is used in the treatment of infectious diseases under the brand name Suprax [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eCefixime is a semi-synthetic antibiotic, Cefixime is the first member of the third-generation cephalosporin class use for oral administration, a wide range of Gram-negative bacteria, and some Gram-positive aerobic bacteria [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThis antibiotic effectively applied against various bacterial organisms and infections, including staphylococcus, hemophilic influenza, Escherichia coli, streptococcus fever, tonsillitis, and throat infections [\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eCefixime is one of the most widely used antibiotics, with e half-life of around 3 and 4 hr, which is longer than other cephalosporins classes. The threshold risk level of Cefixime in water sources as an organic pollutant is 5 \u0026micro;g/L [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe enforcing Environmental laws and public health concerns have resulted in all institutions. The organizations should purify their wastewater before discharging their effluents into surface water or reusing based on the current environmental health standards [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eSince the concentration of antibiotics in surface water, underground water, sewage, and drinking water has been detected in ng/L to \u0026micro;g/L, an advanced system is needed to remove these compounds from aqueous environments. Therefore, conventional water and wastewater treatment processes cannot analyze and remove these compounds [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThus, various technologies have been applied to remove pharmaceutical compounds from wastewater, such as adsorption with activated carbon, reverse osmosis, stripping with air, and biologic methods. The mentioned procedures not only do not remove the pollutant but also transfer it from one phase to another [\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]. In the last decade, the application of advanced oxidation processes (AOPs) has been expanded to reduce the pollution caused by pharmaceutical residues in water. These processes are based on the formation of active hydroxyl radicals (˙OH) that react with organic substances to eradicate their structures [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e]. The typical AOPs in the purification of drugs include photolysis, catalytic ozonation, Fenton oxidation, heterogeneous photocatalyst, electrochemical oxidation, ultrasonic radiation, and wet air oxidation. Depending on the characteristics of wastewater under treatment, AOP\u003csub\u003eS\u003c/sub\u003e processes can be used alone or with other physical, chemical, and biologic processes [\u003cspan additionalcitationids=\"CR16 CR17\" citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eOxidation is a method used in recent years to decompose non-biodegradable pollutants. In oxidation reactions, electrons are transferred from an oxidizing substance to another substance [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e]. Ozone is one of the strong oxidants that directly and indirectly oxidize and decomposes the target pollutant. In the direct mechanism, the ozone molecule directly reacts with the aimed pollutant, and in indirect ozonation, the ozone molecule is decomposed and converted into hydroxyl radicals [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e]. Then, the hydroxyl radical reacts with the pollutant and eradicates it. However, ozone has limitations such as low oxidation rate, high energy consumption, and pollutant selectivity [\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eOne of the advanced oxidation processes is the catalytic ozonation process (COP). Adding a catalyst to the ozonation process leads to an increase in the amount of oxidation, a decrease in reaction time and production of toxic and by-products, and consequently an increase in usability as a complete treatment process or cheap pre-treatment [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]. The catalytic ozonation process can be used in both homogeneous and heterogeneous ways. Among these two methods, the heterogeneous catalytic ozonation process is suitable for wastewater treatment due to its low cost, the potential to regenerate the catalyst, and not cause secondary pollution. Some of the frequent catalysts proposed and used in this method are metal oxides (TiO\u003csub\u003e2\u003c/sub\u003e, MnO\u003csub\u003e2\u003c/sub\u003e, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, etc.), reinforced metals, or metal oxides such as CuTiO\u003csub\u003e2\u003c/sub\u003e, CU/Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, Fe\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, TiO\u003csub\u003e2\u003c/sub\u003e/Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, Co/SiO\u003csub\u003e2\u003c/sub\u003e, Ru/CeO\u003csub\u003e2\u003c/sub\u003e [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e, \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eRecently, another interesting catalyst has been layered double hydroxides (LDH), part of the family of synthetic and natural clay compounds. These minerals have a two-dimensional and layered structure consisting of positively charged cationic hydroxide layers with interlayers containing anions and water, such as clay minerals. Many divalent ions such as nickel, cobalt, copper, and zinc can create different forms of LDH with trivalent ions such as aluminum, chromium, iron, and gallium and produce large structural compounds. The mineral form of LDH of calcium with aluminum is known as hydrocalumite, and LDH of magnesium with aluminum is known as hydrotalcite (double-layer hydroxide).\u003c/p\u003e \u003cp\u003eIn general, the formula of LDHs is expressed as [M\u003csup\u003e2\u0026thinsp;+\u003c/sup\u003e\u0026thinsp;\u003csub\u003e1\u0026minus;x\u003c/sub\u003e M\u003csup\u003e3\u0026thinsp;+\u003c/sup\u003e\u0026thinsp;\u003csub\u003ex\u003c/sub\u003e (OH) \u003csub\u003e2\u003c/sub\u003e] (A\u003csup\u003en\u0026minus;\u003c/sup\u003e) \u003csub\u003ex/n\u003c/sub\u003e.mH\u003csub\u003e2\u003c/sub\u003eO, where M\u003csup\u003e2+\u003c/sup\u003e and M\u003csup\u003e3+\u003c/sup\u003e are divalent and trivalent cations, respectively. Also, A\u003csup\u003en\u0026minus;\u003c/sup\u003e represents the interlayer anions, and x is equal to the molar ratio of M\u003csup\u003e3+\u003c/sup\u003e/ (M\u003csup\u003e2+\u003c/sup\u003e + M\u003csup\u003e3+\u003c/sup\u003e). The layered structure, active interlayer space, high anion exchange, chemical and physical stability, and colloidal properties are prominent features of this nanocatalyst, causing much attention among advanced oxidation processes [\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e, \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe simultaneous application of adsorbent catalysts along with oxidation is called the adsorption-catalyst process (ACP). ACP processes are one of the AOP processes in which adsorption and reaction on the porous catalyst surface coincide [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. In ACP processes, porous materials are used, showing a dual function as adsorbents and catalysts in ozonation. These catalysts are different from non-porous catalysts that are usually used in ozonation processes as metal oxides or natural minerals. Among the porous adsorbents used are zeolite and activated carbon. One of the most common and cheapest natural zeolites is Clinoptilolite, whose features include environmental compatibility, heat resistance (up to 800 ℃), and oxidation by ozone [\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eIn the present study, the optimization of cefixime antibiotic decomposition by a powerful catalytic ozonation process with MgAl-layered double hydroxide nanocomposite placed on clinoptilolite zeolite (MgAl-LDH) under different conditions has been investigated, with RSM-CCD method. According to the authors' review, no study has been conducted on using ACP process with natural zeolite as a porous adsorbent.\u003c/p\u003e"},{"header":"Material and methods","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003eMaterials\u003c/h2\u003e \u003cp\u003eCefixime antibiotic powder used in this study was 98% pure (provided from Sigma Aldrich Company). Some characteristics of this antibiotic are shown in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e, \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]. The H\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e4\u003c/sub\u003e and NaOH solutions (1%) were consumed to adjust the pH level. Also, the ozone output from the reactor was decomposed in an impinger containing KI with a concentration of 20%. Other chemicals used in this study include MgCl\u003csub\u003e2\u003c/sub\u003e(H\u003csub\u003e2\u003c/sub\u003eO)\u003csub\u003e6\u003c/sub\u003e, AlCl\u003csub\u003e3\u003c/sub\u003e(H\u003csub\u003e2\u003c/sub\u003eO)\u003csub\u003e6\u003c/sub\u003e, Na\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e3\u003c/sub\u003e, KH\u003csub\u003e2\u003c/sub\u003ePO\u003csub\u003e4\u003c/sub\u003e, Na\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e3\u003c/sub\u003e, Na\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e3,\u003c/sub\u003e CH\u003csub\u003e3\u003c/sub\u003eOH, H\u003csub\u003e3\u003c/sub\u003ePO\u003csub\u003e4\u003c/sub\u003e and HCl. All chemicals were obtained from Merck, Germany.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eSome characteristics of Cefixime\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"2\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003emedicine name\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCefixime\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eStructure\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eMolecular formula\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eC\u003csub\u003e6\u003c/sub\u003eH\u003csub\u003e15\u003c/sub\u003eN\u003csub\u003e5\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eGroup\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThird-generation cephalosporin\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eMolecular Weight (g/mol)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e453.452\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eλmax\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e290 nm\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDissolvability\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eLow\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eColor\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003elight yellow\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eAverage half-life\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e3\u0026ndash;4 hours\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003epK\u003csub\u003ea1\u003c/sub\u003e (COOH group of cefixime nucleus)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2.1\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003epK\u003csub\u003ea2\u003c/sub\u003e (aminothiazole group)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2.92\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003epK\u003csub\u003ea3\u003c/sub\u003e (chain-COOH group)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e3.45\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eTable\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e Some characteristics of Cefixime\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003eMgAl-LDH synthesis coated on Zeolite\u003c/h2\u003e \u003cp\u003eThe MgAL-LDH Nanocatalyst was synthesized by co-precipitation method at room temperature [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. To prepare LDH coated on Zeolite, the 50 ml of 4 M sodium hydroxide was dropped wisely poured into an Erlenmeyer flask containing 50 ml of a solution containing 10.165 g of magnesium chloride hexahydrate and 9.63 g of aluminum chloride hexahydrate and 10 g of zeolite powder with constant magnetic stirring. After finishing the NaOH, it was sonicated for 30 minutes by BANDELIN machine (Bandelin Company, SONOREX DIGITEC model, made in Germany) with power of 165 W and 30 Hz frequency. Then, the suspension was located in the autoclave tank (Reyhan teb, RT-2 model, Made in Iran) and placed in the oven (FINE TECH Company, SHINSAENG model, made in Korea) at a temperature of 180 ℃ for 24 hr. After the completed the determination time, it was washed 5 times with double distilled water. Finally, it was dried in the oven at 60 ℃ within a day. The physical and structural characteristics of the obtained catalyst were determined by an X-Ray scattering device (PHILIPS Company, PW1730 model, made in the Netherlands). Also, to determine the crystal structure of the catalyst, the size of the catalyst was examined by electron microscopy (FESEM-EDAX; TESCAN mira3, Czech Republic). Moreover, the functional groups of the as-synthesized nanocomposite were investigated through infrared spectroscopy and FTIR (Thermo Company, AVATAR model, made in USA). pH\u003csub\u003eZPC\u003c/sub\u003e analysis was performed to determine the surface charge of MgAl-LDH nanocatalyst.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003eThe procedure for the determination of the pH\u003csub\u003eZPC\u003c/sub\u003e of catalyst\u003c/h2\u003e \u003cp\u003eTo determine the state of electric charge dispersion on the surface of the synthesized catalyst, the value of pH\u003csub\u003epzc\u003c/sub\u003e was measured [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e]. This parameter of catalysts is an index to evaluate and interpret the mechanism of the catalytic ozonation process. NaCl solution (0.01 M), hydrochloric acid (0.1 M), and soda (0.1 M) were used to determine pHpzc. In this process, 30 mL of NaCl electrolyte solution in distilled water was poured into 6 Erlenmeyer flasks with a volume of 50 mL. The pH of the solutions was adjusted in the range of 2 to 12 using the acid mentioned above and base chemicals. Then 1 g of catalyst was added to each flask and placed on a shaker at 200 rpm for 48 hr. After passing the mentioned time, the final pH of the filtered solution was measured with a pH meter (HACH Company, Sension156 model, made in USA). Eventually, the value of pHpzc was calculated by drawing the curve of pH changes against the initial pH.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003eSynthetic wastewater\u003c/h2\u003e \u003cp\u003eThe wastewater used in the reactor contained different concentrations of Cefixime, which was prepared synthetically. For this purpose, a standard solution of 1000 ppm antibiotic was prepared by dissolving 1 g of laboratory-grade antibiotic in 1 L of water. Other desired concentrations were prepared from this solution.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003eApparatus and Analytical Procedures\u003c/h2\u003e \u003cp\u003eAn ozone generator made in Iran with a 6 g/hr nominal capacity was used to supply ozone. The ozone flow rate was set to 1.5 L/min by the rotameter installed at the end of the reactor so that the ozone concentration entering the reactor was about 35 mgL\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003emin\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e using the iodometric titration method [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe measurement of the residual concentration of cefixime antibiotic was performed by a high-performance liquid chromatography device (HPLC, Waters 1525 made in USA) equipped with a UV absorption detector at a wavelength of 290 nm and a C18 column (Restek company, 5-mm particle size, 250 d 4.6 mm). The mobile phase consisted of methanol and 25 mM phosphate buffer 40:60% (v/v) and orthophosphoric acid to adjust the pH to 5.5, with a wavelength of 290 nm and a flow rate of 1.2 mL/min.\u003c/p\u003e \u003cp\u003eThe reactor used in this process was a Plexiglas cylinder with a diameter of 5 cm and a height of 1 m (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e), and the reactor system was designed as a semi-batch. Ozone gas was injected into the effluent through the air stone at the reactor's bottom.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. Schematic of catalytic ozonation reactor for cefixime degradation\u003c/p\u003e \u003cp\u003eIn each experimental run, 200 ml of synthetic wastewater containing a specific concentration of Cefixime was transferred to the reactor and subjected to the ACP process. The nanocatalyst used along with ozone consisted of MgAl-layered double hydroxide (MgAl-LDH), which was placed on a zeolite substrate. The parameters of this study included pH (9\u0026thinsp;\u0026minus;\u0026thinsp;5), nanocomposite concentration (0.5\u0026ndash;25 g/L), cefixime initial concentration (5\u0026ndash;25 mg/L), and reaction time (5\u0026ndash;60 min).\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003eExperiment design\u003c/h2\u003e \u003cp\u003eThis work investigated the removal of the Cefixime antibiotic by MgAl-LDH catalyst. The variables used in the current study were 4, which respectively include the initial concentration of cefixime (5\u0026ndash;25) mg/L, the contact time (5\u0026ndash;60) min, the pH (5\u0026ndash;9), and the adsorbent dosage (0.5\u0026ndash;2.5) g/L. This study was based on employing the RSM method (response surface method) and the Central Composite Design (CCD) test design using design expert version 11.0.3.0 software. The test design table, relevant variables, and results are presented in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. Paying attention to Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e, variable A is the initial concentration range, variable B is the pH range, C is the amount of catalyst, and D is the contact time. The response variable shows the removal efficiency. Also, the predicted removal values ​​are given in the last column of Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. The coefficients using Analysis of Variance (ANOVA) were analyzed, and p-value\u0026thinsp;\u0026ge;\u0026thinsp;0.05 was determined as a significant level.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab2\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 2\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eThe scope of the investigated variables in the design of the Catalytic ozonation process\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"8\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c8\" colnum=\"8\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eMain independent variables\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eUnit\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003esymbol\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colspan=\"5\" nameend=\"c8\" namest=\"c4\"\u003e \u003cp\u003elevel of variables\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003e-α\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003e-1\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c6\"\u003e \u003cp\u003e0\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c7\"\u003e \u003cp\u003e+\u0026thinsp;1\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c8\"\u003e \u003cp\u003e+α\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003epH\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e-\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eB\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c8\"\u003e \u003cp\u003e9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eDose of catalyst\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eg/L\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eC\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e0.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c8\"\u003e \u003cp\u003e2.5\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eReaction time\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003emin\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eD\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c8\"\u003e \u003cp\u003e60\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCefixime concentration\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003emg/L\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eA\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c8\"\u003e \u003cp\u003e25\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eTable\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e The scope of the investigated variables in the design of the Catalytic ozonation process\u003c/p\u003e \u003cp\u003eThe CCD-RSM method uses variance analysis and response surface regression analysis to determine the fit of the test results with the multivariate quadratic model as follows:\u003cdiv id=\"Equa\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equa\" name=\"EquationSource\"\u003e\n$$\\text{Y}= {\\text{a}}_{0}+\\sum _{\\text{i}=1}^{\\text{k}}{\\text{a}}_{\\text{i} }{\\text{x}}_{\\text{i}}+ \\sum _{\\text{i}=1}^{\\text{k}}{\\text{a}}_{\\text{i}\\text{i} }{\\text{x}}_{\\text{i}}^{2} + \\sum _{\\text{i}\\ne 1}^{\\text{n}}{\\text{a}}_{\\text{i}\\text{j}}{\\text{x}}_{\\text{i}}{\\text{x}}_{\\text{j}}+{\\epsilon } \\left(1\\right)$$\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003eWhere y is assigned to the predicted removal efficiency (percentage), a\u003csub\u003e0\u003c/sub\u003e is the constant coefficient, a\u003csub\u003ei\u003c/sub\u003e, a\u003csub\u003eii\u003c/sub\u003e, a\u003csub\u003eij\u003c/sub\u003e are the estimated coefficients for the main, quadratic, and reciprocal effects, respectively, and xi and x\u003csub\u003ej\u003c/sub\u003e are the input variables in actual values. n, specifies the number of input variables, and e is assigned to the model error [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. The CCD method, according to the prediction model, can exhibit the impacts of operating variables on the performance of the cefixime antibiotic removal process. The variables were optimized to achieve the maximum removal efficiency of Cefixime based on the desired performance in the CCD method. The runs determined by the software are shown in Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab3\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 3\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eThe 4-factor CCD matrix with actual factor levels for Cefixime removal based on RSM method\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"7\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eStd\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eA:C\u003csub\u003e0\u003c/sub\u003e\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eB:pH\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eC:Catalyst dosage\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\" morerows=\"1\" rowspan=\"2\"\u003e \u003cp\u003eD:Time reaction\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colspan=\"2\" nameend=\"c7\" namest=\"c6\"\u003e \u003cp\u003eY:Cefixime degradation efficiency\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c6\"\u003e \u003cp\u003eActual Value\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c7\"\u003e \u003cp\u003ePredicted Value\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003emg/L\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003eg/L\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003emin\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e(%)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e(%)\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e75.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e75.33\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e82.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e82.1\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e80.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e80.42\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e4\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e84.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e84.05\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e83.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e82.94\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e87.45\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e88.07\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e90.89\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e18.75\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e93.10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e92.88\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e92.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e92.18\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e97.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e97.19\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e11\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e93.70\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e93.15\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e12\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e95.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e95.03\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e13\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e93.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e93.02\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e14\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e96.85\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e96.39\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e97.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e96.86\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e16\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e46.25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e97.35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e97.09\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e17\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e89.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e88.98\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e18\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e96.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e95.99\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e19\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e87.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e86.56\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.93\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e92.34\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e21\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e0.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e85.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e84.65\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e22\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e94.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e94.32\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e23\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e78.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e77.45\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e24\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e60\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e98.00\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e98.51\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e25\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.47\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e26\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e92.07\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e27\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.80\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e28\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e92.20\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e29\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.93\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e30\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.93\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e31\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.90\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e32\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.95\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e33\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.93\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e34\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.93\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.89\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e36\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e1.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e32.5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e91.83\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003e91.9\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"Results and discussion","content":"\u003cdiv id=\"Sec10\" class=\"Section2\"\u003e \u003ch2\u003eNano-composite properties\u003c/h2\u003e \u003cdiv id=\"Sec11\" class=\"Section3\"\u003e \u003ch2\u003eX-ray diffraction (XRD)\u003c/h2\u003e \u003cp\u003eThis analysis is done to scrutinize the crystallinity or crystal size. The diffraction pattern of the samples is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. The samples were obtained using a diffractometer of 40 kV and 30 mA at a diffraction angle between 5 and 70\u0026deg;C at room temperature with a radiation source (Cu-α\u0026thinsp;=\u0026thinsp;1.54). Scherer equation Eq.\u0026nbsp;\u003cspan refid=\"Equ1\" class=\"InternalRef\"\u003e2\u003c/span\u003e., was computed to estimate the crystallite size [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]:\u003c/p\u003e \u003cp\u003e \u003cdiv id=\"Equ1\" class=\"Equation\"\u003e \u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ1\" name=\"EquationSource\"\u003e\n$$d= \\frac{K\\lambda }{\\beta COS \\theta }$$\u003c/div\u003e \u003cdiv class=\"EquationNumber\"\u003e2\u003c/div\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eIn the above equation, d is the crystal size, λ is the X-ray wavelength, β is the peak width (width at half maximum value (FWHM), θ is the Bragg angle, and K is Scherer's constant (equal to 0.9).\u003c/p\u003e \u003cp\u003eAccording to the crystal structure data of Clinoptilolite in JCPDS (instrument library number 1349-0025-00), the observed pattern of the clinoptilolite zeolite sample demonstrates characteristic peaks at 9.85\u0026deg;, 11.18\u0026deg;, 17.3\u0026deg; and 19.1\u0026deg;, 22.34\u0026deg;, 22.7\u0026deg;, 25\u0026deg;, 26.04\u0026deg;, 28.15\u0026deg;, 30\u0026deg;, and 32\u0026deg;, which is consistent with the results reported by other researchers [\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e, \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e, \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]. The spectrum of zeolite-LDH revealed characteristic diffractions for zeolite is lower intensity with specific shifted, which could be due to overlap with LDH peaks. Also, some other peaks at 45.6\u0026deg;, 56.6\u0026deg;, and 66.5\u0026deg; were also observed in zeolite-LDH with higher intensity, indicating a higher degree of crystallization for LDH crystals [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. Therefore, the XRD (TESCAN Company, Mira3, Czech Republic) pattern of zeolite-LDH shows that peaks related to zeolite and LDH, which demonstrate the successful and effective growth of LDH crystals on zeolite components. By Scherer's equation, the crystallite size of zeolite and zeolite-LDH was estimated to be around 11 nm and 20 nm, respectively.\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e XRD pattern of as-synthesized MgAl-LDH nanocomposite\u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec12\" class=\"Section2\"\u003e \u003ch2\u003eScanning electron microscope (FE-SEM)\u003c/h2\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(a), the synthesized catalyst has a uniform and layered structure with specific nanometer dimensions. As a result, this indicates the proper synthesis conditions.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea) Electron Microscopy Analysis (SEM) (200KX, 5KX); b) Energy-dispersive X-ray spectroscopy (EDS) Spectrum analysis of MgAl-LDH nanocomposite\u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(b) shows the Weight and atomic percentage of the elements toward the synthesized catalyst. Additionally, element mapping analysis by element including O, Na, Mg, Al, Si, Cl, K, and color and overall composition of elements can be seen in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec13\" class=\"Section2\"\u003e \u003ch2\u003eInfrared spectroscopic analysis (FTIR)\u003c/h2\u003e \u003cp\u003eFourier transform infrared (FTIR) spectroscopic analysis was used to present the chemical structure of the functional groups of zeolite (Zeo) and zeolite modified with layered double hydroxide (Zeo-LDH). The FTIR spectra of the above samples in the range of 400 to 4000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e are presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eRegarding the spectrum of zeolite (Clinoptilolite), the vibrations around 1600\u0026ndash;3700 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e can be attributed to the water absorbed by the zeolite. For example, The peak at 3622 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e is related to the interaction of the hydroxyl of water with cations, and the other bands are attributed to the hydrogen bond of the water molecule to the surface oxygen (3451 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) and the bending vibration mode of water (1635 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e). The peak at 1067cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e is responsible for the asymmetric stretching vibrations of the T-O bonds in the TO4 tetrahedron (T equals Si and Al). Furthermore, peaks at 796 and 469 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e can be observed, which are respectively assigned to the stretching vibrations of the O-T-O groups and the bending stretching of the T-O bonds, these results are similar to the results obtained by other authors [\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e, \u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e]. The functional groups observed for the zeolite-LDH spectrum were analogous to the zeolite spectrum, which were slightly different only in the detection frequency and wavelength of the functional groups. Compared to zeolite, zeolite-LDH showed a broad peak at 3477 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, corresponding to the formation of hydrogen bonds in the stretching bands of hydroxyl groups and H\u003csub\u003e2\u003c/sub\u003eO from the surface and interlayer [\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e, \u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]. The spectrum of zeolite-LDH has a weak absorption peak due to the absorption of CO\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e2\u0026minus;\u003c/sup\u003e at 1384 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, this finding is consistent with the study of other researcher[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e FTIR spectrum of zeolite and zeolite-LDH\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec14\" class=\"Section2\"\u003e \u003ch2\u003eDevelopment of regression model\u003c/h2\u003e \u003cp\u003eIn the current work, the efficiency of the catalytic ozonation process with MgAl-LDH nanocomposite based on zeolite in the removal of cefixime antibiotic using CCD to optimize four variables was investigated, and the findings are shown in Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e.\u003c/p\u003e \u003cp\u003eTable\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e The 4-factor CCD matrix with actual factor levels for Cefixime removal based on RSM method\u003c/p\u003e \u003cp\u003eThe compatibility of Linear, 2FI, Quadratic, and Cubic models related to the obtained experimental results was investigated (Table\u0026nbsp;\u003cspan refid=\"Tab4\" class=\"InternalRef\"\u003e4\u003c/span\u003e). Based on the value of \u003cb\u003eAdjusted R\u0026sup2;\u003c/b\u003e, the proposed model was Quadratic model with 0.99 R\u0026sup2;. The value of \u003cb\u003ePredicted R\u0026sup2;\u003c/b\u003e for this model was equal to 0.98, which is in good agreement with \u003cb\u003eAdjusted R\u0026sup2;\u003c/b\u003eas the difference between them is less than 0.2.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab4\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 4\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eThe results of investigating cefixime removal models by RSM-CCD method\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"6\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eSource\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eSequential p-value\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eLack of Fit P-value\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eAdjusted R\u0026sup2;\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003ePredicted R\u0026sup2;\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c6\"\u003e\u0026nbsp;\u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eLinear\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.8481\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.8029\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e2FI\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e0.0004\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.9243\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.8943\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eQuadratic\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e\u003cb\u003e\u0026lt;\u0026thinsp;0.0001\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e\u003cb\u003e0.0007\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e\u003cb\u003e0.9955\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e\u003cb\u003e0.9859\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003e\u003cb\u003eSuggested\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCubic\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e0.7658\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.9991\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.9975\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e \u003cp\u003eAliased\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eTable\u0026nbsp;\u003cspan refid=\"Tab4\" class=\"InternalRef\"\u003e4\u003c/span\u003e The results of investigating cefixime removal models by RSM-CCD method\u003c/p\u003e \u003cp\u003eAccording to the results, for all the investigated parameters, the p-value is less than 0.0001, and all 4 variables are significant. means that the studied model can describe the catalyst's investigation of cefixime antibiotic removal. The F-value for the variables indicates the most significant effect of the reaction time variable on the efficiency of cefixime decomposition by the process. .Based on the results of analysis of Variance from Table\u0026nbsp;\u003cspan refid=\"Tab5\" class=\"InternalRef\"\u003e5\u003c/span\u003e, the selected model was significant. The variables of pH, catalyst dose, cefixime initial concentration and contact time had a significant effect on the reaction rate. Using the response-level statistical method, the predicted model of the quadratic type and the coded relationship below Eq.\u0026nbsp;3. expresses the empirical relationship between the test experiences and the removal efficiency.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab5\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 5\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eThe results of analysis of variance of the quadratic model of cefixime antibiotic removal\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"7\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eSource\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eSum of Squares\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003edf\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eMean Square\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eF-value\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c6\"\u003e \u003cp\u003ep-value\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eModel\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e1071.13\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e14\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e76.51\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e556.15\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003esignificant\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eA-C\u003csub\u003e0\u003c/sub\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e73.68\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e73.68\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e535.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eB-pH\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e50.22\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e50.22\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e365.04\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC-Catalyst\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e140.41\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e140.41\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e1020.64\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eD-time\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e665.18\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e665.18\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e4835.24\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eAB\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e9.84\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e9.84\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e71.56\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eAC\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e2.68\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e2.68\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e19.49\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0002\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eAD\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e3.11\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e3.11\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e22.58\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBC\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e8.19\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e8.19\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e59.56\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBD\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e16.91\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e16.91\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e122.94\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCD\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e45.73\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e45.73\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e332.42\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eA\u0026sup2;\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e0.6712\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.6712\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e4.88\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0384\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eB\u0026sup2;\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e12.04\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e12.04\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e87.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eC\u0026sup2;\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e11.72\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e11.72\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e85.19\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eD\u0026sup2;\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e30.74\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e30.74\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e223.48\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e\u0026lt;\u0026thinsp;0.0001\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eResidual\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e2.89\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e21\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.1376\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eLack of Fit\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e2.56\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.2562\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e8.61\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0007\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e \u003cp\u003esignificant\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePure Error\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e0.3273\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e11\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e0.0298\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCor Total\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e1074.02\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e35\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c6\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c7\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003e \u003cem\u003eCefixime removal (%)=\u003c/em\u003e -20.11081\u0026thinsp;+\u0026thinsp;1.72867A\u0026thinsp;+\u0026thinsp;12.67199B\u0026thinsp;+\u0026thinsp;12.52913C\u0026thinsp;+\u0026thinsp;1.70827D-0.156875 AB-0.163750 AC-0.006409 AD\u0026thinsp;+\u0026thinsp;1.43125 BC-0.074773 BD-0.245909 CD\u0026thinsp;+\u0026thinsp;0.005793A\u003csup\u003e2\u003c/sup\u003e-0.613507B\u003csup\u003e2\u003c/sup\u003e-2.42069C\u003csup\u003e2\u003c/sup\u003e-0.005184D\u003csup\u003e2\u003c/sup\u003e (3)\u003c/p\u003e \u003cp\u003eTable\u0026nbsp;\u003cspan refid=\"Tab5\" class=\"InternalRef\"\u003e5\u003c/span\u003e The results of analysis of variance of the quadratic model of cefixime antibiotic removal\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e (a) Correlation between predicted vs. actual values, (b) Normal plot of residuals values\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIn Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e. (a), the relationship between the predicted and actual values is plotted against each other, and the placement of points near the common line indicates the appropriate results from the experiments. Moreover, in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e (b), the Normal plot of residuals values obtained from the experiments which indicates the normality of the data and the Predictive model expresses a quantitative amount, exhibiting the appropriate accuracy of the results.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec15\" class=\"Section2\"\u003e \u003ch2\u003eThe influence of operational variables on Degredation efficiency\u003c/h2\u003e \u003cp\u003eThe initial pH of the solution is a main parameter affecting the catalytic ozonation process [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. Therefore, the effect of initial pH on the removal efficiency of Cefixime by catalytic ozonation process with LDH nanocatalyst is scrutinized and is shown in 3D response surfaces in the central point values of other parameters in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e. What is more, the graph of pH changes to determine the pHzpc of the catalyst surface is observed in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e. The contours of 3D for cefixime removal by catalytic ozonation process with MgAl-LDH nanocatalyst; Catalyst dosage 1.5 g/L, C\u003csub\u003e0\u003c/sub\u003e_cefexime: 15mg/L, pH 7 and reaction time 32.5 min.\u003c/p\u003e \u003cp\u003eAccording to the findings, increasing the pH level from 5 to 9 improves the removal efficiency from 70 to 90%. Altering the pH of the solution affects the amounts of dissolved ions, the properties of the catalyst surface, and the rate of ionization of the compounds. These changes can be related to the pH\u003csub\u003eZPC\u003c/sub\u003e of the catalyst surface and the pKa of the target pollutant. The results of mass titration of acid and base of MgAl-LDH catalyst in Fig .7. show the value of pHzpc equal to 8.7.\u003c/p\u003e \u003cp\u003eMgAl-LDH nanocatalyst was determined to be 8.7 by the solid addition method. At pH\u0026thinsp;\u0026gt;\u0026thinsp;pH\u003csub\u003eZPC\u003c/sub\u003e, the catalyst surface is negatively charged, while at pH\u0026thinsp;\u0026lt;\u0026thinsp;pH\u003csub\u003eZPC\u003c/sub\u003e is positively charged, at pH\u0026thinsp;\u0026asymp;\u0026thinsp;pH\u003csub\u003eZPC\u003c/sub\u003e is neutral. Since the pKa for Cefixime has been recorded to be 3.73, at higher pH levels, cefixime molecules are ionized as negative ions in solution [\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e, \u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]. Thus, the influence of pH on catalytic ozonation can be attributed to the electrostatic interaction between the surface of nanoparticles and target pollutants. On the other hand, as mentioned in the \u003cspan refid=\"Sec1\" class=\"InternalRef\"\u003eintroduction\u003c/span\u003e section, the mechanism of oxidation by ozone is direct and indirect. The ozone molecule directly oxidizes the target pollutant in acidic pH through selectivity reactions. Consequently, this restriction prevents the oxidation of all pollutants [\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e, \u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e]. However, indirect oxidation occurs at alkaline pH, leading to ozone decomposed and powerful hydroxyl radicals being produced, which in the presence of MgAl-LDH nanocatalyst, improves ozone molecule decomposition and hydroxyl radical production [\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]. Unlike the ozone molecule, hydroxyl radicals act non-selectively in addition to their higher destructive power. In this regard, other studies also reached similar results [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e, \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e, \u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e, \u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e The graph of pH variation to determine the pHzpc of the catalyst surface\u003c/p\u003e \u003cp\u003eThe catalyst dose used in the process is one of the effective factors in increasing the efficiency of cefixime pollutant degradation. As can be seen in the 2D and 3D contours, with the increase of the catalyst dose from 0.5 to 2.5 gr, the cefixime removal efficiency has increased from less than 50% to about 90%. In general, based on other literature, the following mechanisms are suggested for the degradation of cefixime antibiotic by ACP process with MgAl-LDH nanocatalyst supported on zeolite:\u003c/p\u003e \u003cp\u003e \u003col\u003e \u003cspan\u003e \u003cli\u003e \u003cp\u003e(a) Adsorption of ozone molecules on zeolite and LDH, its decomposition into active radicals, and then the destruction of Cefixime by these active radicals\u003c/p\u003e \u003c/li\u003e \u003c/span\u003e \u003cspan\u003e \u003cli\u003e \u003cp\u003e(b) Cefixime molecules adsorbed on the surface of zeolite, and LDH are decomposed and destroyed by ozone molecules and hydroxyl radicals produced.\u003c/p\u003e \u003c/li\u003e \u003c/span\u003e \u003cspan\u003e \u003cli\u003e \u003cp\u003e(c) Ozone and cefixime molecules are simultaneously adsorbed on the surface of zeolite and LDH and react [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e].\u003c/p\u003e \u003c/li\u003e \u003c/span\u003e \u003c/ol\u003e \u003c/p\u003e \u003cp\u003eIn overall, ozone destruction and hydroxyl radical production during the ACP process are according to (4\u0026ndash;10) reactions [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]:\u003c/p\u003e \u003cp\u003eM\u003csup\u003en+\u003c/sup\u003e + O\u003csub\u003e3\u003c/sub\u003e\u0026thinsp;+\u0026thinsp;H\u003csup\u003e+\u003c/sup\u003e \u0026rarr; M\u003csup\u003e(n+1)+\u003c/sup\u003e + HOֺ + O\u003csub\u003e2\u003c/sub\u003e (4)\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec16\" class=\"Section2\"\u003e \u003ch2\u003eO\u003csub\u003e3\u003c/sub\u003e\u0026thinsp;+\u0026thinsp;HOֺ \u0026rarr; O\u003csub\u003e2\u003c/sub\u003e\u0026thinsp;+\u0026thinsp;HO.\u003csup\u003e\u0026minus;\u003c/sup\u003e\u003csub\u003e2\u003c/sub\u003e (5)\u003c/h2\u003e \u003cp\u003eM \u003csup\u003e(n+1)+\u003c/sup\u003e + HO.\u003csup\u003e\u0026minus;\u003c/sup\u003e\u003csub\u003e2\u003c/sub\u003e + HO\u003csup\u003e\u0026minus;\u003c/sup\u003e \u0026rarr; M\u003csup\u003en+\u003c/sup\u003e + H\u003csub\u003e2\u003c/sub\u003eO\u0026thinsp;+\u0026thinsp;O\u003csub\u003e2\u003c/sub\u003e (6)\u003c/p\u003e \u003cp\u003eMn\u003csup\u003e+\u003c/sup\u003e + HOֺ \u0026rarr; M\u003csup\u003e(n+1)+\u003c/sup\u003e + HO\u003csup\u003e\u0026minus;\u003c/sup\u003e (7)\u003c/p\u003e \u003cp\u003eMn\u003csup\u003e+\u003c/sup\u003e + O\u003csub\u003e3\u003c/sub\u003e \u0026rarr; M\u003csup\u003e(n+1)+\u003c/sup\u003e + O.\u003csup\u003e\u0026minus;\u003c/sup\u003e\u003csub\u003e3\u003c/sub\u003e (8)\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec17\" class=\"Section2\"\u003e \u003ch2\u003eO.\u003csup\u003e\u0026minus;\u003c/sup\u003e\u003csub\u003e3\u003c/sub\u003e + H+ \u0026rarr; HOֺ\u003csub\u003e3\u003c/sub\u003e (9)\u003c/h2\u003e \u003cdiv id=\"Sec18\" class=\"Section3\"\u003e \u003ch2\u003eHOֺ\u003csub\u003e3\u003c/sub\u003e + O\u003csub\u003e2\u003c/sub\u003e \u0026rarr; HOֺ (10)\u003c/h2\u003e \u003cp\u003eIn these reactions, M represents cations such as Al and Mg, and n represents the charge of the ion. As mentioned, LDH nanoparticles have a layered and 2D structure, and these layers include positively charged cationic hydroxides and layers containing anions and water. Since Al\u003csup\u003e3+\u003c/sup\u003e and Mg\u003csup\u003e2+\u003c/sup\u003e cations are placed in the center of the octahedral structure of LDH and hydroxyls are placed at the edges, the water molecules adsorbed on these surfaces are ionized to OH\u003csup\u003e\u0026minus;\u003c/sup\u003e and H\u003csup\u003e+\u003c/sup\u003e ions and form surface hydroxyl groups, which result in ozone reacts with these molecules and produces hydroxyl radicals, and finally, these radicals destroy the Cefixime adsorbed in the pores of the MgAl-LDH nanocatalyst placed on the zeolite base, which has an adsorption-catalytic effect[\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]. Therefore, increasing the dose of the catalyst can lead to an increase in the removal efficiency of Cefixime. To date, MgAl-LDH nanocomposite has been used as a catalyst in several studies, and similar results have been obtained. Pourfaraj et al. (2017) investigated the efficiency of MgAl-LDH nanoplates for absorbing Brilliant Yellow dye from aqueous medium. The results of this study indicate an increase in the efficiency of the absorption process by increasing the dose of MgAl-LDH nanoplates, which indicates the direct effect of the nanocomposite dose on the pollutant absorption capacity [\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. In another study, the decomposition of p-nitroaniline by catalytic ozonation process with MgAl-LDH nanocatalyst has been tested, and the results obtained regarding the catalyst dosage are in line with the results of the present study. In fact, with the increase in the dose of this nanocomposite, the production of OHֺ radicals increased, which leads to an increase in the rate of decomposition of the target pollutant [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe initial concentration range of Cefixime was considered to be 5\u0026ndash;25 mg/L by studying other similar literature, and its effect on the efficiency of the catalytic ozonation process was investigated. The results are shown in 2D and 3D response surface plots (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e). The results showed that in this range of Cefixime concentration, with increased Cefixime concentration, its removal efficiency also increased. Increasing the concentration of the target pollutant leads to the enhancement in the catalyst dosage and reaction time. According to the result of the modeling analysis (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e) and the effect of the reaction on the pH of the sample, we see a different removal percentage of the cefixime drug from the samples. In general, the effect of the initial concentration is smaller than the contact time and the catalyst dose.\u003c/p\u003e \u003cp\u003eThe application of MgAl-LDH nanoparticles based on zeolite along with ozone molecules, in addition to the role of a catalyst and the production of hydroxyl radicals, has also improved the absorption capacity, which in the mentioned concentration range of Cefixime, increasing the initial concentration did not have an inhibitory effect on the efficiency of the process [\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e]. Meanwhile, regarding other AOPS studies to remove Cefixime, different results have been obtained. including the study of Salimi et al. (2019), in which the photocatalytic decomposition of Cefixime with MIL125ML/g CN-20 nanocomposite has been investigated, and according to the results, it has been reported that by increasing the initial concentration of Cefixime from 15 to 25 mg/L, the degradation rate of the target contaminant has been declined because of covering the nanocomposite with intermediate molecules and reducing the absorption of light by the nanocomposite [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]. In another study, cefixime degradation was done by photocatalytic ozonation process with N-TiO\u003csub\u003e2\u003c/sub\u003e/graphene oxide/titanium nanosheets at concentrations of 5\u0026ndash;20 mg/L by Sheydaei et al. The results show that with increasing the initial concentration of Cefixime, the reaction rate constant has decreased, and the reason for that is the limitation in the number of active sites of the nanocomposite, which are saturated by absorbing a certain concentration of Cefixime [\u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]. The treatment of wastewater containing diazinon pesticide was conducted by catalytic ozone process with MgAl-LDH nanoparticles. The achieved results are similar to the current. However, in the present study, modification of this nanocomposite with zeolite base and ACP process did not decrease the removal efficiency of higher concentrations, which is one of the strengths of this process [\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eAccording to the analysis of variance and the contact time of the cefixime reaction and the catalytic ozonation process that took place in the time range of 5\u0026ndash;60 min, it shows that the contact time has the most important effect among the variables and we see an increase in the removal efficiency of Cefixime up to 98%.\u003c/p\u003e \u003c/div\u003e \u003c/div\u003e \u003cdiv id=\"Sec19\" class=\"Section2\"\u003e \u003ch2\u003eOptimization\u003c/h2\u003e \u003cp\u003eAccording to the results of the model and using the optimization part of the Design Expert software, the optimal conditions of the process were determined. For the antibiotic Cefixime, the optimal removal conditions by the catalyst were determined at a pH of 7.72, an adsorbent dose of 0.997g/L, with a reaction time of 55.23 min and an initial concentration of 22.8 mg/L.\u003c/p\u003e \u003cp\u003eThe presence of toxic compounds in the environment creates potential hazards for aquatic and terrestrial organisms, and the provision of healthy water is a necessity for the continuation of life. sample in this study was real, the results can be used directly in wastewater treatment produced in the poison manufacturing industry and similar industries.\u003c/p\u003e \u003c/div\u003e"},{"header":"Conclusion","content":"\u003cp\u003eThis study investigated the efficiency of the catalytic ozonation process using MgAl-LDH nanoparticles to cefixime elimination from aqueous solutions. The synthesized MgAl-LDH nanocomposite supported on zeolite was proved to be a potential catalyst for degrading Cefixime by the catalytic ozonation process.\u003c/p\u003e \u003cp\u003eIn this process, the effect of parameters of initial pH, cefixime concentration, catalyst dose, and contact time for cefixime removal was evaluated. In the optimal conditions obtained by the CCD method for the COP process, the removal efficiency of Cefixime at pH of 7.72, nanocatalyst dosage of 0.997 g/L, cefixime concentration of 22.8 mg/L, and reaction time of 55.23 min was stood at 98.37%. The presence of MgAl-LDH nanocatalyst placed on zeolite with ozone, in addition to absorbing the target pollutant, absorbs and decomposes the ozone molecule and produces hydroxyl radicals. The production of more hydroxyl radicals leads to an increase in the removal efficiency of Cefixime. Therefore, the use of this process is suggested for wastewater containing antibiotics.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis research is a part of the\u0026nbsp;doctoral\u0026nbsp;thesis titled\u0026nbsp;\u0026quot;\u003cem\u003eInvestigating the removal of cefixime by Catalytic Ozonation in the presence of LDH nano composite placed on a Zeolite substrate by the central composite design(CCD) method\u0026nbsp;\u003c/em\u003e\u0026quot;. Thanks are hereby given to the support of Islamic Azad University of Gorgan branch and Golestan University of Medical Sciences for conducting this research.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthors\u0026rsquo; contributions\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eConceptualization:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eData curation:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eFormal analysis:\u0026nbsp;Yalda Sheikh.\u003c/p\u003e\n\u003cp\u003eFunding acquisition:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eInvestigation:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eMethodology:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eProject administration:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eResources:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eSoftware:\u0026nbsp;Yalda Sheikh.\u003c/p\u003e\n\u003cp\u003eSupervision:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eValidation:\u0026nbsp;Mohammad Taghi Baei, Hamidreza Jaliliane\u003c/p\u003e\n\u003cp\u003eVisualization:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban-Shahamat.\u003c/p\u003e\n\u003cp\u003eWriting\u0026ndash;original draft:\u0026nbsp;Yalda Sheikh.\u003c/p\u003e\n\u003cp\u003eWriting\u0026ndash;review \u0026amp; editing:\u0026nbsp;Elham\u0026nbsp;Tazikeh-Lemeski\u0026nbsp;,\u0026nbsp;Yousef Dadban Shahamat,\u0026nbsp;Yalda Sheikh, Mohammad Taghi Baei, Hamidreza Jaliliane.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting interests\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe author(s) declare no competing interestsEthical approval\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eEthical approval\u003c/strong\u003e\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThis article does not contain any studies with human participants or animals performed by any of the authors.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe data will be available on the request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eWang L, Jiang H, Wang H, Show PL, Ivanets A, Luo D, Wang C. 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Appl Catal B: Environ. 2010;99(1\u0026ndash;2):27\u0026ndash;42.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSeftel E, Popovici E, Beyers E, Mertens M, Zhu H, Vansant E, Cool P. New TiO2/MgAl-LDH nanocomposites for the photocatalytic degradation of dyes. J Nanosci Nanotechnol. 2010;10(12):8227\u0026ndash;33.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eSheydaei M, Shiadeh HRK, Ayoubi-Feiz B, Ezzati R. Preparation of nano N-TiO\u003csub\u003e2\u003c/sub\u003e/graphene oxide/titan grid sheets for visible light assisted photocatalytic ozonation of cefixime. J Chem Eng. 2018;353:138\u0026ndash;46.\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":true,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"journal-of-environmental-health-science-and-engineering","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"jehs","sideBox":"Learn more about [Journal of Environmental Health Science and Engineering](https://www.springer.com/journal/40201)","snPcode":"40201","submissionUrl":"https://www.editorialmanager.com/jehs/","title":"Journal of Environmental Health Science and Engineering","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Cefixime, LDH, Nanocomposites, Ozonation, Wastewater, Zeolite","lastPublishedDoi":"10.21203/rs.3.rs-4388377/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4388377/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eIn recent decades, the indiscriminate use of antibiotics and their discharge into the environment have caused serious consequences for aquatic and terrestrial organisms. In the present study, the optimization of cefixime antibiotic decomposition by a powerful catalytic ozonation process has been investigated.\u003c/p\u003e \u003cp\u003eIn this study, MgAl-LDH /zeolite nanocomposite was synthesized and use as an ozonation-adsorption catalyst for the degradation of Cefixime antibiotic from aqueous solution. XRD, FE-SEM, and FTIR analyzes were scrutinized to reveal the main characteristics of the as-prepared nanocomposite, showing that it was well-synthesized. The investigated variables in the catalytic ozonation of Cefixime by the mentioned nanocomposite included solution pH level (5\u0026ndash;9), nanocatalyst dose (0.5\u0026ndash;2.5 g/L), Cefixime concentration (5\u0026ndash;25 mg/L) and reaction time (5\u0026ndash;60 min) which they were optimized by adopting RSM-CCD.\u003c/p\u003e \u003cp\u003eThe results showred that all variables had a positive effect on the efficiency of the catalytic ozonation process. Nonetheless, the lowest effect of operational factor pH, the degradation of Cefixime was subjected to the initial content of Cefixime in this treatment system.\u003c/p\u003e \u003cp\u003eThe optimal conditions for cefixime removal by catalytic ozonation process were determined at pH of 7.72, nanocatalyst dosage of 1 g/L, cefixime concentration of 23 mg/L, and reaction time of 55 min. In the optimized operating conditions, the removal efficiency of Cefixime by MgAl-LDH /zeolite nanocomposite was high up to 98.37%.\u003c/p\u003e","manuscriptTitle":"Degradation of Cefixime Antibiotic by Heterogeneous Catalytic Ozonation Process using novel LDH/zeolite nano-composite:Modeling and Optimization Process","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-06-21 20:04:38","doi":"10.21203/rs.3.rs-4388377/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"reviewerAgreed","content":"","date":"2024-06-07T16:04:08+00:00","index":0,"fulltext":""},{"type":"reviewersInvited","content":"","date":"2024-06-07T06:31:15+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-05-08T22:52:28+00:00","index":"","fulltext":""},{"type":"submitted","content":"Journal of Environmental Health Science and Engineering","date":"2024-05-08T05:37:39+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"journal-of-environmental-health-science-and-engineering","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"jehs","sideBox":"Learn more about [Journal of Environmental Health Science and Engineering](https://www.springer.com/journal/40201)","snPcode":"40201","submissionUrl":"https://www.editorialmanager.com/jehs/","title":"Journal of Environmental Health Science and Engineering","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"d8ad54ad-3940-4aef-bb97-92f9fd21d85e","owner":[],"postedDate":"June 21st, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2025-06-02T16:10:43+00:00","versionOfRecord":{"articleIdentity":"rs-4388377","link":"https://doi.org/10.1007/s40201-025-00941-5","journal":{"identity":"journal-of-environmental-health-science-and-engineering","isVorOnly":false,"title":"Journal of Environmental Health Science and Engineering"},"publishedOn":"2025-05-27 15:57:50","publishedOnDateReadable":"May 27th, 2025"},"versionCreatedAt":"2024-06-21 20:04:38","video":"","vorDoi":"10.1007/s40201-025-00941-5","vorDoiUrl":"https://doi.org/10.1007/s40201-025-00941-5","workflowStages":[]},"version":"v1","identity":"rs-4388377","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4388377","identity":"rs-4388377","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}