Adsorption of Copper, Zinc and Nickel Ions from Single and Binary Metal Ion Mixtures on to Chicken Feathers
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1 849 Adsorption of Copper, Zinc and Nickel Ions from Single and Binary Metal Ion Mixtures on to Chicken Feathers Sameer Al-Asheh*, Fawzi Banat and Dheaya Al-Rousan Department of Chemical Engineering, Jordan University of Science and Technology, PO Box 3030, Irbid-22110, Jordan. (Received 5 April 2002; accepted 15 June 2002) INTRODUCTION ABSTRACT: Certain industries often produce mixtures of heavy metal ions in their waste products. Because of the nature of heavy metal ions and the adsorption process, such metal ions can compete with each other for the sorption sites on an adsorbent during adsorption processes. In the present work, binary systems composed of copper, zinc and nickel ions were selected as examples of heavy metal ion mixtures and tested via batch adsorption processes using chicken feathers as an adsorbent. The uptake of individual metal ions was depressed by the presence of another. Thus, the uptake of copper ions from an initial copper ion solution of 20 ppm concentration was reduced from mmol/g to ca mmol/g by the presence of a similar concentration of nickel ions. The Freundlich, Langmuir and Sips multi-component adsorption models were employed to predict the uptake of metal ions from binary metal ion solutions using constants obtained from adsorption isotherm models applied to single-solute systems. Agricultural and animal wastes have been used to remove heavy metal ions from wastewaters. These adsorbents have been developed as alternatives to activated carbon due to the cost of regenerating the latter. Although it is known that, because of its large surface area, activated carbon is characterized by a large sorption capacity towards many heavy metal ions, many of the newly developed adsorbents have also exhibited significant sorption capacities. Examples include the removal of Cu 2+ and Cd 2+ ions from aqueous solutions by seafood processing waste sludge (Lee et al. 2001), the removal of Hg 2+, Pb 2+, Cd 2+, Ni 2+ and Cu 2+ ions from industrial wastewater on the activated agricultural waste of coirpith (Kadirvelu et al. 2001) and the use of biowaste obtained from the fruit juice industry for the removal of Hg 2+, Pb 2+, Cd 2+, Cu 2+, Zn 2+ and Ni 2+ ions (Snthilkumaar et al. 2000). The removal of heavy metal ions from wastewaters is necessary because of their harmful effects to aquatic life. Consequently, their levels must be decreased to the lowest possible values accepted by environmental regulations. In a previous investigation (Banat and Al-Asheh 2000), chicken feathers were used for the adsorption of phenol from aqueous solutions. The selection of chicken feathers was based on their abundant availability. For example, the US poultry industry produces tonne cleaned and dried poultry feathers each week (Merka 1997) and, consequently, the waste arising as a by-product from this industry would pose a burden on the environment if it was not treated further or utilized in other industries. Syama et al. (1996) recognized the potential use of chicken feather waste as an adsorbent of precious heavy metal ions such as gold and platinum. *Author to whom all correspondence should be addressed. alasheh@just.edu.jo.
2 850 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No Adsorption studies for single-solute systems are well established with the experimental data being fitted quantitatively by various types of adsorption equations (Gabaldon et al. 2000; Eligwe et al. 1999; Jain and Ram 1997). However, data on the adsorption of heavy metal ions from multicomponent systems are less widespread. The present work is devoted to a study of the removal of heavy metal ions from binary metal ion solutions. This is important for assessing the degree of interference between metal ions during adsorption. The sorption behaviour of a bi-metal ion system involving iron(iii) and chromium(vi) on the biosorbent Chlorella vulgaris was examined by Aksu et al. (1997). These authors observed that the equilibrium uptakes of iron(iii) or chromium(vi) ions were reduced by the presence of increasing concentrations of other metal ions. Allen and Brown (1995) analyzed the single- and multi-component isotherms for copper, cadmium and zinc ion sorption on to lignite, which indicated the presence of a competitive uptake with the copper ion being adsorbed preferentially by the lignite from multi-component solutions. The results of Al-Asheh and Duvnjak (1998) for binary metal ion sorption by pine bark showed that the presence of one metal ion influenced, competed with or excluded the uptake of the other metal ion. Several isotherm models are available in the literature describing the sorption equilibrium of multi-component systems. These include the extended Langmuir model, the Sips model, the Freundlich model and the Ideal Adsorption Solution Theory (IAST) model. These models can be used either to fit the data for the multi-component isotherms or to predict the multi-component isotherms using the parameters for single-component isotherm models. In the present work, experimental data for the sorption of single metal ions such as copper, nickel and zinc as well as binary combinations of these three metal ions are presented. The extended Langmuir, Sips and Freundlich models were employed to predict the isotherms of the binary systems using the single isotherm parameters. MATERIALS AND METHODS Adsorbent Chicken feathers collected from poultry shops were washed several times with tap water and detergent, rinsed with distilled water and left to dry at room temperature. Thereafter, the chicken feathers were dried for 2 d in an oven at 70ºC to ensure complete dryness. An electrical cutter was employed to disintegrate the dried feathers before use. Batch adsorption experiments In this work, binary metal ion sorption tests were undertaken using chicken feathers. The three binary metal ion combinations employed were Zn 2+ Cu 2+, Zn 2+ Ni 2+ and Cu 2+ Ni 2+, respectively. Solutions of each metal ion at different initial concentrations were prepared from copper sulphate (CuSO 4 5H 2 O), zinc sulphate (ZnSO 4 7H 2 O) and nickel sulphate (NiSO 4 5H 2 O). All chemicals were of analytical grade (Sigma Chemical Company). Two of these metal ion solutions were mixed at different ratios to prepare binary metal ion solutions of different concentrations. A known amount of chicken feathers was then added to these solutions to make the final sorbent concentration equal to 5 mg/ml. The mixtures were agitated using a shaker (Kottermann, Germany) until equilibrium was attained. The system was then filtered and the supernatant analyzed for both metal ions in the solution using an atomic absorption spectrophotometer (Spectra AA10, Varian, Germany). The kinetic data obtained showed that the copper, zinc and nickel ion contents levelled off after exposure for 6 h to the chicken feathers used, indicating the attainment of adsorption equilibrium.
3 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 851 However, to ensure complete achievement of adsorption equilibrium, such contact was extended to 24 h. The experiments were carried out at 25 ± 1ºC. No adsorption or precipitation of metal ions on the walls of the bottles used was observed under the experimental conditions employed. This was demonstrated by testing samples of the metal ion solutions in the absence of adsorbent. After filtration, it was found that the metal concentrations were the same both before and after filtration. Experiments were carried out in duplicate with the mean data being presented here. EQUILIBRIUM ISOTHERM MODELS Freundlich isotherm model As with all isotherm models, the Freundlich isotherm describes the relationship between the sorbate concentration in the solution, C e (mmol/l), and that adsorbed by the sorbent, q e (mmol/g), at equilibrium. The model may be expressed by the equation: q e = k F C e l/n (1) where k F [mmol 1 l/n l l/n )/g] and l/n (dimensionless) represent the Freundlich coefficients. The value of k F is related to the sorption capacity, while the value of l/n is related to the sorption intensity. Most data are represented by the linearized form of the Freundlich equation which may be written as: 1 ln q e = ln k F + ln C e (2) n According to equation (2), a plot of ln q e versus ln C e should be linear with the intercept and slope of the same being ln k F and l/n, respectively. The Freundlich model can be extended to describe a multi-component adsorption process, the following being the Freundlich representation for a binary equilibrium system (Do 1998): where æ k 1 ö 1/n 1 n ç C 1 è n 1 ø q 1 = + DF 2 (3) éæ k 1 ö 1/n 1 æ k 2 ö 1/n 2 ù 1 n êç C 1 + ç C 2 ú ëè n 1 ø è n 2 ø û æ k 1 ö 1/n 1 æ k 2 ö 1/n 2 ç C 1 ç C 2 è n é æ k 1 ö 1/n 1 æ k 2 ö 1/n 2 1 ø è n 2 ø ù DF 2 = (n 1 n 2 ) ln ê ç C 1 ç C 2 ú (4) é æ k 1 ö 1/n 1 æ k 2 ö 1/n 2 ù 2 n ë è n ø è n ø û 1 2 ê ç C 1 + ç C 2 ú ë è n 1 ø è n 2 ø û
4 852 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No æ k 1 ö 1/n 1 æ k 2 ö 1/n 2 n 1 ç C 1 + n 2 ç C 2 è n 1 ø è n 2 ø n = (5) æ k 1 ö 1/n 1 æk 2 ö 1/n 2 ç C 1 + ç C 2 è n 1 ø èn 2 ø with q 1 being the uptake of sorbate 1 by the sorbent and the variables C 1 and C 2 referring to the equilibrium concentration of sorbate 1 and sorbate 2, respectively. The constants k 1, k 2, n 1 and n 2 are the Freundlich constants obtained from the single-solute adsorption isotherm using the same sorbent. Langmuir isotherm model The Langmuir model has been used to describe both physical and chemical adsorption. It assumes monolayer coverage of solute on the sorbent. The model can be expressed by the equation: q m bc e qe = (6) 1 + bc e where q m and b are the Langmuir constants, related to the maximum adsorption capacity of the sorbent and to the energy of adsorption, respectively. The linearized form of the Langmuir model is given by: 1 æ 1 ö æ 1 ö 1 = ç + ç (7) q e è q m ø è bk L ø C e The constants q m and b can be evaluated from the respective intercept and slope of the linear plot of l/q e versus l/c e. The Langmuir model can also be extended to describe multi-component systems. In this case, the model can be written as: qi = q m,i b i C i (8) N 1 + S b k C k = 1 k where q i is the uptake of component i in the multi-component system and C k (k = 1,2...N; N being the number of components) is the equilibrium concentration of each component in the system. The quantities q m,i and b i are the Langmuir constants for species i as obtained from the single-solute isotherm model. Sips isotherm model The Sips model is an empirical model used to describe the relationship between the uptake of solute by the sorbent and the equilibrium concentration of solute in solution. This model is a combination of the Langmuir and Freundlich isotherm models. It contains three parameters and has the following mathematical representation:
5 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 853 K S (bc) 1/n q = (9) 1 + (bc) 1/n The Sips model can also be extended to describe multi-component adsorption systems. The multi-component Sips model can be written as: æ N ö 1/n i 1 K Si b i C i ç S b k C k è k = 1 ø q i = (10) æ N 1 + ç S b k C k è k = 1 ø ö 1/n i In this equation K Si, n i and b i are the single-solute Sips model constants for solute i as obtained from equation (9). It is important to point out that even if the single-solute sorption data are well represented by a particular single isotherm model, this does not necessarily imply that the corresponding multi-component model will give a good representation of the multi-component metal sorption data (Do 1998). RESULTS AND DISCUSSION Single metal ion sorption The sorption of copper, zinc and nickel as single metal ions by chicken feathers was studied at different initial metal ion concentrations ( ppm) and then compared to the sorption of the same metal ion from aqueous binary metal ion solutions. The sorption of each of the three individual metal ions is depicted in Figure 1. The data were fitted to the Langmuir, Freundlich and Sips isotherm models using Microcal Origin Software (Version 4.10). It is seen that all of the models provided a good representation of the data. The constants for these models are listed in Table 1. From the values of q m and k F given in Table 1, the affinity of chicken feathers towards the sorption of the metal ions concerned followed the order: Cu 2+ > Zn 2+ > Ni 2+. These results are comparable or superior to others available in the literature for other sorbents. Thus, for example, the maximum sorption capacities for copper, zinc and nickel ions by chicken feathers were 17.37, 9.28 and 7.42 mg/g, respectively (Table 1), while their corresponding maximum sorption capacities by rice bran were 8.24, 9.37 and 5.28 mg/g, respectively (Marshall et al. 1993). Binary metal ion sorption The following combinations of metal ions were studied as binary systems: Cu 2+ Zn 2+, Cu 2+ Ni 2+, Zn 2+ Ni 2+. The binary data were obtained via batch equilibrium experiments, the concentration of each metal ion being varied in the range ppm. The chicken feather concentration in the metal ion sorbent suspensions was fixed at 5 mg/ml. The results obtained are presented in Tables 2 4. It is obvious from the data listed that the uptake of any metal ion in the binary systems was less than that in the single-solute systems for all metal ion combinations studied. This is clearly demonstrated by the sorption capacity ratio, which may
6 854 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No Figure 1. Experimental data (symbols) and predicted curve fits (, Langmuir; -----, Freundlich;, Sips) for the individual equilibrium isotherms of (a) Cu 2+, (b) Ni 2+ and (c) Zn 2+ ions on to chicken feathers (5 mg/ml concentration).
7 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 855 TABLE 1. Parameters for the Different Isotherm Models Studied for the Sorption of Single Metal Ions on Chicken Feathers a Metal Langmuir model constants Freundlich model constants Sips model constants ion q m b R 2 k F n R 2 k S b n R 2 (mmol/g) (l/mol) Cu Zn Ni a Chicken feather conc. = 5 mg/ml. TABLE 2. Sorption Capacity Ratio for Copper and Zinc Ions by Chicken Feathers a in the Cu 2+ Zn 2+ Binary System at Different Initial Copper and Zinc Ion Concentrations Initial Zn 2+ ion Initial Cu 2+ ion q Zn 2+/q Zn0 2+ q Cu 2+/q Cu0 2+ conc., C 0 (ppm) conc., C 0 (ppm) a Chicken feather conc. = 5 mg/ml.
8 856 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No TABLE 3. Sorption Capacity Ratio for Copper and Nickel Ions by Chicken Feathers a in the Cu 2+ Ni 2+ Binary System at Different Initial Copper and Nickel Ion Concentrations Initial Ni 2+ ion Initial Cu 2+ ion q Ni 2+/q Ni0 2+ q Cu 2+/q Cu0 2+ conc., C 0 (ppm) conc., C 0 (ppm) a Chicken feather conc. = 5 mg/ml. be defined as the ratio of the sorption capacity for one metal ion in the presence of other metal ions, q mix, to the sorption capacity for the same metal ion when alone in solution, q 0. Based on such sorption capacities, it may be stated: q mix 1. When > 1, sorption will be promoted by the presence of other metal ions. q 0 q mix 2. When = 1, no net interaction effect is observed. q 0 q mix 3. When < 1, sorption will be suppressed by the presence of other metal ions. q 0
9 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 857 TABLE 4. Sorption Capacity Ratio for Zinc and Nickel Ions by Chicken Feathers a in the Zn 2+ Ni 2+ Binary System at Different Initial Zinc and Nickel Ion Concentrations Initial Zn 2+ ion Initial Ni 2+ ion q Zn 2+/q Zn0 2+ q Ni 2+/q Ni0 2+ conc., C 0 (ppm) conc., C 0 (ppm) a Chicken feather conc. = 5 mg/ml. From the data in Tables 2 4, it will be seen that in most cases the sorption of one metal ion was suppressed by the presence of the other. The sorption behaviour of each binary system will be discussed individually below. Cu 2+ Zn 2+ binary sorption system The data obtained for the sorption of copper and zinc ions in the two Cu 2+ Zn 2+ binary systems studied are presented in Figure 2(a) and (b) for copper ion and zinc ion adsorption, respectively. Each curve in these figures was plotted by maintaining the initial concentration of one metal ion constant and varying the concentration of the other. It is apparent from the data depicted that the uptake of each metal ion in the binary system was always less than that observed for single metal ion sorption. The level of such depression in the sorption extent of each metal ion increased as the concentration of the other metal ion in the system increased. This may be attributed to competition
10 858 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No Figure 2. Isotherms of (a) Cu 2+ and (b) Zn 2+ ions in Cu 2+ Zn 2+ ion solutions at different Zn 2+ and Cu 2+ ion concentrations, respectively, using 5 mg/ml chicken feathers. Data points: (a), 0 ppm Zn 2+ ;, 20 ppm Zn 2+ ; D, 40 ppm Zn 2+ ; Ñ, 60 ppm Zn 2+ ; {, 80 ppm Zn 2+ ; +, 100 ppm Zn 2+ : (b), 0 ppm Cu 2+ ;, 20 ppm Cu 2+ ; D, 40 ppm Cu 2+ ; Ñ, 60 ppm Cu 2+ ; {, 80 ppm Cu 2+ ; +, 100 ppm Cu 2+.
11 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 859 Figure 3. Predictions of binary equilibrium data for Cu 2+ Zn 2+ using single-solute isotherm parameters. Symbols represent experimental data and lines represent different isotherm models:, Langmuir; -----, Sips;, Freundlich. between zinc and copper ions for the sites available for sorption on the sorbent surface. It may also be concluded from Figure 2 that the presence of copper ions in the solution had a stronger effect on zinc ion sorption than vice versa. This may be related to the higher electronegativity of the copper ion relative to that for the zinc ion. The data depicted in Figure 2(a) and (b) may also be represented as a plot of the mole fraction present in the solid phase (Y) versus the mole fraction present in the liquid phase (X). Such a plot is depicted in Figure 3. This figure also includes predictions of the binary isotherm data using the Langmuir, Freundlich and Sips models, employing parameters obtained from single-solute isotherm experiments. Comparison between the model predictions and the experimental data based on the sum of the square of residuals SSR (Table 5) indicates that the Freundlich model provided a better representation of the data than the other models, with the Langmuir model being the worst. TABLE 5. SSR Values of the Predicted Freundlich, Langmuir and Sips Models for the Three Binary Systems Investigated Model Cu 2+ Zn 2+ Cu 2+ Ni 2+ Zn 2+ Ni 2+ Freundlich Sips Langmuir
12 860 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No Figure 4. Isotherms of (a) Cu 2+ and (b) Ni 2+ ions in Cu 2+ Ni 2+ ion solutions at different Ni 2+ and Cu 2+ ion concentrations, respectively, using 5 mg/ml chicken feathers. Data points: (a), 0 ppm Ni 2+ ;, 20 ppm Ni 2+ ; D, 40 ppm Ni 2+ ; Ñ, 60 ppm Ni 2+ ; {, 80 ppm Ni 2+ ; +, 100 ppm Ni 2+ : (b), 0 ppm Cu 2+ ;, 20 ppm Cu 2+ ; D, 40 ppm Cu 2+ ; Ñ, 60 ppm Cu 2+ ; {, 80 ppm Cu 2+ ; +, 100 ppm Cu 2+.
13 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 861 Figure 5. Predictions of binary equilibrium data for Cu 2+ Ni 2+ system using single-solute isotherm parameters. Symbols represent experimental data and lines represent different isotherm models:, Langmuir; -----, Sips;, Freundlich. Cu 2+ Ni 2+ binary sorption system The copper and nickel ion uptakes in the Cu 2+ Ni 2+ binary system both decreased as the concentration of the other metal ion in the system increased (Figure 4). Explanations for this behaviour are similar to those given above for the Cu 2+ Zn 2+ system. The presence of the nickel ion had a stronger effect on the copper ion uptake than the presence of the zinc ion [compare the data in Figures 4(a) and 2(a)]. This may be attributed to the fact that both the nickel ion and the copper ion have a similar electronegativity. A presentation of the data in terms of mole fractions in the solid and liquid phases is shown in Figure 5. This figure also shows the Langmuir, Freundlich and Sips predictions of the binary isotherm data using parameters taken from the single-solute isotherm data. A comparison based on SSR values (Table 5) between the predicted nickel ion uptakes by the different isotherm models relative to the experimental data showed that the Freundlich model was again best at describing the experimental data for the binary system whilst the Langmuir model again provided the worst prediction.
14 862 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No Figure 6. Isotherms of (a) Ni 2+ and (b) Zn 2+ ions in Ni 2+ Zn 2+ ion solutions at different Zn 2+ and Ni 2+ ion concentrations, respectively, using 5 mg/ml chicken feathers. Data points: (a), 0 ppm Zn 2+ ;, 20 ppm Zn 2+ ; D, 40 ppm Zn 2+ ; Ñ, 60 ppm Zn 2+ ; {, 80 ppm Zn 2+ ; +, 100 ppm Ni 2+ : (b), 0 ppm Ni 2+ ;, 20 ppm Ni 2+ ; D, 40 ppm Ni 2+ ; Ñ, 60 ppm Ni 2+ ; {, 80 ppm Ni 2+ ; +, 100 ppm Ni 2+.
15 Adsorption on to Chicken Feathers from Single and Binary Metal Ion Mixtures 863 Figure 7. Predictions of binary equilibrium data for Ni 2+ Zn 2+ system using single-solute isotherm parameters. Symbols represent experimental data and lines represent different isotherm models:, Langmuir; -----, Sips;, Freundlich. Zn 2+ Ni 2+ binary sorption system The sorption isotherms of zinc and nickel ions in their binary solutions were also considered. The results depicted in Figure 6(a) demonstrate that the nickel ion uptake decreased as the zinc ion concentration in the system increased. Similarly, the zinc ion uptake decreased as the nickel ion concentration increased [Figure 6(b)]. The mole fraction presentation of the data is displayed in Figure 7. As indicated in Table 5, the Freundlich model again provided the best description of the experimental data while the Langmuir model was once more the worst. Banat et al. (2002) have also investigated the predictions for the same three binary systems, i.e. Cu 2+ Zn 2+, Cu 2+ Ni 2+, Zn 2+ Ni 2+, using four multi-component isotherm models, viz, the Freundlich, Langmuir, Sips and Ideal Adsorption Solution Theory (IAST) whilst employing the parameters for the single-solute isotherm equations. They found that all the models investigated showed good agreement with experimental data except for the Langmuir isotherm. This is consistent with the results obtained in the present work. CONCLUSIONS The following conclusions may be drawn from the work undertaken: (a) The affinity of chicken feathers towards the sorption of metal ions from the individual metal ion solutions followed the order Cu 2+ > Zn 2+ > Ni 2+.
16 864 Sameer Al-Asheh et al./adsorption Science & Technology Vol. 20 No (b) The uptake of Cu 2+, Zn 2+ and Ni 2+ ions from the various binary solutions studied was less than that from the single-solute solutions. (c) The uptake of a given metal ion from a binary system diminished as the concentration of the other metal ion increased. (d) The Freundlich model for multi-component systems provided a better representation of the experimental data than the other models studied in this work. REFERENCES Aksu, Z., Ackel, U. and Tulin, K. (1997) J. Chem. Biochem. Biotechnol. 70, 368. Al-Asheh, S. and Duvnjak, Z. (1998) Sep. Sci. Technol. 33, 685. Allen, S. and Brown, P. (1995) J. Chem. Biochem. Biotechnol. 61, 17. Banat, F. and Al-Asheh, S. (2000) Environ. Eng. Policy 2, 85. Banat, F., Al-Asheh, S. and Mohai, F. (2002) Sep. Sci. Technol. 37, 311. Do, D.D. (1998) Adsorption Analysis: Equilibria and Kinetics, Vol. 2, Imperial College Press, London, UK, pp Eligwe, C.A., Okolue, N.B., Nwambu, C.O. and Nwoko, C.I.A. (1999) Chem. Eng. Technol. 22, 45. Gabaldon, C., Marzal, P., Seco, A. and Gonzalez, J.A. (2000) Sep. Sci. Technol. 35, Jain, C.K. and Ram, D. (1997) Water Res. 31, 154. Kadirvelu, K., Thamaraiselvi, K. and Namasivayam, C. (2001) Bioresearch Technol. 76, 63. Lee, S., Davis, M. and Allen, P. (2001) Water Res. 35, 534. Marshall, W.E., Champagne, E.T. and Evans, W.J. (1993) J. Environ. Sci. Health 28, Merka, W.C. (1997) Poultry tips, Snthilkumaar, S., Bharathi, S., Nithyanandhi, D. and Subburam, V. (2000) Bioresearch Technol. 75, 163. Syama, K., Fukazaua, Y. and Suzumura, H. (1996) Appl. Biochem. Biotechnol. 57, 58.
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