Effect of Humic Acid on the Selenite Adsorption onto Hematite

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1 Effect of Humic Acid on the Selenite Adsorption onto Hematite MYOUNG-JIN KIM, MIJEONG JANG, and SE YOUNG PAK Department of Environmental Engineering Korea Maritime University 1, Dongsam-dong, Yeongdo-gu, Busan KOREA Abstract: - In the present study, we investigated the adsorption of selenite [Se(Ⅳ)] onto hematite, which usually exists in soils and rocks, focusing on the effect of humic acid. The selenite adsorption onto hematite varied with the contact time, finally reaching an equilibrium state in 5 hours. The result was in good agreement with the Parabolic diffusion equation (R 2 = 0.97). The adsorption with different initial selenium concentrations was reproduced fairly with a Langmuir isotherm (R 2 = 0.92). The adsorption efficiency of selenite increased with decreasing ph. It increased with increasing ionic strength. Freundlich isotherm successfully described the partition behavior between humic acid and hematite (R 2 = 0.95). In the presence of humic acid (selenite-hematite-humic acid ternary system), the adsorption of selenite onto hematite increased at high ph, but decreased at low ph. The amount of selenite adsorbed on hematite decreased with the concentration of humic acid, and then saturated above 50 mg/l. Key-Words: - Selenium, Selenite, Adsorption, Hematite, Humic Acid, ph, Ionic Strength 1 Introduction Selenium (Se) is an essential element for human and animal, however, excessive intake of Se may cause severe reverse effect such as poisoning. Some works can be found in the literature concerning the adsorption of selenium on iron oxy-hydroxides such as goethite, magnetite, and hematite [1-4]. Competition between metal and other adsorbate for mineral surface has been studied [5-8]. The effect of organic acids on the adsorption of metal onto mineral surfaces has been known to be a complex function of the system components, the molar ratio of the components, and in some instances, the sequence in which components are added [7]. In general, metal adsorption in the presence of organic ligands increased at low ph and decreased at high ph values [7]. Even though a lot of studies of metal adsorption onto mineral surfaces in the presence of organic acids have been conducted, the role of natural organic matter in the selenium adsorption onto hematite is relatively poorly understood [8]. In this study, the effects of reaction time, adsorbate/adsorbent ratio, ph, and ionic strength on the adsorption of selenite onto hematite were investigated. In addition, we focused on the effect of humic acid on the adsorption reaction. 2 Materials and Methods Hematite was synthesized using the method of Sugimoto et al. [9]. The solution of selenite was prepared by dissolving Na 2 SeO 3 into deionized water. Humic acid was purchased from Sigma-Aldrich and was used without further purification. The temperature was 25± Selenite-hematite binary system Kinetics The experiments of adsorption kinetics were conducted for 50µM selenite solution at ph 5.5±0.2. Synthesized hematite (0.08g) and each selenite solution (50 ml) were placed into nine 125 ml Erlenmeyer flasks. Then, 9 flasks were shaken using a platform shaker (225 rpm). One flask was removed from the shaker after each of the time intervals (5min, 10min, 30min, 1h, 3h, 5h, 10h, 24h, and 48h). Then, the phs of suspended mixture were measured. The final ph was considered as the experimental ph value. After filtering the suspended mixture using a 0.45 µm ISBN:

2 membrane filter, the selenium concentration in the filtrate was determined by an ICP-AES Adsorption isotherms Adsorption isotherms of selenite on hematite were obtained at ph 5.5±0.2. A total of 9 initial selenite solution concentrations were prepared to obtain the adsorption equilibrium: 10, 25, 50, 75, 100, 150, 200, 300, 400 µm. Synthesized hematite (0.08g) and each selenite solution (50 ml) were placed into a 125 ml Erlenmeyer flask, and the suspension was shaken for 24 hours. The rest of the experiments were conducted using the same experimental method as mentioned previously Adsorption envelopes The effect of ph on the selenite adsorption was investigated over a ph range from 4.5 to 11.5 at two ionic strengths. Each set of adsorption suspensions contained constant initial selenite concentration (50µM). The ionic strength was adjusted using background electrolyte concentrations of 0 and 0.01M NaCl. The ph of the selenite solution was adjusted using HCl or NaOH. For all experiments, suspensions were shaken for 24 hours. The rest of the experiments were conducted using the same experimental method as mentioned previously. 2.2 Humic acid-hematite binary system Adsorption isotherms of humic acid on hematite were obtained at ph 5.5±0.2. A total of 7 initial humic acid solution concentrations were prepared to obtain the adsorption equilibrium: 25, 50, 100, 150, 200, 300, 500 mg/l. Synthesized hematite (0.08g) and each humic acid solution (50 ml) were placed into a 125 ml Erlenmeyer flask, and the suspension was shaken for 24 hours. The rest of the experiments were conducted using the same experimental method as mentioned previously. Humic acid concentrations in the solution were determined by a total organic carbon analyzer. three concentrations of humic acid (0, 10, and 100 mg/l). Each set of adsorption suspensions contained constant initial selenite concentration (50µM). More experiments were conducted to investigate the effect of humic acid in detail. In the experiments, selenite concentration (50µM) and hematite mass (0.08g) were fixed, but humic acid concentrations were changed like 5, 10, 25, 50, 100, 200, and 300 mg/l. For all experiments, suspensions were shaken for 24 hours. The rest of the experiments were conducted using the same experimental method as mentioned previously. 3 Results and Discussion 3.1 Selenite-hematite binary system Kinetics The results of adsorption kinetics are shown in Figure 1. The adsorption equilibrium was achieved after 5 hours of reaction. The rate of adsorption increased sharply for the first 1 hour, then reached semi-equilibrium after about 3 hours, and finally reached an equilibrium state after about 5 hours.therefore, all further adsorption procedures were performed for 24 hours, which is long enough to reach equilibrium. The result is in good agreement with the Parabolic diffusion equation (R 2 = 0.97). 2.3 Selenite-hemaite-humic acid ternary system Ternary system experiments were performed in the same manner as the binary experiments. The effect of humic acid on the selenite adsorption onto hematite was investigated over a ph range from 4.5 to 11.5 at Fig. 1. Kinetics of 50µM Se(IV) adsorption on hematite at ph 5.5± Adsorption isotherms ISBN:

3 The results of adsorption isotherms are shown in Figure 2. The adsorption with different initial selenium concentrations was reproduced fairly with a Langmuir isotherm (R 2 = 0.92). Fig. 3. Adsorption envelopes of Se(IV) for hematite in initial 50µM Se(IV) concentration at two ionic strengths. 3.2 Humic acid-hematite binary system The results of adsorption isotherms are shown in Figure 4. Isotherm shows that the amount of adsorbed humic acid increased with the humic acid concentration of equilibrium solution. Freundlich isotherm successfully describe the partition behavior between humic acid and hematite (R 2 = 0.95). Fig. 2. Adsorption isotherm of Se(IV) for hematite at ph 5.5± Adsorption envelopes The adsorption of selenite obtained in the examined ph range is shown in Figure 3. The adsorption efficiency of selenite increased with decreasing ph. It also increased with increasing ionic strength. The present results were similar to those observed in previous studies: high (low) adsorption at low (high) ph [2, 3]. The lower adsorption of selenite at higher ph value is attributable to an increased repulsion between the more negatively charged selenite species and negatively charged surface sites. Fig. 4. Adsorption isotherm of humic acid for hematite at ph 5.5± Selenite-hematite-humic acid ternary system The effect of ph on the adsorption of selenite was evaluated in the ph range of at three humic acid concentrations. The wide ph range was selected to obtain equilibrium solutions with various selenite and humic acid species. The charge of hematite surface would be changed depending on the ph of suspension. The adsorption efficiencies of selenite on hematite in ternary system (Se-hematite-humic acid) were lower than those in binary system (Se-hematite) at low ph (ph<8) (Fig. 5). However, at high ph (ph>9), the results showed the opposite trend. Humic acid inhibited the selenite adsorption onto hematite at low ph, and helped the reaction at high ph. The amount of selenite adsorbed on hematite decreased with the concentration of humic acid, and then saturated above 50 mg/l. It could be explained by ISBN:

4 the competition effect for the surface sites of hematite between selenite and humic acid (Fig. 6). environment and to remove selenium. In addition, it would provide an important basic reference in the field of geochemistry of metal oxyanions. Acknowledgement:- This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MEST) (No ). Fig. 5. Effect of humic acid on the Se(IV) adsorption onto hematite at various phs. Fig. 6. Change of amount of adsorbed Se(IV) according to increasing humic acid concentration 4 Conclusion The adsorption of selenite on hematite strongly depended on all the parameters: higher adsorption at lower ph and/or higher ionic strength. It was observed that ph was a very strong factor in immobilization of selenite onto hematite by adsorption. In addition, it was found that humic acid considerably inhibited the selenite adsorption onto hematite at low ph. Results obtained through this study would be helpful to understand the fate and transport of Se in natural References: [1] Y.T. Chan, W.H. Kuan, T.Y. Chen and M.K. Wang, Adsorption mechanism of selenate and selenite on the binary oxide systems, Water Research, Vol. 43, 2009, pp [2] M. Duc, G. Lefèvre and M. Fédoroff, Sorption of selenite, Journal of Colloid and Interface Science, Vol. 298, 2006, pp [3] M. Duc, G. Lefevre, M. Fedoroff, J. Jeanjean, J.C. Rouchaud, F. Monteil-Rivera, J. Dumonceau and S. Milonjic, Sorption of selenium anionic species on apatites and iron oxides from aqueous solutions, Journal of Environmental Radioactivity, Vol. 70, 2003, [4] M. Rovira, J. Giménez, M. Martínez, X. Martínez-Lladó, J. Pablo, V. Martí and L. Duro, Sorption of selenium(iv) and selenium(vi) onto natural iron oxides: Goethite and hematite, Journal of Hazardous Materials, Vol. 150, 2008, pp [5] N. Jordan, N. Marmier, C. Lomenech, E. Giffaut and J.J. Ehrhardt, Competition between selenium (IV) and silicic acid on the hematite surface, Chemosphere, Vol. 75, 2009, pp [6] I. Ko, A.P. Davis, J.Y. Kim and K.W. Kim, Effect of contact order on the adsorption of inorganic arsenic species onto hematite in the presence of humic acid, Journal of Hazardous Materials, Vol. 141, 2007, pp [7] J.J. Lenhart, B.D. Honeyman, Uranium(VI) sorption to hematite in the presence of humic acid, Geochimica et Cosmochimica Acta, Vol. 63, 1999, pp [8] R.J. Murphy, J.J. Lenhart and B.D. Honeyman, The sorption of thorium (IV) and uranium (VI) to hematite in the presence of natural organic matter, Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 157, 1999, pp [9] T. Sugimoto, K. Sakata and A. Muramatsu, Formation mechanism of monodisperse ISBN:

5 pseudocubic α-hematite particles from condensed ferric hydroxide gel, Journal of Colloid and Interface Science, Vol. 159, 1992, pp ISBN:

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