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The Study on the Change of Iron Concentration and the Reaction Mechanism of the 1,4-Dioxane Degradation using Zero Valent Iron and UV  

Son, Hyun-Seok (Institute of Health & Environment, Seoul National University)
Im, Jong-Kwon (Department of Environmental Health, Graduate School of Public Health, Seoul National University)
Zoh, Kyung-Duk (Department of Environmental Health, Graduate School of Public Health, Seoul National University)
Publication Information
Journal of Korean Society of Environmental Engineers / v.30, no.3, 2008 , pp. 323-330 More about this Journal
Abstract
The study presents the results of 1,4-dioxane degradation using zero valent (Fe$^0$) or Fe$^{2+}$ ions with and without UV. During the reaction, the change of [Fe$^{2+}$] and [Fe$^{2+}$]/[Fe(t)], the concentration ratio of ferrous ion to total iron ion in solution was measured. Less than 10% degradation of 1,4-dioxane was observed by UV-only, Fe$^0$-only, and Fe$^{2+}$-only conditions, and also the changes of [Fe$^{2+}$] and [Fe$^{2+}$]/[Fe(t)] were minimal in each reaction. However, the oxidation of Fe$^0$ was enhanced with the irradiation of UV by approximately 25% and the improvement of 1,4-dioxane degradation was observed. Fenton reaction ($Fe^{2+}+H_2O_2$) showed higher degradation efficiency of 1,4-dioxane until 90 min, which of the degradation was stopped after that time. In the reaction of Fe$^{2+}$ and UV, the ratio of [Fe$^{2+}$]/[Fe(t)] decreased then slowly increased after a certain time indicating the reduction of Fe3+ to Fe$^{2+}$. In case of Fe$^0$ in the presence of UV, the first-order rate constant was found to be 1.84$\times$10$^{-3}$ min$^{-1}$ until 90 min, and then changed to 9.33$\times$10$^{-3}$ min$^{-1}$ when the oxidation of Fe$^{2+}$ mainly occurred. In this case [Fe$^{2+}$]/[Fe(t)] kept decreasing for the reaction. However, the addition of perchlortae (ClO$_4^-$) in the reaction of Fe$^0$ and UV induced the continuous increase of [Fe$^{2+}$]/[Fe(t)] ratio. The results mean the primary degradation factor of 1,4-dioxane is the oxidation by the radicals generated from the redox reaction between Fe$^{2+}$ and Fe$^{3+}$. Also, both UV and ClO$_4^-$ played the role inducing the reduction of Fe$^{3+}$, which is important to degrade 1,4-dioxane by enhancing the generation of radicals.
Keywords
Fe$^0$; Fe$^{2+}$; [Fe$^{2+}$]/[Fe(t)]; 1,4-dioxane; ClO$_4^-$;
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1 Lesage, S., Jackson, R. E., Priddle, M. W., and Riemann, P. G., "Occurrence and fate of organic solvent residues in anoxic groundwater at the gloucester landfill," Environ. Sci. Technol., 24, 559-566(1990)   DOI
2 APHA, AWWA, and WEF, "Standard Methods for the examination of water and Wastewater: 20th Edition," APHA, 3.75-3.78(1998)
3 Pignatello, J. J., "Dark and photoassisted $Fe^{3+}$-catalyzed degradation of chlorophenoxy herbicides by hydrogen peroxide," Environ. Sci. Technol., 26(5), 944-951(1992)   DOI
4 박성호, 한인섭, "$Fe^{0}, Fe^{2+}, Fe^{3+}/H_{2}O_{2}$ 시스템을 이용한 침출수의 Fenton 산화반응," 대한환경공학회지, 27(4), 402-408(2005)
5 Walling, C. and Goosen, A., "Mechanism of the ferric ion catalyzed decomposition of hydrogen peroxide. Effect of organic substrates," J. Am. Chem. Soc., 95, 2987-2991(1973)   DOI
6 Tom, M., "GRA's 1,4-dioxane conference profiles national challenge of emerging and unregulated contaminants," in proceedings of the 2003 GRA's ninth symposium on groundwater contaminants focused 1,4-dioxane & other solvent stabilizer compounds in the environment, Groundwater Resource Association, San Jose, pp. 164-168(2003)
7 Chemical Safety Information from Intergovernmental Orgainzations Home Page, http://www.inchem.org/documents/iarc/vol71/019-dioxane.html, July(1999)
8 Rush, J. D., Bielski, B. H. J., "Pulse radiolytic studies of the reactions of $HO_{2}/O_{2}^{-}$ with Fe(II)/Fe(III) ions. The reactivity of $HO_{2}/O_{2}^{-}$ with ferric ions and its implication on the Haber-Weiss reaction," J. phys. Chem., 89, 5062-5066(1985)   DOI
9 Chen, F., He, J. J., and Zhao, J. C., "Fenton degradation of malachite green catalyzed by aromatic additives," J. Phys. Chem. A., 106(41), 9485-9490(2002)   DOI   ScienceOn
10 Wust, W. F., Kober, R., Schlicker, O., and Dahmke, A., "Combined zero- and First-order kinetic model of the degradadtion TCE and cis-DCE with commercial iron," Environ. Sci. Technol., 33, 4304-4309(1999)   DOI   ScienceOn
11 Arnold, W. and Roberts, A. L., "Pathway and kinetics of chllorinated Ethylene and chlorinated acetylene reaction with $Fe^{0}$ Particles," Environ. Sci. Technol., 34, 1794-1805(2000)   DOI   ScienceOn
12 Legrinl, O., Oliveros, E., and Braun, A. M., "Photochemical Processes for water treatment," Chem. Rev., 93, 671-698(1993)   DOI   ScienceOn
13 Mantha, R., Talyor, K. E., and Bewtra, J. K., "A Continuous system for $Fe^{0}$ reduction of nitrobenzene in synthetic Wastewater," Environ. Sci. Technol., 35, 3231-3236(2001)   DOI   ScienceOn
14 Moor, J. K., Doney, S. C., Glover, D. M., and Fung, I. Y., "Iron cycling and nutrient-limitation patteres in surface waters of world ocean," Deep-Sea Research II, 49, 493-507(2002)
15 U.S. Environmental Protection Agency homepage, http://www.epa.gov/iris/subst/1007.htm, February(2005)
16 Beckett, M. A., and Hua, I., "Elucidation of the 1,4-dioxane decomposition pathway at discrete ultrasonic frequencies," Environ. Sci. Technol., 34, 3944-3953(2000)   DOI   ScienceOn
17 Song, W., Ma, W., Ma, J., Chen, C., Zhao, J., Huang, Y., and Xu, Y., "Photochemical oscillation of Fe(II)/Fe(III) ratio induced by periodic flux of dissolved organic matter," Environ. Sci. Technol., 39, 3121-3127(2005)   DOI   ScienceOn
18 Wolff, J., "Perchlorate and the Thyroid Gland," Pharmacol. Rev., 50(1), 89-105(1998)   PUBMED
19 Renner, R., "High Levels of perchlorate found in US mothers' milk," Environ. Sci. Technol. A-Pages, 39(7), 144-145(2005)   DOI   ScienceOn
20 Mater, L., Rosa, E. V. C., Berto, J., Correa, A. X. R., Schwingel, P.R., and Radetski, C. M., "A simple methodology to evaluate influence of $H_{2}O_{2}$ and $Fe^{2+}$ concentrations on the mineralization and biodegradability of organic compounds in water and soil contaminated with crude petroleum," J. Hazard. Mater., 149, 379-386(2007)   DOI   ScienceOn
21 Budavari, S., "Merck Index. An encyclopedia of chemicals, drugs, and biological," 13th ed.; Merck and Co. Inc.: Rahway, NJ, pp. 1204-1210(2001)
22 Urbansky, E. T. and Schock, M. R., "Issues in managing the risks associated with Perchlorate in drinking water," J. Environ. Mange., 56, 79-95(1999)   DOI   ScienceOn
23 Devlin, J. F., Klausen, J., and Schwarzenbch, R. P., "Kinetics of nitroaromatic reduction on granular iron in recirculating bactch experiments," Environ. Sci. Technol., 32, 1941-1947(1998)   DOI   ScienceOn
24 Pignatello, J. J., "Dark and photoassisted $Fe^{3+}$-catalyzed degradation of chlorophenoxy herbicides by hydrogen peroxide," Environ. Sci. Technol., 26(5), 944-951(1992)   DOI
25 Lopes, L., de Laat, J., and Legube, B., "Charge Transfer of iron(III) monomeric and oligomeric aqua hydroxo complexes: Semiempirical investigation into photoactivity," Inorg. Chem., 41, 2505-2517(2002)   DOI   ScienceOn