Sự hình thành của Aldehydes và Axit Carboxylic trong quá trình Ozon hóa Axit Humic

Xin Zhong1, Chongwei Cui1,2, Shuili Yu3
1School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, China
2Harbin City, China
3School of Environmental Science and Engineering, Tongji University, Shanghai, China

Tóm tắt

Mục đích của nghiên cứu này là xác định các loại và nồng độ khác nhau của các chất trung gian, đồng thời điều tra ảnh hưởng của thời gian tiếp xúc và liều lượng ozon (O3) đối với việc loại bỏ axit humic (HA), được coi là chất tiền chất chính của các sản phẩm phụ khử trùng (DBP). Dựa trên đó, khoảng trống kiến thức về DBP được tạo ra. Kết quả cho thấy HA là vật liệu tiền chất chính cho aldehyde và axit carboxylic. Nồng độ aldehyde tăng lên khi thời gian tiếp xúc và liều lượng O3 tăng, đạt mức tối đa ở khoảng 2~10 phút nhưng trở nên ổn định ở liều lượng O3 cao hơn. Nồng độ axit formic và axit acetic cũng tăng lên tương ứng với thời gian tiếp xúc và liều lượng O3. Tuy nhiên, các axit thơm, bao gồm axit protocatechuic, axit 3-hydroxybenzoic, và axit benzoic, giảm nhanh chóng khi thời gian phản ứng dài hơn và liều lượng O3 cao hơn. Đáng chú ý là các axit thơm hiếm khi được báo cáo. Bên cạnh đó, một con đường hình thành có thể xảy ra được đề xuất: (a) HA bị phân hủy thành các hợp chất giống axit fulvic (FA); (b) Các hợp chất giống FA tiếp tục chuyển đổi thành các axit thơm; (c) Các axit thơm sẽ biến đổi thành các chất hữu cơ có trọng lượng phân tử thấp; (d) Clo phản ứng với aldehyde và/hoặc axit carboxylic thông qua các phản ứng cộng, thủy phân và khử carbonyl, dẫn đến sự hình thành DBP. Hơn nữa, không chỉ HA là các tiền chất chính của DBP, mà các chất trung gian oxy hóa của HA cũng có thể là các tiền chất DBP, và chúng đã tạo ra một lượng nhất định của DBP. Do đó, aldehyde và axit carboxylic cần được kiểm soát trong các nhà máy xử lý nước uống.

Từ khóa

#Axit humic #sản phẩm phụ khử trùng #ozon hóa #aldehyde #axit carboxylic

Tài liệu tham khảo

Chiang, P., Chang, E. E., Chang, P., & Huang, C. (2009). Effects of pre-ozonation on the removal of THM precursors by coagulation. Science of the Total Environment, 407, 5735–5742. Dąbrowska, A., Hordern, B. K., & Nawrocki, J. (2005). Aldehydes formation during water disinfection by ozonation and chlorination process. Global NEST, 7, 61–71. Dąbrowska, A., & Nawrocki, J. (2013). Aldehyde concentrations in wet deposition and river waters. Science of the Total Environment, 452-453, 1–9. EFA (U.S. Environmental protection Agency) (1998). Method 556: determinantion of carbonyl compounds in drinking water by pentafluorobenzylhydroxylamine derivatization and capillary gas chromatography with electron capture detection. EFA (U.S. Environmental protection Agency) (1995). Method 552.2: determinantion of haloacetic acids and dalapon in drinking water by liquid-liquid extraction, derivatization and gas chromatography with electron capture detection. Gaffney, J. S., Marley, N. A., & Clark, S. B. (1996). Humic and fulvic acids and organic colloidal materials in the environment (pp. 2–17). Chicago: American Chemical Society national meeting. Gunten, U. V. (2003). Ozonation of drinking water: part I. Oxidation kinetics and product formation. Water Research, 37, 1443–1467. Gunten, U. V., & Ramseier, M. K. (2009). Mechanisms of phenol ozonation-kinetics of formation of primary and secondary reaction products. Ozone: Science and Engineering, 31, 201–215. Hammes, F., Salhi, E., Köster, O., Kaiser, H., Egli, T., & von Gunten, U. (2006). Mechanistic and kinetic evaluation of organic disinfection by-product and assimilable organic carbon (AOC) formation during the ozonation of drinking water. Water Research, 40, 2275–2286. He, R., Tian, B., Zhang, Q., & Zhang, H. (2015). Effect of Fenton oxidation on biodegradability, biotoxicity and dissolved organic matter distribution of concentrated landfill leachate derived from a membrane process. Waste Management, 38, 232–239. Hu, R., Zhang, L., & Hu, J. (2016). Study on the kinetics and transformation products of salicylic acid in water via ozonation. Chemosphere, 153, 394–404. Hua, G., & Reckhow, D. A. (2013). Effect of pre-ozonation on the formation and speciation of DBPs. Water Research, 47, 4322–4330. Huang, W., Fang, G., & Wang, C. (2005). The determination and fate of disinfection by-products from ozonation of polluted raw water. Science of the Total Environment, 345, 261–272. McGwin Jr., G., Lienert, J., & Kennedy Jr., J. I. (2010). Formaldehyde exposure and asthma in children: a systematic review. Environmental Health Perspectives, 118, 3845–3852. Leenheer, J. A., & Croué, J. P. (2003). Peer reviewed: characterizing aquatic dissolved organic matter. Environmental Science & Technology, 37, 18A–26A. Liu, C., Tang, X., Kim, J., & Korshin, G. V. (2015). Formation of aldehydes and carboxylic acids in ozonated surface water and wastewater: a clear relationship with fluorescence changes. Chemosphere, 125, 182–190. Mao, Y., Wang, X., Yang, H., Wang, H., & Xie, Y. F. (2014). Effects of ozonation on disinfection byproduct formation and speciation during subsequent chlorination. Chemosphere, 117, 515–520. Matilainen, A., & Sillanpää, M. (2010). Removal of natural organic matter from drinking water by advanced oxidation processes. Chemosphere, 80, 351–365. Miao, H., & Tao, W. (2008). Ozonation of humic acid in water. Journal of Chemical Technology and Biotechnology, 83, 336–344. Nawrocki, J., Swietlik, J., Raczyk-Stanisawiak, U., Dabrowska, A., Bilozor, S., & Ilecki, W. (2003). Influence of ozonation conditions on aldehyde and carboxylic acid formation. Ozone: Science & Engineering, 25, 53–63. Papageorgiou, A., Stylianou, S. K., Kaffes, P., Zouboulis, A. I., & Vouts, D. (2017). Effects of ozonation pretreatment on natural organic matter and wastewater derived organic matter-possible implications on the formation of ozonation by-products. Chemosphere, 170, 33–40. Papageorgiou, A., Voutsa, D., & Papadakis, N. (2014). Occurrence and fate of ozonation by-products at a full-scale drinking water treatment plant. Science of the Total Environment, 481, 392–400. Ratpukdi, T., Siripattanakul, S., & Khan, E. (2010). Mineralization and biodegradability enhancement of natural organic matter by ozonee VUV in comparison with ozone, VUV, ozone-UV, and UV: effects of pH and ozone dose. Water Research, 44, 3531–3543. Richadrson, S., Plewa, M., Wagner, E., Schoeny, R., & Demarini, D. (2007). Occurrence, genotoxicity, and carcinogenicity of regulated and emerging disinfection by-products in drinking water: a review and roadmap for research. Mutation Research, 636, 178–242. Richardson, S. (2003). Disinfection by-products and other emerging contaminants in drinking water. TrAC Trends in Analytical Chem, 22, 666–684. Samadi, M. T., Azarian, G., Seifipour, F., Huang, C., Yang, X., & Poormohammadi, A. (2015). The formation of aldehydes and ketones ozonation by-products and their variation through general water treatment plant in Hamadan, Iran. Global NEST, 17, 682–691. Sonntag, C.V., Gunten, U.V. (2012). Chemistry of ozone in water and wastewater treatment. IWA Publishing. Staehelin, J., & Hoigne, J. (1985). Decomposition of ozone in water in the presence of organic solutes acting as promoters and inhibitors of radical chain reactions. Environmental Science & Technology, 19, 1206–1213. Tripathi, S., Pathak, V., Tripathi, D. M., & Tripathi, B. D. (2011). Application of ozone based treatments of secondary effluents. Bioresource Technology, 102, 2481–2486. Wang, H., Li, X., Hao, Z., Sun, Y., Wang, Y., Li, W., Tsang, Y.F. (2017). Transformation of dissolved organic matter in concentrated leachate from nanofiltration during ozone-based oxidation processes (O3,O3/H2O2 and O3/UV). Journal of Environmental Management, 191, 244–251. Wert, E. C., Neemann, J. J., Rexing, D. J., & Zegers, R. E. (2008). Biofiltration for removal of BOM and residual ammonia following control of bromate formation. Water Research, 42, 372–378. Yang, X., Gan, W., Zhang, X., Huang, H., & Sharma, V. K. (2015). Effect of pH on the formation of disinfection byproducts in ferrate (VI) pre-oxidation and subsequent chlorination. Separation and Purification Technology, 156, 980–986. Zhang, T., Lu, J., Ma, J., & Qiang, Z. (2008). Comparative study of ozonation and synthetic goethite-catalyzed ozonation of individual NOM fractions isolated and fractionated from a filtered river water. Water Research, 42, 1563–1570. Zhao, G., Lu, X., Zhou, Y., & Gu, Q. (2013). Simultaneous humic acid removal and bromate control by O3 and UV/O3 processes. Chemical Engineering Journal, 232, 74–80. Zhong, X., Cui, C., & Yu, S. (2016). Determination of benzenoid acids in water by solid-phase extraction/ultra-high performance liquid chromatography. China Water & Wastewater, 32, 107–112. Zhong, X., Cui, C., & Yu, S. (2017a). The determination and fate of disinfection by-products from ozonation-chlorination of fulvic acid. Environmental Science and Pollution Research, 24, 6472–6480. Zhong, X., Cui, C., & Yu, S. (2017b). Seasonal evaluation of disinfection by-products throughout two full-scale drinking water treatment plants. Chemosphere, 179, 290–297. Zimmermann, S. G., Wittenwiler, M., Hollender, J., Krauss, M., Ort, C., Siegrist, H., & Gunten, U. V. (2011). Kinetic assessment and modeling of an ozonation step for full-scale municipal wastewater treatment: micropollutant oxidation, by-product formation and disinfection. Water Research, 45, 605–617.