Abstract
Discharge of wastewater containing nitrogen and phosphate can cause eutrophication. Therefore, the development of an efficient material for the immobilization of the nutrients is important. In this study, a low calcium fly ash and high calcium fly ash were converted into zeolite using the hydrothermal method. The removal of ammonium and phosphate that coexist in aqueous solution by the synthesized zeolites were studied. The results showed that zeolitized fly ash could efficiently eliminate ammonium and phosphate at the same time. Saturation of zeolite with Ca2+ rather than Na+ favored the removal of both ammonium and phosphate because the cation exchange reaction by the NH4 + resulted in the release of Ca2+ into the solution and precipitation of Ca2+ with PO4 3− followed. An increase in the temperature elevated the immobilization of phosphate whereas it abated the removal of ammonium. Nearly 60% removal efficiency for ammonium was achieved in the neutral pH range from 5.5 to 10.5, while the increase or decrease in pH out of the neutral range lowered the adsorption. In contrast, the removal of phosphate approached 100% at a pH lower than 5.0 or higher than 9.0, and less phosphate was immobilized at neutral pH. However, there was still a narrow pH range from 9.0 to 10.5 favoring the removal of both ammonium and phosphate. It was concluded that the removal of ammonium was caused by cation exchange; the contribution of NH3 volatilization to immobilization at alkaline conditions (up to pH level of 11.4) was limited. With respect to phosphate immobilization, the mechanism was mainly the formation of precipitate as Ca3(PO4)2 within the basic pH range or as FePO4 and AlPO4 within acidic pH range.
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References
Komarowski S, Yu Q. Ammonium ion removal from wastewater using Australian natural zeolite: batch equilibrium and kinetic studies. Environ Technol, 1997, 18: 1085–1097
Nguyen M L, Tanner C C. Ammonium removal from wastewaters using natural New Zealand zeolites. New Zealand J Agric Res, 1998, 41: 427–446
Hollman G G, Steenbruggen G, Janssen-Jurkovi Čová M. A two-step process for the synthesis of zeolites from coal fly ash. Fuel, 1999, 78: 1225–1230
Murayama N, Yoshida S, Takami Y, Yamamoto H, Shibata J. Simultaneous removal of NH4 + and PO4 3− in aqueous solution and its mechanism by using zeolite synthesized from coal fly ash. Separat Sci Technol, 2003, 38: 113–129
Querol X, Moreno N, Umaña J C, Alastuey A, Hernández E, López-Soler A, Plana F. Synthesis of zeolites from coal fly ash: an overview. Int J Coal Geol, 2002, 50: 413–423
Neufeld R D, Thodos G. Removal of orthophosphate from aqueous solution with activated alumina. Environ Sci Technol, 1969, 3: 661–667
Baker M J, Blowes D W, Ptacek C J. Laboratory development of permeable reactive mixtures for the removal of phosphorous from onsite wastewater disposal systems. Environ Sci Technol, 1998, 32: 2308–2316
Fine L O, Jensen W P. Phosphate in waters: I. Reduction using northern lignite fly ash. Water Resour Bull, 1981, 17: 895–897
Grubb D G, Guimaraes M S, Valencia R. Phosphate immobilization using an acidic type F fly ash. J Hazardous Mater, 2000, 76: 217–236
Drizo A, Frost C A, Grace J, Smith K A. Physico-chemical screening of phosphate-removing substrates for use in constructed wetland systems. Water Res, 1999, 33: 3595–3602
Ugurlu A, Salman B. Phosphorus removal by fly ash. Environ Int, 1998, 24: 911–918
Cheung K C, Venkitachalam T H. Improving phosphate removal of sand infiltration system using alkaline fly ash. Chemosphere, 2000, 41: 243–249
Agyei N M, Strydom C A, Potgieter J H. The removal of phosphate ions from aqueous solution by fly ash, slag, ordinary Portland cement and related blends. Cement Concr Res, 2002, 32: 1889–1897
Oguz E. Removal of phosphate from aqueous solution with blast furnace slag. J Hazardous Mater, 2004, B114, 131–137
Del Bubba M, Arias C A, Brix H. Phosphorus adsorption maximum of sands for use as media in subsurface flow constructed reed beds as measured by the Langmuir isotherm. Water Res, 2003, 37: 3390–3400
Arias C A, Del Bubba M, Brix H. Phosphorus removal by sands for use as media in subsurface flow constructed reed beds. Water Res, 2001, 35: 1159–1168
Tanaka S, Kabayama M, Kawasaki N, Sakiyama T, Nakamura T, Araki M, Tamura T. Removal of phosphate by aluminum oxide hydroxide. J Colloid Interf Sci, 2003, 257: 135–140
Zhao L H, Zhao Z Y. The current situation in the utilization of coal fly ash. Techn Equip Environ Pollut Contr, 2002, 3: 35–39 (in Chinese)
Höller H, Wirsching U. Zeolite formation from fly ash. Forschr Miner, 1985, 63: 21–43
Chen J G, Kong H N, Wu D Y, Hu Z B, Wang Z S, Wang Y H. Removal of phosphate from aqueous solution by zeolite synthesized from fly ash. J Colloid Interf Sci, 2006, 300: 491–497
Wu D Y, Kong H N, Zhao T G. Effects of synthesis conditions on the formation and quality of zeolite during the hydrothermal zeolitization processes of fly ash. J Inorganic Mater, 2005, 20: 1153–1158
Wu D Y, Zhang B H, Li C J, Zhang Z J, Kong H N. Simultaneous removal of ammonium and phosphate by zeolite synthesized from fly ash as influenced by salt treatment. J Colloid Interf Sci, 2006, 304: 300–306
Wu D Y, Zhang B H, Yan L, Kong H N, Wang X Z. Effect of some additives on the formation of zeolite from coal fly ash. Int J Miner Proc, 2006, 80: 266–272
Molina A, Poole C A. Comparative study using two methods to produce zeolites from fly ash. Miner Eng, 2004, 17: 167–173
Shigemoto N, Hayashi H, Miyaura K. Selective formation of Na-X zeolite from coal fly ash by fusion with sodium hydroxide prior to hydrothermal reaction. J Mater Sci, 1993, 28: 4781–4786
Queral X, Plana F, Alastuey A, López-Soler A. Synthesis of Na-zeolites from fly ash. Fuel, 1997, 76: 793–799
Stumm W, Morgan J J. Aquatic Chemistry. 3rd ed. New York: John Wiley and Sons, 1996, 780
Jenkins D, Ferguson J F, Menar A B. Chemical processes for phosphate removal. Water Res, 1971, 5: 369–389
Holford I C R, Mattingly G E G. The high-and low-energy phosphate adsorbing surfaces in calcareous soils. J Soil Sci, 1975, 26: 407–417
Doyle J D, Parsons S A. Struvite formation, control and recovery. Water Res, 2002, 36: 3925–3940
Stratful I, Scrimshaw M D, Lester J N. Conditions influencing the precipitation of magnesium ammonium phosphate. Water Res, 2001, 35: 4191–4199
Goldberg S, Sposito G. A chemical moder of phosphate adsorption by soils: II. Non-calcareous soils. Soil Sci Soc Am J, 1984, 48: 779–783
Parfitt R L. Anion adsorption by soils and soil materials. Adv Agron, 1978, 30: 1–50
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Wu, D., Hu, Z., Wang, X. et al. Use of zeolitized coal fly ash in the simultaneous removal of ammonium and phosphate from aqueous solution. Front.Environ.Sci.Eng.China 1, 213–220 (2007). https://doi.org/10.1007/s11783-007-0037-x
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DOI: https://doi.org/10.1007/s11783-007-0037-x