MSCE  Vol.3 No.9 , September 2015
Modeling and Optimizations of Phosphate Removal from Aqueous Solutions Using Synthetic Zeolite Na-A
Synthetic zeolite Na-A was prepared from Egyptian kaolinite by hydrothermal treatment to be used as an adsorbent for removal of phosphate from aqueous solutions. The present work deals with the application of response surface methodology (RSM) and central composite rotatable design (CCRD) for modeling and optimization of the effect of four operating variables on the removal of phosphate from aqueous solution using zeolite Na-A. The parameters were contact time (0.5 - 6 h), phosphate anion concentrations (10 - 30 mg/L), adsorbent dosage (0.05 - 0.1 g), and solution pH (2 - 7). A total of 26 tests were conducted using the synthetic zeolite Na-A according to the conditions predicted by the statistical design. In order to optimize removal of phosphate by synthetic zeolite Na-A, mathematical equations of quadratic polynomial model were derived from Design Expert Software (Version 6.0.5). Such equations are second-order response functions which represent the amount of phosphate adsorbed (mg/g) and the removal efficiency (%) and are expressed as functions of the selected operating parameters. Predicted values were found to be in good agreement and correlation with experimental results (R2 values of 0.918 and 0.905 for amount of phosphate adsorbed and removal efficiency of it, respectively). To understand the effect of the four variables for optimal removal of phosphate using zeolite Na-A, the models were presented as cube and 3-D response surface graphs. RSM and CCRD could efficiently be applied for the modeling of removing of phosphate from aqueous solution using zeolite Na-A and it is efficient way for obtaining information in a short time and with the fewer number of experiments.

Cite this paper
Mohamed, E. , Selim, A. , Seliem, M. and Abukhadra, M. (2015) Modeling and Optimizations of Phosphate Removal from Aqueous Solutions Using Synthetic Zeolite Na-A. Journal of Materials Science and Chemical Engineering, 3, 15-29. doi: 10.4236/msce.2015.39003.
[1]   Ramakrishnaiah, C.R. and Vismitha (2012) Removal of Phosphate from Waste Water Using Low-Cost Adsorbents. International Journal of Engineering Inventions, 1, 44-50.

[2]   De-Bashan, L.E. and Bashan, Y. (2004) Recent Advances in Removing Phosphorus from Wastewater and Its Future Use as Fertilizer. Water Research, 38, 4222-4246.

[3]   El Sergany, M. and Shanableh, A. (2012) Phosphorus Removal Using Al-Modified Bentonite Clay-Effect of Particle Size. Proceeding Asia Pacific Conference on Environmental Science and Technology, 6, 323-329.

[4]   Luo, H., Li, F., Zeng, Y.-M., Zhang, K. and Huang, B. (2012) Adsorption Control Performance of Phosphorus Removal from Agricultural Non-Point Source Pollution by Nano-Aperture Lanthanum-Modified Active Alumina. Advance Journal of Food Science and Technology, 4, 337-343.

[5]   Xiong, W. (2009) Development and Application of Ferrihydrite Modified Diatomite and Gypsum for Phosphorus Control in Lakes and Reservoirs. Ph.D. Dissertation, College of Graduate Studies and Research, Saskatchewan, Canada.

[6]   Quan, W.M. and Yan, L.J. (2002) Effects of Agricultural Non-Point Source Pollution on Eutrophication of Water Body and Its Control Measure. Acta Ecologica Sinica, 22, 291-299.

[7]   Tang, H., Xiong, L.J. and Huang, S.F. (2011) Review on the Characteristic and Control Measurement of Agriculture Non-Point Source Pollution. Environmental Science & Technology, 34, 107-112.

[8]   Xie, T., Kang, C.X. and Tang, W.K. (2010) Review on the Pollution and Control Measurement of Agriculture Non- Point Source Pollution. Journal of Guangxi Teachers Education University (Natural Science Edition), 27, 70-73.

[9]   Durán, N., Marcarto, P.D., De Souza, G.I.H., Alves, O.L. and Esposito, E. (2007) Antibacterial Effect of Silver Nanoparticles Produced by Fungal Process on Textile Fabrics and Their Effluent Treatment. Journal of Biomedical Nanotechnology, 3, 203-208.

[10]   Karapinar, N. (2009) Application of Natural Zeolite for Phosphorus and Ammonium Removal from Aqueous Solutions. Journal of Hazardous Materials, 170, 1186-1191.

[11]   Stratful, I., Brett, S., Scrimshaw, M.B. and Lester, J.N. (1999) Biological Phosphorus Removal, Its Role in Phosphorus Recycling. Environmental Technology, 20, 681-695.

[12]   Hart, B.T., Roberts, S., James, R., O’Donohue, M., Taylor, J. and Donner, D. (2003) Active Barrier to Reduce Phosphorus Release from Sediments: Effectiveness of Three Forms of CaCO3. Australian Journal of Chemistry, 56, 207- 217.

[13]   Drizo, A., Frost, C.A., Grace, J. and Smith, J.K. (1999) Physico-Chemical Screening of Phosphate Removing Substrates for Use in Constructed Wetland Systems. Water Research, 33, 3595-3602.

[14]   Wadpersdolf, E., Neumann, T. and Stuben, D. (2004) Efficiency of Natural Calcite Precipitation Compared to Lake Marl Application Used for Water Quality Improvement in an Eutrophic Lake. Applied Geochemistry, 19, 1687-1698.

[15]   Xiong, W.H. and Peng, J. (2008) Development and Characterization of Ferrihydrite-Modified Diatomite as a Phosphorus Adsorbent. Water Research, 42, 4869-4877.

[16]   Chaisena, A. and Rangsriwatananon, K. (2005) Synthesis of Sodium Zeolite from Natural and Modified Diatomite. Materials Letters, 59, 1474-1479.

[17]   Breck, D.W. (1974) Zeolite Molecular Sieves: Structure, Chemistry and Use. John Wiley, New York.

[18]   Bowman, R.S. (2003) Application of Surfactant Modified Zeolites to Environmental Remediation. Microporous and Mesoporous Materials, 61, 43-56.

[19]   Youssef, H., Ibrahim, D. and Komarneni, S. (2008) Microwave Assisted versus Conventional Synthesis of Zeolite A from Metakaolinite. Microporous and Mesoporous Materials, 115, 527-534.

[20]   Mousavi, S.F., Jafari, M., Kazemimoghadam, M. and Mohammadi, T. (2013) Template Free Crystallization of Zeolite Rho via Hydrothermal Synthesis: Effects of Synthesis Time, Synthesis Temperature, Water Content and Alkalinity. Ceramic International, 39, 7149-7158.

[21]   Katsuki, H., Furuta, S., Watari, T. and Komarneni, S. (2005) ZSM-5 Zeolite/Porous Carbon Composite: Conventional- and Microwave-Hydrothermal Synthesis from Carbonized Rice Husk. Microporous and Mesoporous Materials, 86, 145-151.

[22]   Ma, Y., Alshameri, A., Qiu, X., Zhou, C. and Li, A. (2014) Synthesis and Characterization of 13X Zeolite from Low Grade Natural Kaolinite. Advanced Powder Technology, 25, 495-499.

[23]   Belviso, C., Cavalcante, F., Lettino, A. and Fiore, S. (2013) A and X Type Zeolites from Kaolinite at Low Temperature. Applied Clay Science, 80, 162-168.

[24]   Cheng, Y., Lu, M., Li, J., Su, X., Pan, S., Jiao, C. and Feng, M. (2012) Synthesis of MCM-22 Source under Varying- Temperature Conditions. Journal of Colloid and Interface Science, 369, 388-394.

[25]   Atta, A.Y., Jibril, B.Y., Aderemi, B.O. and Adefila, S.S. (2012) Preparation of Analcime from Local Kaolin and Rice Husk Ash. Applied Clay Science, 61, 8-13.

[26]   Qiu, W. and Zheng, Y. (2009) Removal of Copper, Nickel, Cobalt and Zinc from Water by a Cancrinite-Type Zeolite Synthesized from Fly Ash. Chemical Engineering Journal, 145, 483-488.

[27]   Wajima, T., Haga, M., Kuzawa, K., Ishimoto, H., Tamada, O., Ito, K., Nishiyama, T., Downs, R.T. and Rakovan, J.T. (2006) Zeolite Synthesis from Paper Sludge Ash at Low Temperature (90°C) with Addition of Diatomite. Journal of Hazardous Materials, 132, 244-252.

[28]   Petkowicz, D.I., Rigo, R.T., Radtke, C., Pergher, S.B. and Dos-Santos, J.H.Z. (2008) Zeolite NaA from Brazilian Chrysotile and Rice Husk. Microporous and Mesoporous Materials, 116, 548-554.

[29]   Liu, H., Shen, T., Yuan, P., Shi, G. and Bao, X. (2014) Green Synthesis of Zeolites from a Natural Aluminosilicate Mineral Rectorite: Effects of Thermal Treatment Temperature. Applied Clay Science, 90, 53-60.

[30]   Liu, X.-D., Wang, Y.-P., Cui, X.-M., He, Y. and Mao, J. (2013) Influence of Synthesis Parameters on NaA Zeolite Crystal. Powder Technology, 243, 184-193.

[31]   Rege, S.U. and Yang, R.T. (1997) Limits for Air Separation by Adsorption with LiX Zeolite. Industrial & Engineering Chemistry Research, 36, 5358.

[32]   Eken-Saracoglu, N. and Culfaz, N. (1999) Clinoptilotile Zeolite as a Builder in Nonphosphated Detergents. Journal of Environmental Science and Health—Part A, 34, 1619-1626.

[33]   Ravikumar, K., Krishnan, S., Ramalingam, S. and Balu, K. (2007) Optimization of Process Variables by the Application of Response Surface Methodology for Dye Removal Using a Novel Adsorbent. Dyes and Pigments, 72, 66-74.

[34]   Myers, R.H. and Montgomery, D.C. (2002) Response Surface Methodology. John Wiley and Sons, New York.

[35]   Nuran, B. (2007) The Response Surface Methodology. Master of Science in Applied Mathematics and Computer Science, PhD Dissertation, Faculty of the Indiana University, South Bend.

[36]   Gunaraj, V. and Murugan, N. (1999) Application of Response Surface Methodologies for Predicting Weld Base Quality in Submerged Arc Welding of Pipes. Journal of Materials Processing Technology, 88, 266-275.

[37]   Box, G.E.P. and Wilson, K.B. (1951) On the Experimental Attainment of Optimum Conditions. Journal of the Royal Statistical Society, 13, 1-45.

[38]   Box, G.E.P. and Hunter, W.G. (1957) Multi-Factor Experimental Design for Exploring Response Surfaces. Mathematical Statistics, 28, 195-241.

[39]   Obeng, D.P., Morrell, S. and Napier-Munn, T.J. (2005) Application of Central Composite Rotatable Design to Modeling the Effect of Some Operating Variables on the Performance of the Three-Product Cyclone. International Journal of Mineral Processing, 76, 181-192.

[40]   Cilliers, J.J., Austin, R.C. and Tucker, J.P. (1992) An Evaluation of Formal Experimental Design Procedures for Hydrocyclone Modeling. Proceeding of the 4th International Conference on Hydrocyclones, Southampton, 23-25 September 1992, 3-49.

[41]   Souzaa, A.S., Walter, N.L., dos Santos, L.C. and Ferreira, S. (2005) Application of Box-Behnken Design in the Optimization of an On-Line Pre-Concentration System Using Knotted Reactor for Cadmium Determination by Flame Atomic Absorption Spectrometry. Spectrochimica Acta, Part B: Atomic Spectroscopy, 60, 737-742.

[42]   Ferreira, A.C., Costa, A.C.S. and Korn, M.G.A. (2004) Preliminary Evaluation of the Cadmium Concentration in Sea Water of the Salvador City, Brazil. Microchemical Journal, 78, 77-83.

[43]   Gougazeh, M. and Buhl, J.C. (2014) Synthesis and Characterization of Zeolite A by Hydrothermal Transformation of Natural Jourdanian Kaolin. Journal of the Association of Arab Universities for Basic and Applied Sciences, 15, 35-42.

[44]   Treacy, M.M.J. and Higgins, J.B. (2001) Collection of Simulated XRD Powder Patterns for Zeolites. Elsevier, Amsterdam.

[45]   Rajasimman, M. and Murugaiyan, K. (2012) Application of the Statistical Design for the Sorption of Lead by Hypneavalentiae. Journal of Advanced Chemical Engineering, 2, 1-7.

[46]   Deepa, C.N., Sayed, A. and Suresha, S. (2014) Kinrtic and Isothermal Studies on the Removal of Copper (П) from Aqueous Solution by Araucaria Cook П: Response Surface Methodology for the Optimization. International Journal of Recent Scientific Research, 5, 820-827.

[47]   Chen, J.C., Kong, H.N., Wu, D.Y., Hu, Z.B., Wang, Z.S. and Wang, Y.H. (2006) Removal of Phosphate from Aqueous Solution by Zeolite Synthesized from Fly Ash. Journal of Colloid and Interface Science, 300, 491-497.

[48]   Hamdi, N. and Srasra, E. (2012) Removal of Phosphate Ions from Aqueous Solution using Tunisian Clays Minerals and Synthetic Zeolite. Journal of Environmental Sciences, 24, 617-623.

[49]   Akar, T. and Tunali, S. (2006) Biosorption Characteristics of Aspergillus flavus Biomass for Removal of Pb (II) and Cu (II) Ions from Aqueous Solution. Bioresource Technology, 97, 1780-1787.

[50]   Mall, D.I., Srivastava, V.C. and Agarwal, N.K. (2006) Removal of Orange-G and Methyl Violet Dyes by Adsorption onto Bagasse Fly Ash-Kinetic Study and Equilibrium Isotherm Analyses. Dyes and Pigments, 69, 210-223.