Removal of 4-chlorophenol from aqueous solution by granular activated carbon/nanoscale zero valent iron based on Response Surface Modeling

Open access


The phenolic compounds are known as priority pollutants, even in low concentrations, as a result of their toxicity and non-biodegradability. For this reason, strict standards have been established for them. In addition, chlorophenols are placed in the 38th to 43th in highest priority order of toxic pollutants. As a consequence, contaminated water or wastewaters with phenolic compounds have to be treated before discharging into the receiving water. In this study, Response Surface Methodology (RSM) has been used in order to optimize the effect of main operational variables responsible for the higher 4-chlorophenol removal by Activated Carbon-Supported Nanoscale Zero Valent Iron (AC/NZVI). A Box-Behnken factorial Design (BBD) with three levels was applied to optimize the initial concentration, time, pH, and adsorbent dose. The characterization of adsorbents was conducted by using SEM-EDS and XRD analyses. Furthermore, the adsorption isotherm and kinetics of 4-chlorophenol on AC and AC/NZVI under various conditions were studied. The model anticipated 100% removal efficiency for AC/NZVI at the optimum concentration (5.48 mg 4-chlorophenol/L), pH (5.44), contact time (44.7 min) and dose (0.65g/L). Analysis of the response surface quadratic model signified that the experiments are accurate and the model is highly significant. Moreover, the synthetic adsorbent is highly efficient in removing of 4-chlorophenol.

Akar, T., Ozcan, A. S., Tunali, S. & Ozcan, A. (2008). Biosorption of a textile dye (Acid Blue 40) by cone biomass of Thuja orientalis: Estimation of equilibrium, thermodynamic and kinetic parameters, Bioresource Technology, 99, 8, pp. 3057-3065.

Asghar, A., Abdul Raman, A.A. & Daud, W.M.A.W. (2014). A comparison of central composite design and Taguchi method for optimizing Fenton process, The Scientifi c World Journal, vol. 2014, pp. 1-14.

Babuponnusami, A. & Muthukumar, K. (2012). Removal of phenol by heterogenous photo electro Fenton-like process using nano-zero valent iron, Separation and Purifi cation Technology, 98, pp. 130-135.

Bayramoğlu, G. & Arıca, M.Y. (2008). Enzymatic removal of phenol and p-chlorophenol in enzyme reactor: Horseradish peroxidase immobilized on magnetic beads, Journal of Hazardous Materials, 156, 1-3, pp. 148-155.

Bayramoglu, G., Gursel, I., Tunali, Y. & Arica, M.Y. (2009). Biosorption of phenol and 2-chlorophenol by Funaliatrogii pellets, Bioresource Technology, 100, 10, pp. 2685-2691.

Cai, H.-M., Chen, G.-J., Peng, C.-Y., Zhang, Z.-Z., Dong, Y.-Y., Shang, G.-Z., Zhu, X.-H., Gao, H.-J. & Wan, X.-C. (2015). Removal of fl uoride from drinking water using tea waste loaded with Al/Fe oxides: A novel, safe and effi cient biosorbent, Applied Surface Science, 328, pp. 34-44.

Cheng, W., Dastgheib, S.A. & Karanfi l, T. (2005). Adsorption of dissolved natural organic matter by modifi ed activated carbons, Water Research, 39, 11, pp. 2281-2290.

Choe, S., Lee, S.-H., Chang, Y.-Y., Hwang, K.-Y. & Khim, J. (2001). Rapid reductive destruction of hazardous organic compounds by nanoscale Fe0, Chemosphere, 42, 4, pp. 367-372.

Ciobanu, G., Barna, S. & Harja, M. (2016). Kinetic and equilibrium studies on adsorption of Reactive Blue 19 dye from aqueous solutions by nanohydroxyapatite adsorbent, Archives of Environmental Protection, 42, 2, pp. 3-11.

Doddapaneni, K.K., Tatineni, R., Potumarthi, R. & Mangamoori, L.N. (2007). Optimization of media constituents through response surface methodology for improved production of alkaline proteases by Serratia rubidaea, Journal of Chemical Technology and Biotechnology, 82, 8, pp. 721-729.

Eckenfelder, W.W. (1989). Industrial water pollution control, McGraw-Hill, 1989.

Fakhri, A. (2015). Investigation of mercury (II) adsorption from aqueous solution onto copper oxide nanoparticles: optimization using response surface methodology, Process Safety and Environmental Protection, 93, pp. 1-8.

Foo, K. & Hameed, B. (2010). Insights into the modeling of adsorption isotherm systems, Chemical Engineering Journal, 156, 1, pp. 2-10.

Handbook, E. (1998). Advanced Photochemical Oxidation Processes, Offi ce of Research and Development Washington, DC, 20460.

Jafari, A., Mahvi, A. H., Godini, H., Rezaee, R. & Hosseini, S.S. (2014). Process optimization for fl uoride removal from water by Moringa Oleifera seed extract, Fluoride, 47, pp. 152-160.

Joo, S.H., Feitz, A.J. & Waite, T.D. (2004). Oxidative degradation of the carbothioate herbicide, molinate, using nanoscale zero-valent iron, Environmental Science & Technology, 38, 7, pp. 2242-2247.

Kanel, S.R., Manning, B., Charlet, L. & Choi, H. (2005). Removal of arsenic (III) from groundwater by nanoscale zero-valent iron, Environmental Science & Technology, 39, 5, 1291-1298.

Kassaee, M.Z., Motamedi, E., Mikhak, A. & Rahnemaie, R. (2011). Nitrate removal from water using iron nanoparticles produced by arc discharge vs. reduction, Chemical Engineering Journal, 166, 2, pp. 490-495.

Lai, C. & Chen, C.-Y. (2001). Removal of metal ions and humic acid from water by iron-coated fi lter media, Chemosphere, 44, 5, pp. 1177-1184.

Lin, K.-Y. A., Liu, Y.-T. & Chen, S.-Y. (2016). Adsorption of fl uoride to UiO-66-NH2 in water: stability, kinetic, isotherm and thermodynamic studies, Journal of Colloid And Interface Science, 461, pp. 79-87.

Mangal, H., Saxena, A., Rawat, A.S., Kumar, V., Rai, P.K. & Datta, M. (2013). Adsorption of nitrobenzene on zero valent iron loaded metal oxide nanoparticles under static conditions, Microporous and Mesoporous Materials, 168, pp. 247-256.

Michaux, F., Carteret, C., Stébé, M.-J. & Blin, J.-L. (2013). Investigation of properties of mesoporous silica materials based on nonionic fl uorinated surfactant using Box-Behnken experimental designs, Microporous and Mesoporous Materials, 174, pp. 135-143.

Moradi, M., Fazlzadehdavil, M., Pirsaheb, M., Mansouri, Y., Khosravi, T. & Sharafi , K. (2016). Response surface methodology (RSM) and its application for optimization of ammonium ions removal from aqueous solutions by pumice as a natural and low cost adsorbent, Archives of Environmental Protection, 42, 2, pp. 33-43.

Mourabet, M., El Rhilassi, A., El Boujaady, H., Bennani-Ziatni, M., El Hamri, R. & Taitai, A. (2012). Removal of fl uoride from aqueous solution by adsorption on Apatitic tricalcium phosphate using Box-Behnken design and desirability function, Applied Surface Science, 258, 10, pp. 4402-4410.

Myers, R.H., Montgomery, D.C. & Anderson-Cook, C.M. (2016). Response surface methodology: process and product optimization using designed experiments, John Wiley & Sons, 2016.

Navarro, A.E., Portales, R.F., Sun-Kou, M.R. & Llanos, B.P. (2008). Effect of pH on phenol biosorption by marine seaweeds, Journal of Hazardous Materials, 156, 1-3, pp. 405-411.

Ponder, S.M., Darab, J.G. & Mallouk, T.E. (2000). Remediation of Cr (VI) and Pb (II) aqueous solutions using supported, nanoscale zero-valent iron, Environmental Science & Technology, 34, 12, pp. 2564-2569.

Qin, Q., Wang, Q., Fu, D. & Ma, J. (2011). An effi cient approach for Pb(II) and Cd(II) removal using manganese dioxide formed in situ, Chemical Engineering Journal, 172, 1, pp. 68-74.

Ra, J.S., Oh, S.-Y., Lee, B.C. & Kim, S.D. (2008). The effect of suspended particles coated by humic acid on the toxicity of pharmaceuticals, estrogens, and phenolic compounds, Environment International, 34, 2, pp. 184-192.

Rappoport, Z. (2004). The Chemistry of Phenols, 2 Volume Set, John Wiley & Sons, 2004.

Rice, E.W., Baird, R.B., Eaton, A.D. & Clesceri, L.S. (2012). Standard methods for the examination of water and wastewater, American Public Health Association, American Water Works Association, Water Environment Federation, 2012.

Rodríguez, M. (2003). Fenton and UV-vis based advanced oxidation processes in wastewater treatment: Degradation, mineralization and biodegradability enhancement, Universitat de Barcelona, 2003.

Sądej, W., Żołnowski, A.C. & Marczuk, O. (2016). Content of phenolic compounds in soils originating from two long-term fertilization experiments, Archives of Environmental Protection, 42, 4, pp. 104-113.

Souza, A.S., Dos Santos, W.N. & Ferreira, S.L. (2005). Application of Box-Behnken design in the optimisation of an on-line pre- -concentration system using knotted reactor for cadmium determination by fl ame atomic absorption spectrometry, Spectrochimica Acta Part B: Atomic Spectroscopy, 60, 5, pp. 737-742.

Tepe, O. & Dursun, A.Y. (2008). Combined effects of external mass transfer and biodegradation rates on removal of phenol by immobilized Ralstonia eutropha in a packed bed reactor, Journal of Hazardous Materials, 151, 1, pp. 9-16.

Tseng, H.-H., Su, J.-G. & Liang, C. (2011). Synthesis of granular activated carbon/zero valent iron composites for simultaneous adsorption/dechlorination of trichloroethylene, Journal of Hazardous Materials, 192, 2, pp. 500-506.

Vadivelan, V. & Kumar, K.V. (2005). Equilibrium, kinetics, mechanism, and process design for the sorption of methylene blue onto rice husk, Journal of Colloid And Interface Science, 286, 1, pp. 90-100.

W.H.O. 1989. Chlorophenols other than pentachlorophenol. Geneva: World Health Organization.

Wu, F.-C., Wu, P.-H., Tseng, R.-L. & Juang, R.-S. (2011). Preparation of novel activated carbons from H2SO4-Pretreated corncob hulls with KOH activation for quick adsorption of dye and 4-chlorophenol, Journal of Environmental Management, 92, 3, pp. 708-713.

Wu, J. & Yu, H.-Q. (2007). Biosorption of 2,4-dichlorophenol by immobilized white-rot fungus Phanerochaete chrysosporium from aqueous solutions, Bioresource Technology, 98, 2, pp. 253-259.

Yaneva, Z.L., Koumanova, B.K. & Georgieva, N.V. (2012). Linear and nonlinear regression methods for equilibrium modelling of p-nitrophenol biosorption by Rhizopus oryzae: Comparison of error analysis criteria, Journal of Chemistry, 2013.

Yazdanbakhsh, A.R. & Hashempour, Y. (2015). Experimental design and response surface modeling for optimization of humic substances removal by activated carbon: A kinetic and isotherm study, Journal of Advances in Environmental Health Research, 3, 2, pp. 91-101.

Zhang, W.-H., Quan, X. & Zhang, Z.-Y. (2007). Catalytic reductive dechlorination of p-chlorophenol in water using Ni/Fe nanoscale particles, Journal of Environmental Sciences, 19, 3, pp. 362-366.

Archives of Environmental Protection

The Journal of Institute of Environmental Engineering and Committee of Environmental Engineering of Polish Academy of Sciences

Journal Information

IMPACT FACTOR 2016: 0.708
5-year IMPACT FACTOR: 0.835

CiteScore 2017: 1.01

SCImago Journal Rank (SJR) 2017: 0.371
Source Normalized Impact per Paper (SNIP) 2017: 0.737


All Time Past Year Past 30 Days
Abstract Views 0 0 0
Full Text Views 288 288 37
PDF Downloads 186 186 31