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Synthesis of urea-modified MnFe2O4 for aromatic micro-pollutants adsorption from wastewater: Mechanism and modeling

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Abstract

Amine-terminated MnFe2O4, using urea solution (UMF-MNPs) fabricated by a combined ultrasonic/microwave technique, was characterized and applied as a magnetic adsorbent to remove catechol, phenol, and benzene micro-pollutants from wastewater solutions. The simultaneous effect of solution pH, TDS, micro-pollutants concentrations, UMF-MNPs dose, and temperature was investigated and optimized using D-optimal design in a batch experiment. The quadratic regression, as the best-structured simulated model, predicted the maximum adsorption rates at pH 6.0, TDS 1855 mg/l, UMF-MNPs dose of 0.73 g/l, and temperature 320 K for 50 mg/l micro-pollutant concentrations. Kinetic and isotherm models, through linear and nonlinear regression methods, reflected an excellent correlation (R 2 ≈ 0.83 to 1) to simulate the adsorption data. The column breakthrough curves were tested using the equivalent length of the unused bed approach, which well fitted the Thomas model equation. The film diffusion, consequently with Lewis acid–base, is the major rate-controlling adsorption mechanism, and recovered by alkali ethanolic solution.

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References

  • Asenjo NG, Àlvarez P, Granda M, Blanco C, Santamarîa R, Menéndez R (2011) High performance activated carbon for benzene/toluene adsorption from industrial wastewater. J Hazard Mater 192:1525–1532

    Article  CAS  Google Scholar 

  • Beyki MH, Alijani H, Fazli Y (2016) Solvent free synthesized MnFe2O4@polyamid resin as a novel green nanohybrid for fast removing Congo red. J Mol Liq 216:6–11

    Article  CAS  Google Scholar 

  • Dai Y, Niu J, Yin L, Xu J, Xi Y (2011) Sorption of polycyclic aromatic hydrocarbons on electrospun nanofibrous membranes: sorption kinetics and mechanism. J Hazard Mater 192:1409–1417

    Article  CAS  Google Scholar 

  • Fang X, Xiao J, Yang S, He H, Sun C (2015) Investigation on microwave absorbing properties of loaded MnFe2O4 and degradation of reactive brilliant red X-3B. Appl Catal B Environ 162:544–550

    Article  CAS  Google Scholar 

  • Fegade SL, Tande BM, Cho H, Seames WS, Sakodynskaya I, Muggli DS, Kozliak EI (2013) Aromatization of propylene over hzsm-5: a design of experiments (DOE) approach. Chem Eng Commun 200:1039–1056

    Article  CAS  Google Scholar 

  • Feliczak-Guzik A, Jadach B, Piotrowska H, Murias M, Lulek J, Nowak I (2016) Synthesis and characterization of SBA-16 type mesoporous materials containing amine groups. Micropor Mesopor Mat 220:231–238

    Article  CAS  Google Scholar 

  • Gherca D, Pui A, Cornei N, Cojocariu A, Nica V, Caltun O (2012) Synthesis, characterization and magnetic properties of MFe2O4 (M¼Co, Mg, Mn, Ni) nanoparticles using ricin oil as capping agent. J Magn Magn Mater 324:3906–3911

    Article  CAS  Google Scholar 

  • Huang J, Jin X, Deng S (2012) Phenol adsorption on an N-methylacetamide-modified hyper cross linked resin from aqueous solutions. Chem Eng J 192:192–200

    Article  CAS  Google Scholar 

  • Karunarathne HDSS, Amarasinghe BMWPK (2013) Fixed bed adsorption column studies for the removal of aqueous phenol from activated carbon prepared from sugarcane bagass. Energy Proc 34:83–90

    Article  CAS  Google Scholar 

  • Khan TA, Khan EA, Shahjahan (2015) Removal of basic dyes from aqueous solution by adsorption onto binary iron-manganese oxide coated kaolinite: non-linear isotherm and kinetics modeling. Appl Clay Sci 107:70–77

    Article  CAS  Google Scholar 

  • Kumar KV (2006) Linear and non-linear regression analysis for the sorption kinetics of methylene blue onto activated carbon. J Hazard Mater B137:1538–1544

    Article  Google Scholar 

  • Lawson J, Erjavec J (2000) Modern statistics for engineering and quality improvement. Brooks/Cole-Thomson Learning, Pacific Grove

    Google Scholar 

  • Lazo-Cannata JC, Nieto-Márquez A, Jacoby A, Paredes-Doig AL, Romero A, Sun-Kou MR, Valverde JL (2011) Adsorption of phenol and nitrophenols by carbon nanospheres: effect of pH and ionic strength. Sep Purif Technol 80:217–224

    Article  CAS  Google Scholar 

  • Liu Y (2009) Is the free energy change of adsorption correctly calculated. J Chem Eng Data 54:1981–1985

    Article  CAS  Google Scholar 

  • Liu Y, Gao M, Gu Z, Luo Z, Ye Y, Lu L (2014) Comparison between the removal of phenol and catechol by modified montmorillonite with two novel hydroxyl-containing gemini surfactants. J Hazard Mater 267:71–80

    Article  CAS  Google Scholar 

  • Luo Y, Guo W, Ngo HH, Nghiem LD, Hai FI, Zhang J, Liang S, Wang XC (2014) A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. Sci Total Environ 473–474:619–641

    Article  Google Scholar 

  • Luo Z, Gao M, Yang S, Yang Q (2015) Adsorption of phenols on reduced-charge montmorillonites modified by bispyridinium dibromides: mechanism, kinetics and thermodynamics studies. Colloids Surf Physisochem Eng Asp 482:222–230

    Article  CAS  Google Scholar 

  • Mohammed J, Nasri NS, Abbas M, Zaini A, Hamza UD, Ani FN (2015) Adsorption of benzene and toluene onto KOH activated coconut shell based carbon treated with NH3. Int Biodeter Biodegr 102:245–255

    Article  CAS  Google Scholar 

  • Myers WR, Montgomery DC (2003) Response surface methodology. Encycl Biopharm Stat 1:858–869

    Google Scholar 

  • Nam S-W, Choi D-J, Kim S-K, Her N, Zoh K-D (2014) Adsorption characteristics of selected hydrophilic and hydrophobic micropollutants in water using activated carbon. J Hazard Mater 270:144–152

    Article  CAS  Google Scholar 

  • Naushad M, ALOthman ZA, Khan MR, ALQahtani NJ, ALSohaimi IH (2014) Equilibrium, kinetics and thermodynamic studies for the removal of organophosphorus pesticide using Amberlyst-15 resin: quantitative analysis by liquid chromatography–mass spectrometry. J Ind Eng Chem 20:4393–4400

    Article  CAS  Google Scholar 

  • Shao L, Ren Z, Zhang G, Chen L (2012) Facile synthesis, characterization of a MnFe2O4/activated carbon magnetic composite and its effectiveness in tetracycline removal. Mater Chem Phys 135:16–24

    Article  CAS  Google Scholar 

  • Shi Y, Du J, Zhou L, Li X, Zhou Y, Li L, Zang X, Zhang X, Pan F, Zhang H, Wang Z, Zhu X (2012) Size-controlled preparation of magnetic iron oxide nanocrystals within hyperbranched polymers and their magnetofection in vitro. J Mater Chem 22:355–360

    Article  CAS  Google Scholar 

  • Shojaat R, Saadatjooa N, Karimi A, Aber S (2016) Simultaneous adsorption–degradation of organic dyes using MnFe2O4/calcium alginate nano-composites coupled with GOx and laccase. J Environ Chem Eng (JECE) 4:1722–1730

    Article  CAS  Google Scholar 

  • Şimşek T, Akansel S, Özcann S, Ceylan A (2014) Synthesis of MnFe2O4 nanocrystals by wet-milling under atmospheric conditions. Ceram Int 40:7953–7956

    Article  Google Scholar 

  • Singh KP, Gupta S, Singh AK, Sinha S (2011) Optimizing adsorption of crystal violet dye from water by magnetic nanocomposite using response surface modeling approach. J Hazard Mater 186:1462–1473

    Article  CAS  Google Scholar 

  • Tan IAW, Ahmad AL, Hameed BH (2009) Adsorption isotherms, kinetics, thermodynamics and desorption studies of 2,4,6-trichlorophenol on oil palm empty fruit bunch-based activated carbon. J Hazard Mater 164:473–482

    Article  CAS  Google Scholar 

  • Weber WJ, Morris JC (1962) In: Proceedings of international conference water pollution symposium, vol 2, Pergamon, Oxford, pp 231–266

  • Wiśniewski M, Werengowska-Ciećwierz K, Terzyk AP (2015) New findings on the influence of carbon surface curvature on energetics of benzene adsorption from aqueous solutions. Chem Phys Lett 619:219–222

    Article  Google Scholar 

  • Xiao Y, Liang H, Chen W, Wang Z (2013) Synthesis and adsorption behavior of chitosan-coated MnFe2O4 nanoparticles for trace heavy metal ions removal. Appl Surf Sci 285P:498–504

    Article  Google Scholar 

  • Yang G, Chen H, Qin H, Feng Y (2014) Amination of activated carbon for enhancing phenol adsorption: effect of nitrogen-containing functional groups. Appl Surf Sci 293:299–305

    Article  CAS  Google Scholar 

  • Yetilmezsoy K, Demirel S, Vanderbei RJ (2009) Response surface modeling of Pb(II) removal from aqueous solution by Pistacia vera L.: Box-Behnken experimental design. J Hazard Mater 171:551–562

    Article  CAS  Google Scholar 

  • Younis SA, El-Gendy NSh, El-Azab WI, Moustafa YN, Hashem AI (2014) The biosorption of phenol from petroleum refinery wastewater using spent waste biomass. Energy Sour Part A 36:2566–2578

    Article  CAS  Google Scholar 

  • Yousefa RI, El-Eswed B (2009) The effect of pH on the adsorption of phenol and chlorophenols onto natural zeolite. Colloids Surf A Physicochem Eng Asp 334:92–99

    Article  Google Scholar 

  • Zaghouane-Boudiaf H, Boutahala M, Sahnoun S, Tiar C, Gomri F (2014) Adsorption characteristics, isotherm, kinetics, and diffusion of modified natural bentonite for removing the 2,4,5-trichlorophenol. Appl Clay Sci 90:81–87

    Article  CAS  Google Scholar 

  • Zaini MS, Ismail N, Lim CK, Neoh CH, Lam CY, Aris A, Majid ZA, Manan FA, Ibrahim Z (2015) Optimization of biostructure for the adsorption of petrochemical wastewater using statistical approach. Clean Technol Environ 17:249–256

    Article  CAS  Google Scholar 

  • Zaki T, Saed D, Aman D, Younis SA, Moustafa YM (2013) Synthesis and characterization of MFe2O4 sulfur nanoadsorbents. J Sol-Gel Sci Technol 65:269–276

    Article  CAS  Google Scholar 

  • Zietzschmann F, Stützer C, Jekel M (2016) Granular activated carbon adsorption of organic micro-pollutants in drinking water and treated wastewater-Aligning breakthrough curves and capacities. Water Res 92:180–187

    Article  CAS  Google Scholar 

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Authors and Affiliations

  1. Analysis and Evaluation Department, Egyptian Petroleum Research Institute, Nasr City, Cairo, 11727, Egypt

    Sherif A. Younis & Yasser M. Moustafa

  2. Liquid Chromatography Unit, Central Laboratories, Egyptian Petroleum Research Institute, Nasr City, Cairo, 11727, Egypt

    Sherif A. Younis & Yasser M. Moustafa

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  1. Sherif A. Younis
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  2. Yasser M. Moustafa
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Correspondence to Sherif A. Younis.

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Younis, S.A., Moustafa, Y.M. Synthesis of urea-modified MnFe2O4 for aromatic micro-pollutants adsorption from wastewater: Mechanism and modeling. Clean Techn Environ Policy 19, 527–540 (2017). https://doi.org/10.1007/s10098-016-1244-6

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