Fe3O4 NPs are synthesized by the co-precipitation technique. Moreover, the pristine was coated by silica layer and then functionalized by 3-aminopropyltrimethoxysilane (APTS). The sample possessed saturation magnetization with value equals 37 emu/g which made them to easily separate using external magnet. FT-IR, TGA, EDX, and VSM confirmed the aminosilane loading. The surface topography and composition were characterized using XRD, TEM, SEM, BJH, and BET methods. Where adsorption capacity of the surface toward the removal of four commercial reactive wool dyes (RD), Itowol black (IB), Itowol Red (IR), Sunzol black (SB), and Lanasol blue (LB) have been investigated. The influence variables such as pH, adsorbent dose, dye concentration, and temperature were calculated. Where experimental results fitted to Langmuir isotherm model with qmax equals 161.29, 151.51, 123.45, and 98.20 mg/g, for IR, LB, SB, and IB respectively. The results showed that the RD adsorption described by pseudo-second-order kinetics. The calculated thermodynamic parameters indicated that RD adsorption onto Fe3O4@SiO2–NH2 was spontaneous and exothermic in nature. The possible mechanisms monitoring RD adsorption on the surface included hydrogen bonding and electrostatic interactions. The reusability of adsorbent carried with four cycles without releasing of magnetite and thus excluding the potential hazardous of nanomaterial to the environment.
This is a preview of subscription content, log in to check access.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
Tax calculation will be finalised during checkout.
Abkenar SD, Khoobi M, Tarasi R et al (2015) Fast removal of methylene blue from aqueous solution using magnetic-modified Fe3O4 nanoparticles. J Environ Eng 141:04014049–04014047. https://doi.org/10.1061/(ASCE)EE.1943-7870.0000878
Aboelfetoh EF, Elhelaly AA, Gemeay AH (2018) Synergistic effect of Cu(II) in the one-pot synthesis of reduced graphene oxide (rGO/CuxO) nanohybrids as adsorbents for cationic and anionic dyes. J Environ Chem Eng 6:623–634. https://doi.org/10.1016/j.jece.2017.12.047
Aguado J, Arsuaga JM, Arencibia A et al (2009) Aqueous heavy metals removal by adsorption on amine-functionalized mesoporous silica. J Hazard Mater 163:213–221. https://doi.org/10.1016/j.jhazmat.2008.06.080
Aljarrah MT, Al-Harahsheh MS, Mayyas M, Alrebaki M (2018) In situ synthesis of quaternary ammonium on silica-coated magnetic nanoparticles and it’s application for the removal of uranium (VI) from aqueous media. J Environ Chem Eng 6:5662–5669. https://doi.org/10.1016/j.jece.2018.08.070
Arica TA, Ayas E, Arica MY (2017) Magnetic MCM-41 silica particles grafted with poly (glycidylmethacrylate) brush: Modification and application for removal of direct dyes. Microporous Mesoporous Mater 243:164–175. https://doi.org/10.1016/j.micromeso.2017.02.011
Arica TA, Kuman M, Gercel O, Ayas E (2019) Poly (dopamine) grafted bio-silica composite with tetraethylenepentamine ligands for enhanced adsorption of pollutants. Chem Eng Res Des 141:317–327. https://doi.org/10.1016/j.cherd.2018.11.003
Bayramoglu G, Arica MY (2018) Adsorption of Congo Red dye by native amine and carboxyl modified biomass of Funalia trogii: isotherms, kinetics and thermodynamics mechanisms. Korean J Chem Eng 35:1303–1311
Bayramoglu G, Adiguzel N, Ersoy G et al (2013) Removal of textile dyes from aqueous solution using amine-modified plant biomass of A. caricum: equilibrium and kinetic studies. Water, Air, Soil Pollut 224:1640
Bayramoglu G, Akbulut A, Liman G, Arica MY (2017) Removal of metal complexed azo dyes from aqueous solution using tris(2-aminoethyl)amine ligand modified magnetic p(GMA-EGDMA) cationic resin: adsorption, isotherm and kinetic studies. Chem Eng Res Des 124:85–97. https://doi.org/10.1016/j.cherd.2017.06.005
Dalvand A, Nabizadeh R, Reza Ganjali M et al (2016) Modeling of Reactive Blue 19 azo dye removal from colored textile wastewater using L-arginine-functionalized Fe3O4 nanoparticles: optimization, reusability, kinetic and equilibrium studies. J Magn Magn Mater 404:179–189. https://doi.org/10.1016/j.jmmm.2015.12.040
Darwish MSA, Nguyen NHA, Ševců A (2015) Stibor I (2015) Functionalized magnetic nanoparticles and their effect on escherichia coli and staphylococcus aureus. J Nanomater. https://doi.org/10.1155/2015/416012
Egerton RF (2005) Physical principles of electron microscopy. Springer
El-Alaily TM, El-Nimr MK, Saafan SA et al (2015) Construction and calibration of a low cost and fully automated vibrating sample magnetometer. J Magn Magn Mater 386:25–30. https://doi.org/10.1016/j.jmmm.2015.03.051
Elsherbiny AS, El Hefnawy ME, Gemeay AH (2018) Adsorption efficiency of polyaspartate-montmorillonite composite towards the removal of Pb ( II ) and Cd ( II ) from aqueous solution. J Polym Environ 26:411–422. https://doi.org/10.1007/s10924-017-0958-9
Freundlich HMF (1906) Over the adsorption in solution. J Phys Chem 57:1100–1107
Freundlich H, Heller W (1939) The adsorption of cis-and trans-azobenzene. J Am Chem Soc 61:2228–2230
Gawande MB, Monga Y, Zboril R, Sharma RK (2015) Silica-decorated magnetic nanocomposites for catalytic applications. Coord Chem Rev 288:118–143. https://doi.org/10.1016/j.ccr.2015.01.001
Ge S, Agbakpe M, Zhang W, Kuang L (2015) Heteroaggregation between PEI-coated magnetic nanoparticles and algae: effect of particle size on algal harvesting efficiency. ACS Appl Mater Interfaces 7:6102–6108. https://doi.org/10.1021/acsami.5b00572
Gemeay AH (2002) Adsorption characteristics and the kinetics of the cation exchange of Rhodamine-6G with Na+-montmorillonite. J Colloid Interface Sci 251:235–241. https://doi.org/10.1006/jcis.2002.8410
Ghasemzadeh MA, Abdollahi-Basir MH, Babaei M (2015) Fe3O4@SiO2–NH2 core-shell nanocomposite as an efficient and green catalyst for the multi-component synthesis of highly substituted chromeno[2,3-b]pyridines in aqueous ethanol media. Green Chem Lett Rev 8:40–49. https://doi.org/10.1080/17518253.2015.1107139
Ghorbani F, Kamari S (2019) Core – shell magnetic nanocomposite of Fe3O4@SiO2@NH2 as an efficient and highly recyclable adsorbent of methyl red dye from aqueous environments. Environ Technol Innov 14:100333. https://doi.org/10.1016/j.eti.2019.100333
Golmohammadi F, Hazrati M, Safari M (2019) Removal of reactive yellow 15 from water sample using a magnetite nanoparticles coated with covalently immobilized dimethyl octadecyl[3-(trimethoxysilylpropyl)]ammonium chloride ionic liquid. Microchem J 144:64–72. https://doi.org/10.1016/j.microc.2018.08.057
Han R, Zou W, Yu W et al (2007) Biosorption of methylene blue from aqueous solution by fallen phoenix tree’s leaves. J Hazard Mater 141:156–162. https://doi.org/10.1016/j.jhazmat.2006.06.107
Hou A, Zhang X (2011) Decolorisation of reactive dye wastewater and the effect of surfactants using laccase. Color Technol 127:200–204. https://doi.org/10.1111/j.1478-4408.2011.00299.x
Hozhabr Araghi S, Entezari MH (2015) Amino-functionalized silica magnetite nanoparticles for the simultaneous removal of pollutants from aqueous solution. Appl Surf Sci 333:68–77. https://doi.org/10.1016/j.apsusc.2015.01.211
Huang SH, Chen DH (2014) Isolation of DNA using magnetic nanoparticles coated with dimercaptosuccinic acid. Anal Biochem J 447:114–118 Contents. https://doi.org/10.1016/j.jhazmat.2008.06.075
Huo Y, Wu H, Wang Z, et al (2018) Preparation of core / shell nanocomposite adsorbents based on amine polymer-modified magnetic materials for the efficient adsorption of anionic dyes. Colloids Surfaces A 549:174–183. https://doi.org/10.1016/j.colsurfa.2018.04.021
Jiang F, Fu Y, Zhu Y et al (2012) Fabrication of iron oxide/silica core–shell nanoparticles and their magnetic characteristics. J Alloys Compd 543:43–48. https://doi.org/10.1016/j.jallcom.2012.07.079
Jiang R, Fu Y, Zhu H, et al (2012b) Removal of Methyl Orange from Aqueous Solutions by Magnetic Maghemite / Chitosan Nanocomposite Films : Adsorption Kinetics and Equilibrium. J Appl Polym Sci 125:E540–E549. https://doi.org/10.1002/app.37003
Jeon I-Y, Noh H-J, Baek J-B (2018) Hyperbranched macromolecules: From synthesis to applications. Molecules 23:657
Ghorbani F, Kamari S (2019) Core – shell magnetic nanocomposite of Fe3O4@SiO2@NH2 as an efficient and highly recyclable adsorbent of methyl red dye from aqueous environments. Environ Technol Innov 14:100333. https://doi.org/10.1002/app.37003
Kandisa RV, Saibaba KVN (2016) Dye removal by adsorption: a review. J Bioremediation Biodegrad 07:2155–6199. https://doi.org/10.4172/2155-6199.1000371
Kefeni KK, Mamba BB, Msagati TAM (2017) Application of spinel ferrite nanoparticles in water and wastewater treatment: a review. Sep Purif Technol 188:399–422. https://doi.org/10.1016/j.seppur.2017.07.015
Kumar A, Shalini, Sharma G et al (2017) Facile hetero-assembly of superparamagnetic Fe3O4/BiVO4 stacked on biochar for solar photo-degradation of methyl paraben and pesticide removal from soil. J Photochem Photobiol A Chem 337:118–131. https://doi.org/10.1016/j.jphotochem.2017.01.010
Langmuir I (1918) The adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40:1361–1403
Li Y, Gao H, Wang C, et al (2018) One-step fabrication of chitosan-Fe(OH)3 beads for efficient adsorption of anionic dyes. Int J Biol Macromol 117:30–41. https://doi.org/10.1016/j.ijbiomac.2018.05.137
Lin C-CC, Ho J-MM (2014) Structural analysis and catalytic activity of Fe3O4 nanoparticles prepared by a facile co-precipitation method in a rotating packed bed. Ceram Int 40:10275–10282. https://doi.org/10.1016/j.ceramint.2014.02.119
Lin J, Wang L (2009) Comparison between linear and non-linear forms of pseudo-first-order and pseudo-second-order adsorption kinetic models for the removal of methylene blue by activated carbon. Front Environ Sci Eng China 3:320–324. https://doi.org/10.1007/s11783-009-0030-7
Liu X, Ma Z, Xing J, Liu H (2004) Preparation and characterization of amino-silane modified superparamagnetic silica nanospheres. J Magn Magn Mater 270:1–6. https://doi.org/10.1016/j.jmmm.2003.07.006
Liu SQ, Feng LR, Xu N et al (2012) Magnetic nickel ferrite as a heterogeneous photo-Fenton catalyst for the degradation of rhodamine B in the presence of oxalic acid. Chem Eng J 203:432–439. https://doi.org/10.1016/j.cej.2012.07.071
Liu Y, Li Y, Li X-M, He T (2013) Kinetics of (3-aminopropyl)triethoxylsilane (APTES) silanization of superparamagnetic iron oxide nanoparticles. Langmuir 29:15275–15282. https://doi.org/10.1021/la403269u
Lu Y, Yin Y, Mayers BT, Xia Y (2002) Modifying the surface properties of superparamagnetic iron oxide nanoparticles through a sol-gel approach. Nano Lett 2:183–186. https://doi.org/10.1021/nl015681q
Mahdavi M, Bin AM, Haron MJ et al (2013) Synthesis, surface modification and characterisation of biocompatible magnetic iron oxide nanoparticles for biomedical applications. Molecules 18:7533–7548. https://doi.org/10.3390/molecules18077533
Mazo-Zuluaga J, Barrero CA, Díaz-Terán J, Jerez A (2003) Thermally induced magnetite-haematite transformation. Hyperfine Interact 148–149:153–161. https://doi.org/10.1023/B:HYPE.0000003776.84005.89
Meng C, Zhikun W, Qiang L et al (2018) Preparation of amino-functionalized Fe3O4@mSiO2 core-shell magnetic nanoparticles and their application for aqueous Fe3+ removal. J Hazard Mater 341:198–206. https://doi.org/10.1016/j.jhazmat.2017.07.062
Meroufel B, Benali O, Benyahia M et al (2015) Adsorptive removal of anionic dye from aqueous solutions by mixture of Kaolin and Bentonite clay: characteristics, isotherm, kinetic and thermodynamic studies. Iran J Energy Environ 6:482–491. https://doi.org/10.5829/idosi.ijee.2015.06.02.11
Messina PV, Schulz PC (2006) Adsorption of reactive dyes on titania– silica mesoporous materials. Adsorpt J Int Adsorpt Soc 299:305–320. https://doi.org/10.1016/j.jcis.2006.01.039
Mojić B, Giannakopoulos KP, Cvejić Ž, Srdić VV (2012) Silica coated ferrite nanoparticles: influence of citrate functionalization procedure on final particle morphology. Ceram Int 38:6635–6641. https://doi.org/10.1016/j.ceramint.2012.05.050
Molina L, Gaete J, Alfaro I et al (2018) Synthesis and characterization of magnetite nanoparticles functionalized with organophosphorus compounds and its application as an adsorbent for La (III), Nd (III) and Pr (III) ions from aqueous solutions. J Mol Liq 275:178–191. https://doi.org/10.1016/j.molliq.2018.11.074
Mutneja R, Singh R, Kaur V et al (2016) Schiff base tailed silatranes for the fabrication of functionalized silica based magnetic nano-cores possessing active sites for the adsorption of copper ions. New J Chem 40:1640–1648. https://doi.org/10.1039/c5nj02287h
Naiya TK, Bhattacharya AK, Das SK (2009) Adsorption of Cd(II) and Pb(II) from aqueous solutions on activated alumina. J Colloid Interface Sci 333:14–26. https://doi.org/10.1016/j.jcis.2009.01.003
Pang Y, Zeng G, Tang L et al (2011) Preparation and application of stability enhanced magnetic nanoparticles for rapid removal of Cr(VI). Chem Eng J 175:222–227. https://doi.org/10.1016/j.cej.2011.09.098
Pasternack RM, Amy SR, Chabal YJ (2008) Attachment of 3-(aminopropyl)triethoxysilane on silicon oxide surfaces: dependence on solution temperature. Langmuir 24:12963–12971. https://doi.org/10.1021/la8024827
Petcharoen K, Sirivat A (2012) Synthesis and characterization of magnetite nanoparticles via the chemical co-precipitation method. Mater Sci Eng B Solid-State Mater Adv Technol 177:421–427. https://doi.org/10.1016/j.mseb.2012.01.003
Phan NTS, Jones CW (2006) Highly accessible catalytic sites on recyclable organosilane-functionalized magnetic nanoparticles: an alternative to functionalized porous silica catalysts. J Mol Catal A Chem 253:123–131. https://doi.org/10.1016/j.molcata.2006.03.019
Plueddemann EP (1991) Chemistry of Silane Coupling Agents. Springer
Prasad C, Yuvaraja G, Venkateswarlu P (2017) Biogenic synthesis of Fe3O4 magnetic nanoparticles using Pisum sativum peels extract and its effect on magnetic and Methyl orange dye degradation studies. J Magn Magn Mater 424:376–381. https://doi.org/10.1016/j.jmmm.2016.10.084
Redlich O, Peterson DL (1959) A useful adsorption isotherm. J Phys Chem 63:1024
Saffour Z, Viallier P, Dupuis D (2006) Rheology of gel-like materials in textile printing. Rheol Acta 45:479–485. https://doi.org/10.1007/s00397-005-0079-6
Sakızcı M, Özer M (2019) The characterization and methane adsorption of Ag-, Cu-, Fe-, and H-exchanged chabazite-rich tuff from Turkey. Environ Sci Pollut Res 26:16616–16627. https://doi.org/10.1007/s11356-019-04996-4
Salem IA, Salem MA, El-Ghobashy MA (2017) The dual role of ZnO nanoparticles for efficient capture of heavy metals and Acid blue 92 from water. J Mol Liq 248:527–538. https://doi.org/10.1016/j.molliq.2017.10.060
Sheng W, Wei W, Li J et al (2016) Amine-functionalized magnetic mesoporous silica nanoparticles for DNA separation. Appl Surf Sci 387:1116–1124. https://doi.org/10.1016/j.apsusc.2016.07.061
Singh NB, Nagpal G, Agrawal S, Rachna (2018) Water purification by using adsorbents: a review. Environ Technol Innov 11:187–240. https://doi.org/10.1016/j.eti.2018.05.006
Stöber W, Fink A, Bohn E (1968) Controlled growth of monodisperse silica spheres in the micron size range. J Colloid Interface Sci 26:62–69. https://doi.org/10.1016/0021-9797(68)90272-5
Sun Y, Duan L, Guo Z et al (2005) An improved way to prepare superparamagnetic magnetite-silica core-shell nanoparticles for possible biological application. J Magn Magn Mater 285:65–70. https://doi.org/10.1016/j.jmmm.2004.07.016
Sun X, Yang L, Li Q et al (2014) Amino-functionalized magnetic cellulose nanocomposite as adsorbent for removal of Cr(VI): synthesis and adsorption studies. Chem Eng J 241:175–183. https://doi.org/10.1016/j.cej.2013.12.051
Temkin MJ (1963) V. Pyzhev Recent modifications to Langmuir isotherms. Acta Physicochim USSR, 12, 1940, 217-222 Weber Morris
Ulu A, Ozcan I, Koytepe S, Ates B (2018) Design of epoxy-functionalized Fe3O4@MCM-41 core–shell nanoparticles for enzyme immobilization. Int J Biol Macromol 115:1122–1130. https://doi.org/10.1016/j.ijbiomac.2018.04.157
Vojoudi H, Badiei A, Bahar S et al (2017) A new nano-sorbent for fast and efficient removal of heavy metals from aqueous solutions based on modification of magnetic mesoporous silica nanospheres. J Magn Magn Mater 441:193–203. https://doi.org/10.1016/j.jmmm.2017.05.065
von Gunten U (2003) Ozonation of drinking water: part I. Oxidation kinetics and product formation. Water Res 37:1443–1467. https://doi.org/10.1016/S0043-1354(02)00457-8
Yang H, Feng Q (2010) Characterization of pore-expanded amino-functionalized mesoporous silicas directly synthesized with dimethyldecylamine and its application for decolorization of sulphonated azo dyes. J Hazard Mater 180:106–114. https://doi.org/10.1016/j.jhazmat.2010.03.116
Yang X, Chen W, Huang J et al (2015) Rapid degradation of methylene blue in a novel heterogeneous Fe3O4@rGO@TiO2-catalyzed photo-Fenton system. Sci Rep 5:10632. https://doi.org/10.1038/srep10632
Zhang P, Wang L (2010) Extended Langmuir equation for correlating multilayer adsorption equilibrium data. Sep Purif Technol 70:367–371. https://doi.org/10.1016/j.seppur.2009.10.007
Zhang B, Xing J, Lang Y, Liu H (2008) Synthesis of amino-silane modified magnetic silica adsorbents and application for adsorption of flavonoids from Glycyrrhiza uralensis Fisch. Sci China, Ser B Chem 51:145–151. https://doi.org/10.1007/s11426-007-0104-y
Zhang X, Hu Y, Yunxia Liu BC (2011) Je Sc Sc 23:601–606. https://doi.org/10.1016/S1001-0742(08)62314-1
Zhang S, Zhang Y, Liu J et al (2013) Thiol modified Fe3O4@SiO2 as a robust, high effective, and recycling magnetic sorbent for mercury removal. Chem Eng J 226:30–38. https://doi.org/10.1016/j.cej.2013.04.060
Zhao SY, Don KL, Chang WK et al (2006) Synthesis of magnetic nanoparticles of Fe3O4and CoFe2O4 and their surface modification by surfactant adsorption. Bull Korean Chem Soc 27:237–242. https://doi.org/10.5012/bkcs.2006.27.2.237
The authors would like to thank Tanta University for financial support of this study under the project number (TU-03-16).
1. The as-prepared magnetite showed polycrystalline structure.
2. Coating of Fe3O4 with silica layer enhanced their surface area and adsorption capacity.
3. The adsorbent surface was simply separated.
4. The adsorption mechanisms of the dyes under study involve hydrogen bonding and electrostatic interactions.
5. The adsorption process is greatly improved at low temperature (exothermic process).
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Responsible editor: Tito Roberto Cadaval Jr
About this article
Cite this article
Gemeay, A.H., Keshta, B.E., El-Sharkawy, R.G. et al. Chemical insight into the adsorption of reactive wool dyes onto amine-functionalized magnetite/silica core-shell from industrial wastewaters. Environ Sci Pollut Res 27, 32341–32358 (2020). https://doi.org/10.1007/s11356-019-06530-y
- Reactive dyes
- Wastewater treatment