Abstract
Fe3O4/MWCNTs nanocomposites were prepared by chemical oxidation coprecipitation method and developed as highly efficient heterogeneous Fenton-like catalyst. XRD results revealed that Fe3O4 nanoparticles deposited onto MWCNTs surface remained the inverse spinel crystal structure of cubic Fe3O4 phase. The FTIR characteristic peaks of MWCNTs weakened or disappeared due to the anchor of Fe3O4 nanoparticles and Fe–O peak at 570 cm–1 was indicative of the formation of Fe3O4. TEM observation revealed that Fe3O4 nanoparticles were tightly anchored by MWCNTs. The Fenton-like catalytic activity of Fe3O4/MWCNTs nanocomposites for the discoloration of methyl orange (MO) was much higher than that of Fe3O4 nanoparticles. The process optimization of this heterogeneous Fenton-like system was implemented by response surface methodology (RSM). The optimum conditions for MO discoloration were determined to be of 12.3 mmol/L H2O2 concentration, 2.9 g/L catalyst dosage, solution pH 2.7 and 39.3 min reaction time, with the maximum predicted value for MO discoloration ratio of 101.85%. The corresponding experimental value under the identical conditions was obtained as 99.86%, which was very close to the predicted one with the absolute deviation of 1.99%.
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References
Konstantinou I K, Albanis T A. TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations–A review. Applied Catalysis B: Environmental, 2004, 49(1): 1–14
Das L, Chatterjee S, Naik D B, et al. Role of surfactant derived intermediates in the efficacy and mechanism for radiation chemical degradation of a hydrophobic azo dye, 1-phenylazo-2-naphthol. Journal of Hazardous Materials, 2015, 298: 19–27
Das D, Dutta R K. A novel method of synthesis of small band gap SnS nanorods and its efficient photocatalytic dye degradation. Journal of Colloid and Interface Science, 2015, 457: 339–344
Nie Y, Zhang L, Li Y-Y, et al. Enhanced Fenton-like degradation of refractory organic compounds by surface complex formation of LaFeO3 and H2O2. Journal of Hazardous Materials, 2015, 294: 195–200
Chen H, Zhang Z L, Yang Z L, et al. Heterogeneous Fenton-like catalytic degradation of 2,4-dichlorophenoxyacetic acid in water with FeS. Chemical Engineering Journal, 2015, 273: 481–489
Xue X, Hanna K, Deng N. Fenton-like oxidation of rhodamine B in the presence of two types of iron (II, III) oxide. Journal of Hazardous Materials, 2009, 166(1): 407–414
Rusevova K, Kopinke F D, Georgi A. Nano-sized magnetic iron oxides as catalysts for heterogeneous Fenton-like reactions–Influence of Fe(II)/Fe(III) ratio on catalytic performance. Journal of Hazardous Materials, 2012, 241-242: 433–440
Xu L J, Wang J L. Fenton-like degradation of 2,4-dichlorophenol using Fe3O4 magnetic nanoparticles. Applied Catalysis B: Environmental, 2012, 123-124: 117–126
Gao L, Zhuang J, Nie L, et al. Intrinsic peroxidase-like activity of ferromagnetic nanoparticles. Nature Nanotechnology, 2007, 2(9): 577–583
Wan D, Li W B, Wang G H, et al. Adsorption and heterogeneous degradation of rhodamine B on the surface of magnetic bentonite material. Applied Surface Science, 2015, 349: 988–996
Hammouda S B, Adhoum N, Monser L. Synthesis of magnetic alginate beads based on Fe3O4 nanoparticles for the removal of 3-methylindole from aqueous solution using Fenton process. Journal of Hazardous Materials, 2015, 294: 128–136
Seyed Dorraji M S, Mirmohseni A, Carraro M, et al. Fenton-like catalytic activity of wet-spun chitosan hollow fibers loaded with Fe3O4 nanoparticles: Batch and continuous flow investigations. Journal of Molecular Catalysis A: Chemical, 2015, 398: 353–357
Cleveland V, Bingham J P, Kan E. Heterogeneous Fenton degradation of bisphenol A by carbon nanotube-supported Fe3O4. Separation and Purification Technology, 2014, 133: 388–395
Deng J H, Wen X H, Wang Q N. Solvothermal in situ synthesis of Fe3O4-multiwalled carbon nanotubes with enhanced heterogeneous Fenton-like activity. Materials Research Bulletin, 2012, 47 (11): 3369–3376
Hu X B, Deng Y H, Gao Z Q, et al. Transformation and reduction of androgenic activity of 17α-methyltestosterone in Fe3O4/MWCNTs–H2O2 system. Applied Catalysis B: Environmental, 2012, 127: 167–174
Zhou L C, Zhang H, Ji L Q, et al. Fe3O4/MWCNT as a heterogeneous Fenton catalyst: degradation pathways of tetrabromobisphenol A. RSC Advances, 2014, 4(47): 24900–24908
Yu L, Yang X F, Ye Y S, et al. Efficient removal of atrazine in water with a Fe3O4/MWCNTs nanocomposite as a heterogeneous Fenton-like catalyst. RSC Advances, 2015, 5(57): 46059–46066
Tristão J C, de Mendonça F G, Lago R M, et al. Controlled formation of reactive Fe particles dispersed in a carbon matrix active for the oxidation of aqueous contaminants with H2O2. Environmental Science and Pollution Research International, 2015, 22(2): 856–863
Zhang J K, Wang G J, Zhang L P, et al. Catalytic oxidative desulfurization of benzothiophene with hydrogen peroxide catalyzed by Fenton-like catalysts. Reaction Kinetics, Mechanisms and Catalysis, 2014, 113(2): 347–360
Hua Z, Ma W, Bai X, et al. Heterogeneous Fenton degradation of bisphenol A catalyzed by efficient adsorptive Fe3O4/GO nanocomposites. Environmental Science and Pollution Research International, 2014, 21(12): 7737–7745
Zubir N A, Yacou C, Motuzas J, et al. The sacrificial role of graphene oxide in stabilising a Fenton-like catalyst GO–Fe3O4. Chemical Communications, 2015, 51(45): 9291–9293
Zubir N A, Zhang XW, Yacou C, et al. Fenton-like degradation of acid Orange 7 using graphene oxide–iron oxide nanocomposite. Science of Advanced Materials, 2014, 6(7): 1382–1388
Buang N A, Fadil F, Majid Z A, et al. Characteristic of mild acid functionalized multiwalled carbon nanotubes towards high dispersion with low structural defects. Digest Journal of Nanomaterials and Biostructures, 2012, 7: 33–39
Aboutalebi S H, Chidembo A T, Salari M, et al. Comparison of GO, GO/MWCNTs composite and MWCNTs as potential electrode materials for supercapacitors. Energy & Environmental Science, 2011, 4(5): 1855–1865
Gulkaya I, Surucu G A, Dilek F B. Importance of H2O2/Fe2+ ratio in Fenton’s treatment of a carpet dyeing wastewater. Journal of Hazardous Materials, 2006, 136(3): 763–769
Gil Pavas E, Dobrosz-Gómez I, Gómez-García M Á. Decolorization and mineralization of Diarylide Yellow 12 (PY12) by photo-Fenton process: the Response Surface Methodology as the optimization tool. Water Science and Technology, 2012, 65(10): 1795–1800
Khataee A R, Safarpour M, Zarei M, et al. Combined heterogeneous and homogeneous photodegradation of a dye using immobilized TiO2 nanophotocatalyst and modified graphite electrode with carbon nanotubes. Journal of Molecular Catalysis A: Chemical, 2012, 363–364: 58–68
Ghanbarzadeh Lak M, Sabour M R, Amiri A, et al. Application of quadratic regression model for Fenton treatment of municipal landfill leachate. Waste Management, 2012, 32(10): 1895–1902
Cao M S, Yang J, Song W L, et al. Ferroferric oxide/multiwalled carbon nanotube vs polyaniline/ferroferric oxide/multiwalled carbon nanotube multiheterostructures for highly effective micro-wave absorption. ACS Applied Materials & Interfaces, 2012, 4 (12): 6949–6956
Chen Y X, Gu H C. Microwave assisted fast fabrication of Fe3O4–MWCNTs nanocomposites and their application as MRI contrast agents. Materials Letters, 2012, 67(1): 49–51
Hu X B, Liu B Z, Deng Y H, et al. Adsorption and heterogeneous Fenton degradation of 17a-methyltestosterone on nano Fe3O4/MWCNTs in aqueous solution. Applied Catalysis B: Environmental, 2011, 107(3–4): 274–283
Chen J H, Lu D Q, Chen B, et al. Removal of U(VI) from aqueous solutions by using MWCNTs and chitosan modified MWCNTs. Journal of Radioanalytical and Nuclear Chemistry, 2013, 295(3): 2233–2241
Abdullahi N, Saion E, Shaari A H, et al. Optimisation of the photonic efficiency of TiO2 decorated on MWCNTs for Methylene Blue photodegradation. PLoS ONE, 2015, 10(5): e0125511
Stobinski L, Lesiak B, Kövér L, et al. Multiwall carbon nanotubes purification and oxidation by nitric acid studied by the FTIR and electron spectroscopy methods. Journal of Alloys and Compounds, 2010, 501(1): 77–84
Wang J, Li Z, Li S, et al. Adsorption of Cu(II) on oxidized multiwalled carbon nanotubes in the presence of hydroxylated and carboxylated fullerenes. PLoS ONE, 2013, 8(8): e72475
Xiao D L, Dramou P, He H, et al. Magnetic carbon nanotubes: synthesis by a simple solvothermal process and application in magnetic targeted drug delivery system. Journal of Nanoparticle Research, 2012, 14(7): 984–995
Azami M, Bahram M, Nouri S, et al. A central composite design for the optimization of the removal of the azo dye, methyl orange, from waste water using the Fenton reaction. Journal of the Serbian Chemical Society, 2012, 77(2): 235–246
Idel-aouad R, Valiente M, Yaacoubi A, et al. Rapid decolourization and mineralization of the azo dye C.I. Acid Red 14 by heterogeneous Fenton reaction. Journal of Hazardous Materials, 2011, 186(1): 745–750
Xu H Y, Shi T N, Wu L C, et al. Discoloration of methyl orange in the presence of schorl and H2O2: Kinetics and mechanism. Water, Air, and Soil Pollution, 2013, 224(10): 1740
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Xu, HY., Shi, TN., Zhao, H. et al. Heterogeneous Fenton-like discoloration of methyl orange using Fe3O4/MWCNTs as catalyst: process optimization by response surface methodology. Front. Mater. Sci. 10, 45–55 (2016). https://doi.org/10.1007/s11706-016-0326-z
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DOI: https://doi.org/10.1007/s11706-016-0326-z