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Frontiers of Materials Science

ISSN 2095-025X

ISSN 2095-0268(Online)

CN 11-5985/TB

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Front. Mater. Sci.    2018, Vol. 12 Issue (1) : 34-44    https://doi.org/10.1007/s11706-018-0412-5
RESEARCH ARTICLE
Heterogeneous Fenton-like discoloration of methyl orange using Fe3O4/MWCNTs as catalyst: kinetics and Fenton-like mechanism
Huan-Yan XU(), Yuan WANG, Tian-Nuo SHI, Hang ZHAO, Qu TAN, Bo-Chao ZHAO, Xiu-Lan HE, Shu-Yan QI
School of Materials Science and Engineering, Harbin University of Science and Technology, Harbin 150040, China
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Abstract

The kinetics and Fenton-like mechanism are two challenging tasks for heterogeneous Fenton-like catalytic oxidation of organic pollutants. In this study, three kinetic models were used for the kinetic studies of Fe3O4/MWCNTs-H2O2 Fenton-like reaction for MO degradation. The results indicated that this reaction followed the first-order kinetic model. The relationship of reaction rate constant and temperature followed the Arrhenius equation. The activation energy and frequency factor of this system were calculated as 8.2 kJ·mol−1 and 2.72 s−1, respectively. The quantifications of Fe ions dissolution and ?OH radicals generation confirmed that the homogeneous and heterogeneous catalyses were involved in Fe3O4/MWCNTs-H2O2 Fenton-like reaction. The reaction rate constant was closely related with Fe ions dissolution and ?OH radicals generation. Fe3O4/MWCNTs nanocomposites had typical ferromagnetic property and could be easily separated from solution by an external magnet after being used. Furthermore, Fe3O4/MWCNTs nanocomposites exhibited good stability and recyclability. Finally, the Fenton-like mechanisms on homogeneous and heterogeneous catalyses were described.
Keywords MWCNTs      Fe3O4 NPs      kinetics      ?OH radicals      Fenton-like mechanism     
Corresponding Author(s): Huan-Yan XU   
Online First Date: 02 February 2018    Issue Date: 07 March 2018
 Cite this article:   
Huan-Yan XU,Yuan WANG,Tian-Nuo SHI, et al. Heterogeneous Fenton-like discoloration of methyl orange using Fe3O4/MWCNTs as catalyst: kinetics and Fenton-like mechanism[J]. Front. Mater. Sci., 2018, 12(1): 34-44.
 URL:  
https://academic.hep.com.cn/foms/EN/10.1007/s11706-018-0412-5
https://academic.hep.com.cn/foms/EN/Y2018/V12/I1/34
Fig.1  Scheme 1&chsp;Hydroxylation reaction of SA as the probe molecule for detection of •OH radicals.
MO concentration
/(mg·L−1)		 H2O2 concentration
/(mmol·L−1)		 Catalyst dosage
/(g·L−1)		 Temperature/K pH First order Second order BMG
k1 adj.R2 k2 adj.R2 m b adj.R2
50 19.38 2 293 1 0.0888 0.9552 0.0363 0.8291 27.8205 0.4378 0.4104
50 19.38 2 293 2 0.0943 0.9545 0.0490 0.8237 25.8592 0.4713 0.4338
50 19.38 2 293 3 0.0702 0.9388 0.0132 0.8491 46.4999 0.0901 0.2147
50 19.38 2 293 4 0.0601 0.8884 0.0090 0.5916 84.6027 −0.5537 0.3261
50 19.38 2 293 5 0.0256 0.8942 0.0011 0.7717 136.006 −1.1163 0.8300
50 9.69 2 293 2 0.0844 0.9578 0.0283 0.7901 46.0899 0.0570 0.2435
50 19.38 2 293 2 0.0943 0.9545 0.0490 0.8237 25.8592 0.4713 0.4338
50 29.07 2 293 2 0.0708 0.9511 0.0147 0.6713 70.3582 −0.3913 0.0247
50 38.76 2 293 2 0.0636 0.9389 0.0099 0.7217 74.1351 −0.4334 0.0775
50 48.45 2 293 2 0.0584 0.9072 0.0076 0.6664 131.340 −1.5645 0.4670
50 19.38 1 293 2 0.0818 0.9317 0.0233 0.6809 128.723 −1.6327 0.3049
50 19.38 2 293 2 0.0943 0.9545 0.0490 0.8237 25.8592 0.4713 0.4338
50 19.38 3 293 2 0.0978 0.9716 0.0695 0.7189 15.4185 0.6870 0.8476
50 19.38 4 293 2 0.0999 0.9482 0.0913 0.7972 8.38025 0.8299 0.9569
50 19.38 5 293 2 0.1200 0.9685 0.3239 0.6121 4.30795 0.9121 0.9914
50 19.38 2 293 2 0.0943 0.9545 0.0490 0.8237 25.8592 0.4713 0.4338
50 19.38 2 303 2 0.1002 0.9209 0.0764 0.5130 15.3699 0.6896 0.8774
50 19.38 2 313 2 0.1244 0.9590 0.3471 0.6092 7.26785 0.8551 0.9863
50 19.38 2 323 2 0.1261 0.9324 0.3427 0.5859 0.82664 0.9853 0.9999
50 19.38 2 333 2 0.1391 0.9659 0.4117 0.5947 0.25183 0.9960 1.0000
10 19.38 2 293 2 0.1240 0.9293 1.1519 0.7215 1.02254 0.9809 0.9999
30 19.38 2 293 2 0.1008 0.9730 0.1324 0.6527 17.2043 0.6512 0.8272
50 19.38 2 293 2 0.0943 0.9545 0.0363 0.8291 25.8592 0.4713 0.4338
70 19.38 2 293 2 0.0658 0.9780 0.0089 0.6809 41.9439 0.1936 0.1108
90 19.38 2 293 2 0.0596 0.9541 0.0048 0.7293 58.1683 −0.1193 0.2245
Tab.1  Kinetic parameters of three models and their adjusted correlation coefficients (adj.R2)
Fig.2  The linear regression analysis to lnk1 versus 103/T.
Fig.3  Fe dissolution (bar chart) and •OH generation (line graph) at different solution pHs in Fe3O4/MWCNTs-H2O2 Fenton-like reaction (experimental conditions: [MO]0 = 50 mg·L−1, [H2O2]0 = 19.38 mmol·L−1, catalyst dosage= 2 g·L−1, t = 30 min and T = 293 K).
Fig.4  Fe dissolution (bar chart) and •OH generation (line graph) with different initial H2O2 concentrations in Fe3O4/MWCNTs-H2O2 Fenton-like reaction (experimental conditions: [MO]0 = 50 mg·L−1, pH= 2, catalyst dosage= 2 g·L−1, t = 30 min and T = 293 K).
Fig.5  Fe dissolution (bar chart) and •OH generation (line graph) with different catalyst dosages in Fe3O4/MWCNTs-H2O2 Fenton-like reaction (experimental conditions: [MO]0 = 50 mg·L−1, pH= 2, [H2O2]0 = 19.38 mmol·L−1, t = 30 min and T = 293 K).
Fig.6  Fe dissolution (bar chart) and •OH generation (line graph) at different reaction temperatures in Fe3O4/MWCNTs-H2O2 Fenton-like reaction (experimental conditions: [MO]0 = 50 mg·L−1, pH= 2, [H2O2]0 = 19.38 mmol·L−1, catalyst dosage= 2 g·L−1 and t = 30 min).
Fig.7  Magnetization curves of Fe3O4 NPs and Fe3O4/MWCNTs nanocomposites (inset: magnetic separation of Fe3O4/MWCNTs nanocomposites from solution after being used).
Fig.8  Cycling tests on MO degradation (bar chart) and weight loss of Fe3O4/MWCNTs (line graph) in Fe3O4/MWCNTs-H2O2 Fenton-like reaction (experimental conditions: [MO]0 = 50 mg·L−1, pH= 2, [H2O2]0 = 19.38 mmol·L−1, catalyst dosage= 2 g·L−1, t = 60 min and T = 293 K).
Fig.9  Contrast experiments on the removal of 50 mg·L−1 MO at pH= 2 and room temperature in different systems (the dosage of solid material is 2.0 g·L−1, and if needed, the initial H2O2 concentration is 19.38 mmol·L−1).
Fig.10  UV-vis absorption spectra and digital images (inset) of MO solution after different periods during the Fenton-like reaction (experimental conditions: pH 2.0, initial MO concentration 50 mg·L−1, catalyst dosage 2.0 g·L−1, initial H2O2 concentration 19.38 mmol·L−1, and room temperature).
Fig.11  Fenton-like mechanisms on homogeneous and heterogeneous catalyses in the Fe3O4/MWCNTs-H2O2 system.
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