Heterogeneous Fenton-like discoloration of methyl orange using Fe<sub>3</sub>O<sub>4</sub>/MWCNTs as catalyst: combination mechanism and affecting parameters

doi:10.1007/s11706-018-0408-1

Front. Mater. Sci.

2018, Vol. 12

Issue (1) : 21-33 https://doi.org/10.1007/s11706-018-0408-1

RESEARCH ARTICLE

Heterogeneous Fenton-like discoloration of methyl orange using Fe₃O₄/MWCNTs as catalyst: combination mechanism and affecting parameters

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

Download: PDF(702 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

Multi-walled carbon nanotubes (MWCNTs) can act not only as a support for Fe₃O₄ nanoparticles (NPs) but also as a coworker with synergistic effect, accordingly improving the heterogeneous Fenton-like efficiency of Fe₃O₄ NPs. In this study, Fe₃O₄ NPs were in situ anchored onto MWCNTs by a moderate co-precipitation method and the as-prepared Fe₃O₄/MWCNTs nanocomposites were employed as the highly efficient Fenton-like catalysts. The analyses of XRD, FTIR, Raman, FESEM, TEM and HRTEM results indicated the formation of Fe₃O₄ crystals in Fe₃O₄/MWCNTs nanocomposites prepared at different conditions and the interaction between Fe₃O₄ NPs and MWCNTs. Over a wide pH range, the surface of modified MWCNTs possessed negative charges. Based on these results, the possible combination mechanism between Fe₃O₄ NPs and MWCNTs was discussed and proposed. Moreover, the effects of preparation and catalytic conditions on the Fenton-like catalytic efficiency were investigated in order to gain further insight into the heterogeneous Fenton-like reaction catalyzed by Fe₃O₄/MWCNTs nanocomposites.

Keywords MWCNTs Fe₃O₄ NPs Fenton-like catalyst combination mechanism affecting parameters

Corresponding Author(s): Huan-Yan XU

Online First Date: 11 January 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: combination mechanism and affecting parameters[J]. Front. Mater. Sci., 2018, 12(1): 21-33.

URL:

https://academic.hep.com.cn/foms/EN/10.1007/s11706-018-0408-1
https://academic.hep.com.cn/foms/EN/Y2018/V12/I1/21

Fig.1 XRD patterns: (a) modified MWCNTs, Fe₃O₄ NPs, and Fe₃O₄/MWCNTs nanocomposites with different MWCNTs contents; (b) Fe₃O₄/MWCNTs nanocomposites prepared at different temperatures; (c) Fe₃O₄/MWCNTs nanocomposites prepared with different reaction times.

Fig.2 FTIR spectra of Fe₃O₄ NPs, MWCNTs, modified MWCNTs, and Fe₃O₄/MWCNTs nanocomposite (FC-20CW).

Fig.3 Raman spectra of Fe₃O₄ NPs, MWCNTs, modified MWCNTs, and Fe₃O₄/MWCNTs nanocomposite (FC-20CW).

Fig.4 FESEM images of MWCNTs, modified MWCNTs, Fe₃O₄ NPs, and Fe₃O₄/MWCNTs nanocomposites prepared at different conditions.

Fig.5 (a) TEM and (b) HRTEM images of modified MWCNTs, (c) TEM image of Fe₃O₄ NPs, and (d) TEM image of Fe₃O₄/MWCNTs nanocomposite (inset: SAED of Fe₃O₄ NPs anchored onto MWCNTs).

Fig.6 Zeta potentials of modified MWCNTs at different pH values.

Fig.7 Combination mechanism between modified MWCNTs and Fe₃O₄ NPs.

Fig.8 Effect of MWCNTs content on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.9 Effect of water-bath temperature on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.10 Effect of water-bath time on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.11 Effect of solution pH on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.12 Effect of H₂O₂ concentration on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.13 Effect of catalyst dosage on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.14 Effect of catalytic temperature on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

Fig.15 Effect of initial MO concentration on Fenton-like efficiency of Fe₃O₄/MWCNTs nanocomposite.

1	Cai Z Q, Sun Y M, Liu W, et al.. An overview of nanomaterials applied for removing dyes from wastewater. Environmental Science and Pollution Research International, 2017, 24(19): 15882–15904 https://doi.org/10.1007/s11356-017-9003-8
2	Freyria F S, Armandi M, Compagnoni M, et al.. Catalytic and photocatalytic processes for the abatement of N-containing pollutants from wastewater. Part 2: organic pollutants. Journal of Nanoscience and Nanotechnology, 2017, 17(6): 3654–3672 https://doi.org/10.1166/jnn.2017.14014
3	Holkar C R, Jadhav A J, Pinjari D V, et al.. A critical review on textile wastewater treatments: possible approaches. Journal of Environmental Management, 2016, 182: 351–366 https://doi.org/10.1016/j.jenvman.2016.07.090
4	Quadrado R F N, Fajardo A R. Fast decolorization of azo methyl orange via heterogeneous Fenton and Fenton-like reactions using alginate-Fe2+/Fe3+ films as catalysts. Carbohydrate Polymers, 2017, 177: 443–450 https://doi.org/10.1016/j.carbpol.2017.08.083
5	Feng J X, Li S Y, Sheng Y, et al.. Remarkable improvement of cycling Fenton process for catalytic degradation of phenol: tuning of triggering effect. Applied Catalysis A: General, 2017, 542: 21–27 https://doi.org/10.1016/j.apcata.2017.05.009
6	Clarizia L, Russo D, Somma D I, et al.. Homogeneous photo-Fenton processes at near neutral pH: a review. Applied Catalysis B: Environmental, 2017, 209: 358–371 https://doi.org/10.1016/j.apcatb.2017.03.011
7	Mirzaei A, Chen Z, Haghighat F, et al.. Removal of pharmaceuticals from water by homo/heterogonous Fenton-type processes: a review. Chemosphere, 2017, 174: 665–688 https://doi.org/10.1016/j.chemosphere.2017.02.019
8	Teixeira A P C, Tristão J C, Araujo M H, et al.. Iron: a versatile element to produce materials for environmental applications. Journal of the Brazilian Chemical Society, 2012, 23(9): 1579–1593 https://doi.org/10.1590/S0103-50532012005000039
9	Yang S, Wu P, Yang Q, et al.. Regeneration of iron-montmorillonite adsorbent as an efficient heterogeneous Fenton catalytic for degradation of Bisphenol A: structure, performance and mechanism. Chemical Engineering Journal, 2017, 328: 737–747 https://doi.org/10.1016/j.cej.2017.07.093
10	Abass O K, Zhuo M S, Zhang K S. Concomitant degradation of complex organics and metals recovery from fracking wastewater: roles of nanozerovalent iron initiated oxidation and adsorption. Chemical Engineering Journal, 2017, 328: 159–171 https://doi.org/10.1016/j.cej.2017.07.030
11	Zhong Y H, Yu L, Chen Z F, et al.. Microwave-assisted synthesis of Fe3O4 nanocrystals with predominantly exposed facets and their heterogeneous UVA/Fenton catalytic activity. ACS Applied Materials & Interfaces, 2017, 9(34): 29203–29212 https://doi.org/10.1021/acsami.7b06925
12	Liu Y Y, Jin W, Zhao Y P, et al.. Enhanced catalytic degradation of methylene blue by α-Fe2O3/graphene oxide via heterogeneous photo-Fenton reactions. Applied Catalysis B: Environmental, 2017, 206: 642–652 https://doi.org/10.1016/j.apcatb.2017.01.075
13	Wang Y, Fang J S, Crittenden J C, et al.. Novel RGO/α-FeOOH supported catalyst for Fenton oxidation of phenol at a wide pH range using solar-light-driven irradiation. Journal of Hazardous Materials, 2017, 329: 321–329 doi:10.1016/j.jhazmat.2017.01.041
14	Xiao F, Li W T, Fang L P, et al.. Synthesis of akageneite (β-FeOOH)/reduced graphene oxide nanocomposites for oxidative decomposition of 2-chlorophenol by Fenton-like reaction. Journal of Hazardous Materials, 2016, 308: 11–20 https://doi.org/10.1016/j.jhazmat.2016.01.011
15	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 https://doi.org/10.1016/j.apcatb.2012.04.028
16	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 https://doi.org/10.1016/j.jhazmat.2012.09.068
17	Li K Y, Zhao Y Q, Song C S, et al.. Magnetic ordered mesoporous Fe3O4/CeO2 composites with synergy of adsorption and Fenton catalysis. Applied Surface Science, 2017, 425: 526–534 https://doi.org/10.1016/j.apsusc.2017.07.041
18	Haber F, Weiss J. The catalytic decomposition of hydrogen peroxide by iron salts. Proceedings of the Royal Society, 1934, 147(861): 332–351 https://doi.org/10.1098/rspa.1934.0221
19	Ribeiro R S, Silva A M T, Tavares P B, et al.. Hybrid magnetic graphitic nanocomposites for catalytic wet peroxide oxidation applications. Catalysis Today, 2017, 280: 184–191 https://doi.org/10.1016/j.cattod.2016.04.040
20	Tian X, Jin H, Nie Y, et al.. Heterogeneous Fenton-like degradation of ofloxacin over a wide pH range of 3.6‒10.0 over modified mesoporous iron oxide. Chemical Engineering Journal, 2017, 328: 397–405 https://doi.org/10.1016/j.cej.2017.07.049
21	Tang X K, Feng Q M, Liu K, et al.. Fabrication of magnetic Fe3O4/silica nanofiber composites with enhanced Fenton-like catalytic performance for Rhodamine B degradation. Journal of Materials Science, 2018, 53(1): 369–384 https://doi.org/10.1007/s10853-017-1490-y
22	Zhou Z Y, Su M H, Shih K M. Highly efficient and recyclable graphene oxide‒magnetite composites for isatin mineralization. Journal of Alloys and Compounds, 2017, 725: 302–309 https://doi.org/10.1016/j.jallcom.2017.07.087
23	Xu H Y, Shi T N, Zhao H, et al.. Heterogeneous Fenton-like discoloration of methyl orange using Fe3O4/MWCNTs as catalyst: process optimization by response surface methodology. Frontiers of Materials Science, 2016, 10(1): 45–55 https://doi.org/10.1007/s11706-016-0326-z
24	Jafari A J, Kakavandi B, Jaafarzadeh N, et al.. Fenton-like catalytic oxidation of tetracycline by AC@Fe3O4 as a heterogeneous persulfate activator: adsorption and degradation studies. Journal of Industrial and Engineering Chemistry, 2017, 45: 323–333 https://doi.org/10.1016/j.jiec.2016.09.044
25	Zhao H, Weng L, Cui W W, et al.. In situ anchor of magnetic Fe3O4 nanoparticles onto natural maifanite as efficient heterogeneous Fenton-like catalyst. Frontiers of Materials Science, 2016, 10(3): 300–309 https://doi.org/10.1007/s11706-016-0346-8
26	Wan D, Wang G H, Li W B, et al.. Investigation into the morphology and structure of magnetic bentonite nanocomposites with their catalytic activity. Applied Surface Science, 2017, 413: 398–407 https://doi.org/10.1016/j.apsusc.2017.03.265
27	Ribeiro R S, Silva A M T, Figueiredo J L, et al.. Catalytic wet peroxide oxidation: a route towards the application of hybrid magnetic carbon nanocomposites for the degradation of organic pollutants. A review. Applied Catalysis B: Environmental, 2016, 187: 428–460 https://doi.org/10.1016/j.apcatb.2016.01.033
28	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 https://doi.org/10.1016/j.materresbull.2012.07.021
29	Tian X, Liu Y, Chi W, et al.. Catalytic degradation of phenol and p-nitrophenol using Fe3O4/MWCNT nanocomposites as heterogeneous Fenton-like catalyst. Water, Air, and Soil Pollution, 2017, 228(8): 297 https://doi.org/10.1007/s11270-017-3485-3
30	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 https://doi.org/10.1039/c1ee01039e
31	Hu X B, Liu B Z, Deng Y H, et al.. Adsorption and heterogeneous Fenton degradation of 17α-methyltestosterone on nano Fe3O4/MWCNTs in aqueous solution. Applied Catalysis B: Environmental, 2011, 107(3‒4): 274–283 https://doi.org/10.1016/j.apcatb.2011.07.025
32	Xu H Y, Zheng Z, Mao G J. Enhanced photocatalytic discoloration of acid fuchsine wastewater by TiO2/schorl composite catalyst. Journal of Hazardous Materials, 2010, 175(1‒3): 658–665 https://doi.org/10.1016/j.jhazmat.2009.10.059
33	Zubir N A, Motuzas J, Yacou C, et al.. Graphene oxide with zinc partially substituted magnetite (GO-Fe1−xZnxOy) for the UV-assisted heterogeneous Fenton-like reaction. RSC Advances, 2016, 6(50): 44749–44757 https://doi.org/10.1039/C6RA04068C
34	Wang X, Zhao Z, Qu J, et al.. Fabrication and characterization of magnetic Fe3O4‒CNT composites. Journal of Physics and Chemistry of Solids, 2010, 71(4): 673–676 https://doi.org/10.1016/j.jpcs.2009.12.063
35	Wang H, Jiang H, Wang S, et al.. Fe3O4‒MWCNT magnetic nanocomposites as efficient peroxidase mimic catalysts in a Fenton-like reaction for water purification without pH limitation. RSC Advances, 2014, 4(86): 45809–45815 https://doi.org/10.1039/C4RA07327D
36	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 https://doi.org/10.1016/j.jallcom.2010.04.032
37	Song S, Rao R, Yang H, et al.. Facile synthesis of Fe3O4/MWCNTs by spontaneous redox and their catalytic performance. Nanotechnology, 2010, 21(18): 185602 https://doi.org/10.1088/0957-4484/21/18/185602
38	Yu L, Yang X, Ye Y, 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 https://doi.org/10.1039/C5RA04249F
39	Shamsudin M S, Asli N A, Abdullah S, et al.. Effect of synthesis temperature on the growth iron-filled carbon nanotubes as evidenced by structural, micro-Raman, and thermogravimetric analyses. Advances in Condensed Matter Physics, 2012, 420619 (7 pages) doi.org/10.1155/2012/420619
40	Chen G, Futaba D N, Sakurai S, et al.. Interplay of wall number and diameter on the electrical conductivity of carbon nanotube thin films. Carbon, 2014, 67: 318–325 https://doi.org/10.1016/j.carbon.2013.10.001
41	Futaba D N, Yamada T, Kobashi K, et al.. Macroscopic wall number analysis of single-walled, double-walled, and few-walled carbon nanotubes by X-ray diffraction. Journal of the American Chemical Society, 2011, 133(15): 5716–5719 https://doi.org/10.1021/ja2005994
42	Kim B, Sigmund W M. Functionalized multiwall carbon nanotube/gold nanoparticle composites. Langmuir, 2004, 20(19): 8239–8242 https://doi.org/10.1021/la049424n
43	Li D, Müller M B, Gilje S, et al.. Processable aqueous dispersions of graphene nanosheets. Nature Nanotechnology, 2008, 3(2): 101–105 https://doi.org/10.1038/nnano.2007.451
44	Iida H, Takayanagi K, Nakanishi T, et al.. Synthesis of Fe3O4 nanoparticles with various sizes and magnetic properties by controlled hydrolysis. Journal of Colloid and Interface Science, 2007, 314(1): 274–280 https://doi.org/10.1016/j.jcis.2007.05.047
45	Cheng Z P, Chu X Z, Yin J Z, et al.. Surfactantless synthesis of Fe3O4 magnetic nanobelts by a simple hydrothermal process. Materials Letters, 2012, 75: 172–174 https://doi.org/10.1016/j.matlet.2012.02.029
46	Zhang J, Liu G D, Wang P H, et al.. Facile synthesis of FeOCl/iron hydroxide hybrid nanosheets: enhanced catalytic activity as a Fenton-like catalyst. New Journal of Chemistry, 2017, 41(18): 10339–10346 https://doi.org/10.1039/C7NJ01993A
47	Hassan H, Hameed B H. Fe-clay as effective heterogeneous Fenton catalyst for the decolorization of Reactive Blue 4. Chemical Engineering Journal, 2011, 171(3): 912–918 https://doi.org/10.1016/j.cej.2011.04.040
48	Xu H Y, Prasad M, Liu Y. Schorl: a novel catalyst in mineral-catalyzed Fenton-like system for dyeing wastewater discoloration. Journal of Hazardous Materials, 2009, 165(1‒3): 1186–1192 https://doi.org/10.1016/j.jhazmat.2008.10.108
49	Kwan W P, Voelker B M. Rates of hydroxyl radical generation and organic compound oxidation in mineral-catalyzed Fenton-like systems. Environmental Science & Technology, 2003, 37(6): 1150–1158 https://doi.org/10.1021/es020874g
50	Feng J, Hu X, Yue P L. Novel bentonite clay-based Fe-nanocomposite as a heterogeneous catalyst for photo-Fenton discoloration and mineralization of Orange II. Environmental Science & Technology, 2004, 38(1): 269–275 https://doi.org/10.1021/es034515c

[1]	Huan-Yan XU, Yuan WANG, Tian-Nuo SHI, Hang ZHAO, Qu TAN, Bo-Chao ZHAO, Xiu-Lan HE, Shu-Yan QI. 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.
[2]	Hang ZHAO,Ling WENG,Wei-Wei CUI,Xiao-Rui ZHANG,Huan-Yan XU,Li-Zhu LIU. In situ anchor of magnetic Fe₃O₄ nanoparticles onto natural maifanite as efficient heterogeneous Fenton-like catalyst[J]. Front. Mater. Sci., 2016, 10(3): 300-309.
[3]	Huan-Yan XU,Tian-Nuo SHI,Hang ZHAO,Li-Guo JIN,Feng-Chun WANG,Chun-Yan WANG,Shu-Yan QI. Heterogeneous Fenton-like discoloration of methyl orange using Fe₃O₄/MWCNTs as catalyst: process optimization by response surface methodology[J]. Front. Mater. Sci., 2016, 10(1): 45-55.

Viewed

Full text

Abstract

Cited

Shared

Discussed