Skip to main content
SpringerLink
Log in

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

  • Research Article
  • Published:
Frontiers of Materials Science Aims and scope Submit manuscript

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.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Similar content being viewed by others

References

  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

    Article  Google Scholar 

  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

    Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  12. Liu Y Y, Jin W, Zhao Y P, et al. Enhanced catalytic degradation of methylene blue by a-Fe2O3/graphene oxide via heterogeneous photo-Fenton reactions. Applied Catalysis B: Environmental, 2017, 206: 642–652

    Article  Google Scholar 

  13. Wang Y, Fang J S, Crittenden J C, et al. Novel RGO/a-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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  18. Haber F, Weiss J. The catalytic decomposition of hydrogen peroxide by iron salts. Proceedings of the Royal Society, 1934, 147(861): 332–351

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  29. Tian X, Liu Y, Chi W, et al. Catalytic degradation of phenol and pnitrophenol using Fe3O4/MWCNT nanocomposites as heterogeneous Fenton-like catalyst. Water, Air, and Soil Pollution, 2017, 228(8): 297

    Article  Google Scholar 

  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

    Article  Google Scholar 

  31. 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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  33. Zubir N A, Motuzas J, Yacou C, et al. Graphene oxide with zinc partially substituted magnetite (GO-Fe1–xZnxOy) for the UVassisted heterogeneous Fenton-like reaction. RSC Advances, 2016, 6(50): 44749–44757

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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)

    Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  42. Kim B, Sigmund W M. Functionalized multiwall carbon nanotube/gold nanoparticle composites. Langmuir, 2004, 20 (19): 8239–8242

    Article  Google Scholar 

  43. Li D, Müller M B, Gilje S, et al. Processable aqueous dispersions of graphene nanosheets. Nature Nanotechnology, 2008, 3(2): 101–105

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  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

    Article  Google Scholar 

  48. Xu H Y, Prasad M, Liu Y. Schorl: a novel catalyst in mineralcatalyzed Fenton-like system for dyeing wastewater discoloration. Journal of Hazardous Materials, 2009, 165(1–3): 1186–1192

    Article  Google Scholar 

  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

    Article  Google Scholar 

  50. Feng J, Hu X, Yue P L. Novel bentonite clay-based Fenanocomposite as a heterogeneous catalyst for photo-Fenton discoloration and mineralization of Orange II. Environmental Science & Technology, 2004, 38(1): 269–275

    Article  Google Scholar 

Download references

Acknowledgement

This work was financially supported by the Natural Science Foundation of Heilongjiang Province, China (No. E2015065).

Author information

Authors and Affiliations

  1. School of Materials Science and Engineering, Harbin University of Science and Technology, Harbin, 150040, China

    Huan-Yan Xu, Yuan Wang, Tian-Nuo Shi, Hang Zhao, Qu Tan, Bo-Chao Zhao, Xiu-Lan He & Shu-Yan Qi

Authors
  1. Huan-Yan Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yuan Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Tian-Nuo Shi
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Hang Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Qu Tan
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Bo-Chao Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Xiu-Lan He
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Shu-Yan Qi
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Huan-Yan Xu.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Xu, HY., Wang, Y., Shi, TN. et al. Heterogeneous Fenton-like discoloration of methyl orange using Fe3O4/MWCNTs as catalyst: combination mechanism and affecting parameters. Front. Mater. Sci. 12, 21–33 (2018). https://doi.org/10.1007/s11706-018-0408-1

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11706-018-0408-1

Keywords

Search

Navigation