Synthesis of Graphene Oxide/Silica/Carbon Nanotubes Composite for Removal of Dyes from Wastewater

  • Noha Almoisheer
  • Fathia A. Alseroury
  • Rajeev Kumar
  • Talal Almeelbi
  • M. A. BarakatEmail author
Original Article


The recent interest in adsorption of pollutants on nanomaterials has been gaining widespread attention especially in the utilization of nanocarbon based composite materials. Herein, graphene oxide/silica/single-wall carbon nanotubes (GO/SiO2/SWCNTs) composite was successfully prepared by a hydrothermal method for the adsorption of Congo red (CR) dye from synthetic wastewater. The nanocomposite morphology was characterized by X-ray diffraction (XRD), Field emission scanning electron microscope (FESEM), and Energy-dispersive X-ray spectroscopy (EDX). The present study focuses on the adsorption performance of CR dye from aqueous solution on GO/SiO2/SWCNTs composite in terms of kinetics, isotherm, thermodynamics studies and optimization of factors such as pH, temperature, concentration and adsorption time. The results showed that a higher adsorption of CR was observed onto GO/SiO2/SWCNT composite at pH 3.0 as compared to that with SiO2 and SWCNT. Similarly, the maximum adsorption capacity of 456.15 mg g−1 was achieved at optimum temperature 20 °C, time (330 min) and 300 mg L−1 CR solution concentration. The dye adsorption on the nanocomposite was found to be obeying pseudo-second-order rate equation. Thermodynamic parameters showed that the adsorption of CR dye was spontaneous in nature.


GO/SiO2/SWCNTs Nanocomposite Adsorption Congo red dye Kinetics Isotherms Wastewater 


  1. Afkhami A, Moosavi R (2010) Adsorptive removal of Congo red, a carcinogenic textile dye, from aqueous solutions by maghemite nanoparticles. J Hazard Mater 174(1–3):398–403CrossRefGoogle Scholar
  2. Ahmad A, Mohd-Setapar S, Chuong C, Khatoon A, Wani W, Kumar R, Rafatullah M (2015) Recent advances in new generation dye removal technologies: novel search for approaches to reprocess wastewater. RSC Adv 5(39):30801–30818CrossRefGoogle Scholar
  3. Barakat MA, Al-Ansari AM, Kumar R (2016) Synthesis and characterization of Fe–Al binary oxyhydroxides/MWCNTs nanocomposite for the removal of Cr(VI) from aqueous solution. J Taiwan Inst Chem Eng 63:303–311. CrossRefGoogle Scholar
  4. Chatterjee S, Lee MW, Woo SH (2010) Adsorption of congo red by chitosan hydrogel beads impregnated with carbon nanotubes. Biores Technol 101(6):1800–1806CrossRefGoogle Scholar
  5. Chen L, Chai S, Liu K, Ning N, Gao J, Liu Q, Fu Q (2012) Enhanced epoxy/silica composites mechanical properties by introducing graphene oxide to the interface. ACS Appl Mater Interfaces 4(8):4398–4404CrossRefGoogle Scholar
  6. Cheng Z, Liao J, He B, Zhang F, Zhang F, Huang X, Zhou L (2015) One-step fabrication of graphene oxide enhanced magnetic composite gel for highly efficient dye adsorption and catalysis. ACS Sustain Chem Eng 3(7):1677–1685CrossRefGoogle Scholar
  7. de Carvalho T, Fungaro D, Magdalena C, Cunico P (2011) Adsorption of indigo carmine from aqueous solution using coal fly ash and zeolite from fly ash. J Radioanal Nucl Chem 289(2):617–626CrossRefGoogle Scholar
  8. Dehghani MH, Naghizadeh A, Rashidi A, Derakhshani E (2013) Adsorption of reactive blue 29 dye from aqueous solution by multiwall carbon nanotubes. Desalin Water Treat 51(40–42):7655–7662CrossRefGoogle Scholar
  9. Deng C, Fu H, Teng L, Hu Z, Xu X, Chen J, Ren T (2013a) Anti-tumor activity of the regenerated triple-helical polysaccharide from Dictyophora indusiata. Int J Biol Macromol 61:453–458. CrossRefGoogle Scholar
  10. Deng JH, Zhang XR, Zeng GM, Gong JL, Niu QY, Liang J (2013b) Simultaneous removal of Cd (II) and ionic dyes from aqueous solution using magnetic graphene oxide nanocomposite as an adsorbent. Chem Eng J 226:189–200. CrossRefGoogle Scholar
  11. Enaime G, Ennaciri K, Ounas A, Baçaoui A, Seffen M, Selmi T, Yaacoubi A (2017) Preparation and characterization of activated carbons from olive wastes by physical and chemical activation: application to Indigo carmine adsorption. J Mater Environ Sci 8(11):4125–4137Google Scholar
  12. Fan L, Luo C, Li X, Lu F, Qiu H, Sun M (2012) Fabrication of novel magnetic chitosan grafted with graphene oxide to enhance adsorption properties for methyl blue. J Hazard Mater 215:272–279CrossRefGoogle Scholar
  13. Gao H, Zhao S, Cheng X, Wang X, Zheng L (2013) Removal of anionic azo dyes from aqueous solution using magnetic polymer multi-wall carbon nanotube nanocomposite as adsorbent. Chem Eng J 223:84–90. CrossRefGoogle Scholar
  14. Gharbani P, Tabatabaii SM, Mehrizad A (2008) Removal of Congo red from textile wastewater by ozonation. Int J Environ Sci Technol 5(4):495–500CrossRefGoogle Scholar
  15. Gupta VK, Kumar R, Nayak A, Saleh TA, Barakat MA (2013) Review article; adsorptive removal of dyes from aqueous solution onto carbon nanotubes: a review. Adv Coll Interface Sci 193:24–34. CrossRefGoogle Scholar
  16. Hamidi Malayeri F, Sohrabi MR, Ghourchian H (2012) Magnetic multi-walled carbon nanotube as an adsorbent for toluidine blue o removal from aqueous solution. Int J Nanosci Nanotechnol 8(2):79–86Google Scholar
  17. Han R, Ding D, Xu Y, Zou W, Wang Y, Li Y, Zou L (2008) Use of rice husk for the adsorption of congo red from aqueous solution in column mode. Bioresour Technol 99(8):2938–2946CrossRefGoogle Scholar
  18. Hao T, Yang C, Rao X, Wang J, Niu C, Su X (2014) Facile additive-free synthesis of iron oxide nanoparticles for efficient adsorptive removal of Congo red and Cr(VI). Appl Surf Sci 292:174–180. CrossRefGoogle Scholar
  19. Ho YS, Ofomaja AE (2006) Biosorption thermodynamics of cadmium on coconut copra meal as biosorbent. Biochem Eng J 30(2):117–123CrossRefGoogle Scholar
  20. Hu M, Yan X, Hu X, Zhang J, Feng R, Zhou M (2018) Ultra-high adsorption capacity of MgO/SiO2 composites with rough surfaces for Congo red removal from water. J Colloid Interface Sci 510:111–117. CrossRefGoogle Scholar
  21. Jain R, Sikarwar S (2006) Photocatalytic and adsorption studies on the removal of dye Congo red from wastewater. Int J Environ Pollut 27(1–3):158–178CrossRefGoogle Scholar
  22. Jawaid M, Khan MM (2018) Polymer-based nanocomposites for energy and environmental applications. Woodhead Publishing, CambridgeGoogle Scholar
  23. Jin LN, Qian XY, Wang JG, Aslan H, Dong M (2015) MIL-68 (In) nano-rods for the removal of Congo red dye from aqueous solution. J Colloid Interface Sci 453:270–275. CrossRefGoogle Scholar
  24. Kuhn JN, Muralidharan R, Li X, Goswami DY, Stefanakos EK (2013) Reversible hydrogen storage in the LieMgeNeH system e The effects of Ru doped single walled carbon nanotubes on NH3 emission and kinetics. Int J Hydrogen Energy 38(10039):e10049Google Scholar
  25. Kumar R, Ansari MO, Parveen N, Barakat MA, Cho MH (2015) Simple route for the generation of differently functionalized PVC@ graphene–polyaniline fiber bundles for the removal of Congo red from wastewater. RSC Adv 5(76):61486–61494CrossRefGoogle Scholar
  26. Kumar R, Laskar MA, Hewaidy IF, Barakat MA (2019) Modified adsorbents for removal of heavy metals from aqueous environment: a review. Earth Syst Environ 3:83–93CrossRefGoogle Scholar
  27. Lachheb H, Puzenat E, Houas A, Ksibi M, Elaloui E, Guillard C, Herrmann JM (2002) Photocatalytic degradation of various types of dyes (Alizarin S, Crocein Orange G, Methyl Red, Congo Red, Methylene Blue) in water by UV-irradiated titania. Appl Catal B 39(1):75–90CrossRefGoogle Scholar
  28. Liu S, Ding Y, Li P, Diao K, Tan X, Lei F, Huang Z (2014) Adsorption of the anionic dye Congo red from aqueous solution onto natural zeolites modified with N,N-dimethyl dehydroabietylamine oxide. Chem Eng J 248:135–144. CrossRefGoogle Scholar
  29. Lu H, Wang J, Stoller M, Wang T, Bao Y, Hao H (2016) Review article; An overview of nanomaterials for water and wastewater treatment. Adv Mater Sci Eng 2016:1–10. Google Scholar
  30. Miandad R, Kumar R, Barakat MA, Basheer C, Aburiazaiza AS, Nizami AS, Rehan M (2018) Untapped conversion of plastic waste char into carbon-metal LDOs for the adsorption of Congo red. J Colloid Interface Sci 511:402–410. CrossRefGoogle Scholar
  31. Mittal A, Mittal J, Malviya A, Gupta VK (2009) Adsorptive removal of hazardous anionic dye “Congo red” from wastewater using waste materials and recovery by desorption. J Colloid Interface Sci 340(1):16–26CrossRefGoogle Scholar
  32. Molinari R, Pirillo F, Falco M, Loddo V, Palmisano L (2004) Photocatalytic degradation of dyes by using a membrane reactor. Chem Eng Process 43(9):1103–1114CrossRefGoogle Scholar
  33. Namasivayam C, Kavitha D (2002) Removal of Congo Red from water by adsorption onto activated carbon prepared from coir pith, an agricultural solid waste. Dyes Pigm 54(1):47–58CrossRefGoogle Scholar
  34. Ngah WW, Teong LC, Hanafiah MAKM (2011) Review article; Adsorption of dyes and heavy metal ions by chitosan composites: a review. Carbohyd Polym 83(4):1446–1456CrossRefGoogle Scholar
  35. Ojedokun AT, Bello OS (2017) Kinetic modeling of liquid-phase adsorption of Congo red dye using guava leaf-based activated carbon. Appl Water Sci 7(4):1965–1977CrossRefGoogle Scholar
  36. Ong YT, Ahmad AL, Zein SHS, Tan SH (2010) Review Article; A review on carbon nanotubes in an environmental protection and green engineering perspective. Braz J Chem Eng 27(2):227–242CrossRefGoogle Scholar
  37. Ouyang X, Li W, Xie S, Zhai T, Yu M, Gan J, Lu X (2013) Hierarchical CeO2 nanospheres as highly-efficient adsorbents for dye removal. New J Chem 37(3):585–588CrossRefGoogle Scholar
  38. Ozmen EY, Yilmaz M (2007) Use of β-cyclodextrin and starch based polymers for sorption of Congo red from aqueous solutions. J Hazard Mater 148(1–2):303–310CrossRefGoogle Scholar
  39. Panda GC, Das SK, Guha AK (2009) Jute stick powder as a potential biomass for the removal of congo red and rhodamine B from their aqueous solution. J Hazard Mater 164(1):374–379CrossRefGoogle Scholar
  40. Pandey G, Singh S, Hitkari G (2018) Synthesis and characterization of polyvinyl pyrrolidone (PVP)-coated Fe3 O4 nanoparticles by chemical co-precipitation method and removal of Congo red dye by adsorption process. Int Nano Lett 8:111–121. CrossRefGoogle Scholar
  41. Pavan FA, Dias SL, Lima EC, Benvenutti EV (2008) Removal of Congo red from aqueous solution by anilinepropylsilica xerogel. Dyes Pigments 76(1):64–69.Google Scholar
  42. Purkait MK, Maiti A, Dasgupta S, De S (2007) Removal of congo red using activated carbon and its regeneration. J Hazard Mater 145(1–2):287–295CrossRefGoogle Scholar
  43. Rohaeti E (2015) Reduction of high purity silicon from bamboo leaf as basic material in development of sensors manufacture in satellite technology. Proc Environ Sci 24:308–316. CrossRefGoogle Scholar
  44. Sadegh H, Shahryari-ghoshekandi R, Kazemi M (2014) Study in synthesis and characterization of carbon nanotubes decorated by magnetic iron oxide nanoparticles. Int Nano Lett 4(4):129–135CrossRefGoogle Scholar
  45. Saleh TA (2015) Mercury sorption by silica/carbon nanotubes and silica/activated carbon: a comparison study. J Water Supply Res Technol Aqua 64(8):892–903CrossRefGoogle Scholar
  46. Saleh TA (2016) Nanocomposite of carbon nanotubes/silica nanoparticles and their use for adsorption of Pb(II): from surface properties to sorption mechanism. Desalin Water Treat 57(23):10730–10744CrossRefGoogle Scholar
  47. Shaban M, Sayed MI, Shahien MG, Abukhadra MR, Ahmed ZM (2018) Adsorption behavior of inorganic-and organic-modified kaolinite for Congo red dye from water, kinetic modeling, and equilibrium studies. J Sol-Gel Sci Technol 87:427–441. CrossRefGoogle Scholar
  48. Tan IAW, Ahmad AL, Hameed BH (2009) Adsorption isotherms, kinetics, thermodynamics and desorption studies of 2,4,6-trichlorophenol on oil palm empty fruit bunch-based activated carbon. J Hazard Mater 164(2–3):473–482CrossRefGoogle Scholar
  49. Tan KB, Vakili M, Horri BA, Poh PE, Abdullah AZ, Salamatinia B (2015) Adsorption of dyes by nanomaterials: recent developments and adsorption mechanisms. Sep Purif Technol 150:229–242. CrossRefGoogle Scholar
  50. Vimonses V, Lei S, Jin B, Chow CW, Saint C (2009) Kinetic study and equilibrium isotherm analysis of Congo Red adsorption by clay materials. Chem Eng J 148(2–3):354–364CrossRefGoogle Scholar
  51. Wang L, Li J, Wang Y, Zhao L, Jiang Q (2012) Adsorption capability for Congo red on nanocrystalline MFe2O4 (M = Mn, Fe Co, Ni) spinel ferrites. Chem Eng J 181:72–79. CrossRefGoogle Scholar
  52. Wang J, Liu M, Chen T, Chen J, Ge W, Fu Z, Lu Y (2018) Core-shelled mesoporous CoFe2O4–SiO2 material with good adsorption and high-temperature magnetic recycling capabilities. J Phys Chem Solids 115:300–306. CrossRefGoogle Scholar
  53. Wanyonyi WC, Onyari JM, Shiundu PM (2014) Adsorption of Congo Red Dye from aqueous solutions using roots of Eichhornia crassipes: kinetic and equilibrium studies. Energy Proc 50:862–869.
  54. Yao Y, Xu F, Chen M, Xu Z, Zhu Z (2010) Adsorption behavior of methylene blue on carbon nanotubes. Bioresour Technol 101(9):3040–3046CrossRefGoogle Scholar
  55. Yu JG, Zhao XH, Yang H, Chen XH, Yang Q, Yu LY, Chen XQ (2014) Review Article; Aqueous adsorption and removal of organic contaminants by carbon nanotubes. Sci Total Environ 482:241–251. CrossRefGoogle Scholar
  56. Zare K, Sadegh H, Shahryari-Ghoshekandi R, Maazinejad B, Ali V, Tyagi I, Gupta VK (2015) Enhanced removal of toxic Congo red dye using multi walled carbon nanotubes: kinetic, equilibrium studies and its comparison with other adsorbents. J Mol Liq 212:266–271. CrossRefGoogle Scholar
  57. Zazouli MA, Balarak D, Mahdavi Y, Ebrahimi M (2013) Adsorption rate of 198 reactive red dye from aqueous solutions by using activated red mud. Iran J Health Sci 1(1):36–43CrossRefGoogle Scholar
  58. Zulfikar MA, Setiyanto H (2013) Adsorption of congo red from aqueous solution using powdered eggshell. Int J Chem Tech Res 5(4):1532–1540Google Scholar

Copyright information

© King Abdulaziz University and Springer Nature Switzerland AG 2019

Authors and Affiliations

  1. 1.Department of Physics, Faculty of ScienceKing Abdulaziz UniversityJeddahKingdom of Saudi Arabia
  2. 2.Department of Physics, Faculty of ScienceUniversity of JeddahJeddahKingdom of Saudi Arabia
  3. 3.Department of Environmental Sciences, Faculty of Meteorology, Environment and Arid Land AgricultureKing Abdulaziz UniversityJeddahKingdom of Saudi Arabia
  4. 4.Central Metallurgical R&D InstituteHelwanEgypt

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