Environmental Science and Pollution Research

, Volume 24, Issue 12, pp 11764–11778 | Cite as

Application of a novel magnetic carbon nanotube adsorbent for removal of mercury from aqueous solutions

  • Farshid Homayoon
  • Hossein FaghihianEmail author
  • Firoozeh Torki
Research Article


In this research, multiwall carbon nanotube was magnetized and subsequently functionalized by thiosemicarbazide. After characterization by FTIR, BET, SEM, EDAX, and VSM techniques, the magnetized adsorbent (multi-walled carbon nanotubes (MWCNTs)/Fe3O4) was used for removal of Hg2+ from aqueous solutions and the experimental conditions were optimized. The adsorption capacity of 172.83 mg g−1 was obtained at 25 °C and pH = 3 which was superior to the value obtained for initial multiwall carbon nanotube, magnetized sample, and many previously reported values. In the presence of Pb+2 and Cd+2, the adsorbent was selective towards mercury when their concentration was respectively below 50 and 100 mg L−1. The adsorption process was kinetically fast and the equilibration was attained within 60 min with 69.5% of the capacity obtained within 10 min. The used adsorbent was regenerated by HNO3 solution, and the regenerated adsorbent retained 92% of its initial capacity. The magnetic sensitivity of the adsorbent allowed the simple separation of the used adsorbent from the solution by implying an appropriate external magnetic field. The adsorption data was well fitted to the Langmuir isotherm model, indicating homogeneous and monolayer adsorption of mercury by the adsorbent.


Mercury Magnetized carbon nanotubes Functionalization Thiosemicarbazide Adsorption 


  1. Abraham TN, Kumar R, Misra RK, Jain SK (2012) Poly (vinyl alcohol)-based MWCNT hydrogel for lead ion removal from contaminated water. J Appl Polym Sci 125(S1):E670–E674CrossRefGoogle Scholar
  2. Afkhami A, Bagheri H, Khoshsafar H, Saber-Tehrani MS, Tabatabaee M, Shirzadmehr A (2012) Simultaneous trace-levels determination of Hg(II) and Pb(II) ions in various samples using a modified carbon paste electrode based on multi-walled carbon nano tubes and a new synthesized Schiff base. Anal Chim Acta 746:98–106CrossRefGoogle Scholar
  3. Ai L, Zhang C, Liao F, Wang Y, Li M, Meng L, Jiang J (2011) Removal of methylene blue from aqueous solution with magnetite loaded multi-wall carbon nano tube: kinetic, isotherm and mechanism analysis. J Hazard Mater 198:282–290CrossRefGoogle Scholar
  4. Allen SJ, Mckay G, Porter JF (2004) Adsorption isotherm models for basic dye adsorption by peat in single and binary component systems. J Colloid Interface Sci 280(2):322–333CrossRefGoogle Scholar
  5. Bandaru NM, Reta N, Dalal H, Ellis AV, Shapter J, Voelcker NH (2013) Enhanced adsorption of mercury ions on thiol derivatized single wall carbon nano tubes. J Hazard Mater 261:534–541CrossRefGoogle Scholar
  6. Bandegharaei AH, Hosseini MS, Jalalabadi Y, Sarwghadi M, Nedaie M, Taherian A, Ghaznavi A, Eftekhari A (2011) Removal of Hg(II) from aqueous solutions using a novel impregnated resin containing 1-(2-thiazolylazo)-2-naphthol (TAN). Chem Eng J 168(3):1163–1173CrossRefGoogle Scholar
  7. Cui H, Qian Y, Li Q, Wei Z, Zhai J (2013) Fast removal of Hg(II) ions from aqueous solution by amine-modified attapulgite. Appl Clay Sci 72:84–90CrossRefGoogle Scholar
  8. Cui L, Guo X, Wei Q, Wang Y, Gao L, Yan L, Yan T, Du B (2015) Removal of mercury and methylene blue from aqueous solution by xanthate functionalized magnetic graphene oxide: sorption kinetic and uptake mechanism. J Colloid Interface Sci 439:112–120CrossRefGoogle Scholar
  9. De M, Azargohar R, Dalai AK, Shewchuk SR (2013) Mercury removal by bio-char based modified activated carbons. Fuel 103:570–578CrossRefGoogle Scholar
  10. Freundlich HMF (1906) Over the adsorption in solution. Z Phys Chem 57A(5):385–470Google Scholar
  11. Gao R, Hu Z, Chang X, He Q, Zhang L, Tu Z, Shi J (2009) Chemically modified activated carbon with 1-acylthiosemicarbazide for selective solid-phase extraction and pre-concentration of trace Cu(II), Hg(II) and Pb (II) from water samples. J Hazard Mater 172(1):324–329CrossRefGoogle Scholar
  12. Ge F, Li MM, Ye H, Zhao BX (2012) Effective removal of heavy metal ions Cd2+, Zn2+, Pb2+, Cu2+ from aqueous solution by polymer-modified magnetic nanoparticles. J Hazard Mater 211-212:366–372CrossRefGoogle Scholar
  13. Gupta A, Vidyarthi SR, Sankararamakrishnan N (2014) Enhanced sorption of mercury from compact fluorescent bulbs and contaminated water streams using functionalized multiwalled carbon nano tubes. J Hazard Mater 274C:132–144CrossRefGoogle Scholar
  14. Hadavifar M, Bahramifar N, Younesi H, Li Q (2014) Adsorption of mercury ions from synthetic and real wastewater aqueous solution by functionalized multi-walled carbon nano tube with both amino and thiolated groups. Chem Eng J 237:217–228CrossRefGoogle Scholar
  15. Hakami O, Zhang Y, Banks CJ (2012) Thiol-functionalized mesoporous silica-coated magnetite nanoparticles for high efficiency removal and recovery of Hg from water. Water Res 46(12):3913–3922CrossRefGoogle Scholar
  16. Herrera AVH, Curbelo MAG, Borges JH, Delgado MAR (2012) Carbon nano tubes applications in separation science: a review. Anal Chim Acta 734:1–30CrossRefGoogle Scholar
  17. Juang RS, Wu FC, Tseng RL (1996) Adsorption isotherms of phenolic compounds from aqueous solutions onto activated carbon fibers. J Chem Eng Data 41(3):487–492CrossRefGoogle Scholar
  18. Kabay N, Baygu Y, Alpoguz HK, Kaya A, Gok Y (2013) Synthesis and characterization of porphyrazines as novel extractants for the removal of Ag(I) and Hg(II) from aqueous solution. Dyes Pigments 96(2):372–376CrossRefGoogle Scholar
  19. Langmuir I (1916) The constitution and fundamental properties of solids and liquids. J Am Chem Soc 38(5):2221–2295CrossRefGoogle Scholar
  20. Latorre CH, Mendez JA, Garcia JB, Martin SG, Crecente RMP (2012) Carbon nano tubes as solid-phase extraction sorbents prior to atomic spectrometric determination of metal species: a review. Anal Chim Acta 749:16–35CrossRefGoogle Scholar
  21. Li Q, Sun L, Zhang Y, Qian Y, Zhai J (2011a) Characteristics of equilibrium, kinetics studies for adsorption of Hg(II) and Cr(VI) by polyaniline/humic acid composite. Desalination 266(1–3):188–194CrossRefGoogle Scholar
  22. Li SX, Zheng FY, Yang H, Ni JC (2011b) Thorough removal of inorganic and organic mercury from aqueous solutions by adsorption on Lemna minor powder. J Hazard Mater 186(1):423–429CrossRefGoogle Scholar
  23. Li Z, Wu L, Liu H, Lan H, Qu J (2013) Improvement of aqueous mercury adsorption on activated coke by thiol-functionalization. Chem Eng J 228:925–934CrossRefGoogle Scholar
  24. Lopez-Marzo AM, Pons J, Merkoci A (2014) Extremely fast and high Pb2+ removal capacity using a nanostructured hybrid material. J Mater Chem A 2(23):8766–8772CrossRefGoogle Scholar
  25. Luo C, Tian Z, Yang B, Zhang L, Yan S (2013) Manganese dioxide/iron oxide/acid oxidized multi-walled carbon nano tube magnetic nanocomposite for enhanced hexavalent chromium removal. Chem Eng J 234:256–265CrossRefGoogle Scholar
  26. Moghaddam HK, Pakizeh M (2014) Experimental study on mercury ions removal from aqueous solution by MnO2/CNTs nanocomposite adsorbent. J Ind Eng Chem 21:221–229CrossRefGoogle Scholar
  27. Mondal DK, Nandi BK, Purkait MK (2013) Removal of mercury (II) from aqueous solution using bamboo leaf powder: equilibrium, thermodynamic and kinetic studies. J Environ Chem Eng 1(4):891–898CrossRefGoogle Scholar
  28. Monier M, Abdel-Latif DA (2013) Modification and characterization of PET fibers for fast removal of Hg(II), Cu(II) and Co(II) metal ions from aqueous solutions. J Hazard Mater 250-251:122–130CrossRefGoogle Scholar
  29. Monier M, Kenawy IM, Hashem MA (2014) Synthesis and characterization of selective thiourea modified Hg(II) ion-imprinted cellulosic cotton fibers. Carbohydr Polym 106:49–59CrossRefGoogle Scholar
  30. Murthy BN, Zeile S, Nambiar M, Nussio MR, Gibson CT, Shapter JG, Jayaraman N, Voelcker NH (2012) Self-assembly of bivalent glycolipids on single walled carbon nano tubes and their specific molecular recognition properties. RSC Adv 1(4):1329–1333CrossRefGoogle Scholar
  31. Natale, F.D., Erto, A., Musmarra, D., (2011) Mercury adsorption on granular activated carbon in aqueous solutions containing nitrates and chlorides. 192 (3), 1842–1850.Google Scholar
  32. Pan S, Zhang Y, Shen H, Hu M (2012a) An intensive study on the magnetic effect of mercapto-functionalized nano-magnetic Fe3O4 polymers and their adsorption mechanism for the removal of Hg(II) from aqueous solution. Chem Eng J 210:564–574CrossRefGoogle Scholar
  33. Pan S, Shen H, Xu Q, Luo J, Hu M (2012b) Surface mercapto engineered magnetic Fe3O4 nanoadsorbent for the removal of mercury from aqueous solutions. J Colloid Interface Sci 365(1):204–212CrossRefGoogle Scholar
  34. Parham H, Zargar B, Shiralipour R (2012) Fast and efficient removal of mercury from water samples using magnetic iron oxide nanoparticles modified with 2-mercaptobenzothiazole. J Hazard Mater 205-206:94–100CrossRefGoogle Scholar
  35. Pillay K, Cukrowska EM, Coville NJ (2013) Improved uptake of mercury by sulphur-containing carbon nano tubes. Microchem J 108:124–130CrossRefGoogle Scholar
  36. Pu Y, Yang X, Zheng H, Wang D, Su Y, He J (2013) Adsorption and desorption of thallium(I) on multiwalled carbon nano tubes. Chem Eng J 219:403–410CrossRefGoogle Scholar
  37. Rao GP, Lu C, Su F (2007) Sorption of divalent metal ions from aqueous solution by carbon nano tubes: a review. Sep Purif Technol 58(1):224–231CrossRefGoogle Scholar
  38. Redlich O, Peterson DL (1959) A useful adsorption isotherm. J Phys Chem 63(5):1024–1024CrossRefGoogle Scholar
  39. Ren X, Chen C, Nagatsu M, Wang X (2011) Carbon nano tubes as adsorbents in environmental pollution management: a review. Chem Eng J 170(2–3):395–410CrossRefGoogle Scholar
  40. Rooney JPK (2007) The role of thiols, dithiols, nutritional factors and interacting ligands in the toxicology of mercury. Toxicology 234(3):145–156CrossRefGoogle Scholar
  41. Shadbad MJ, Mohebbi A, Soltani A (2011) Mercury(II) removal from aqueous solutions by adsorption on multi-walled carbon nano tubes. Korean J Chem Eng 28(4):1029–1034CrossRefGoogle Scholar
  42. Sharififard H, Ashtiani FZ, Soleimani M (2013) Adsorption of palladium and platinum from aqueous solutions by chitosan and activated carbon coated with chitosan. Asia Pac J Chem Eng 8(3):384–395CrossRefGoogle Scholar
  43. Shawky HA, Aassar AHME, Zeid DEA (2012) Chitosan/carbon nano tube composite beads: preparation, characterization, and cost evaluation for mercury removal from wastewater of some industrial cities in Egypt. J Appl Polym Sci 125(S1):93–101CrossRefGoogle Scholar
  44. Song ST, Saman N, Johari K, Mat H (2013) Removal of Hg(II) from aqueous solution by adsorption using raw and chemically modified rice straw as novel adsorbents. Ind Eng Chem Res 52(36):13092–13101CrossRefGoogle Scholar
  45. Tavallali H, Abdardideh D, Aalaei M, Zahmatkesh S (2012) New application of chemically modified multiwalled carbon nano tubes with thiosemicarbazide as a sorbent for separation and preconcentration of trace amounts of Co(II), Cd(II), Cu(II), and Zn(II) in environmental and biological samples prior to determination by flame atomic absorption spectrometry. J Chin Chem Soc 59(1):114–121CrossRefGoogle Scholar
  46. Tawabini B, Khaldi SA, Atieh M, Khaled M (2010) Removal of mercury from water by multi-walled carbon nano tubes. Water Sci Technol 61(3):591–598CrossRefGoogle Scholar
  47. Tofighy MA, Mohammadi T (2010) Salty water desalination using carbon nano tube sheets. Desalination 258(1–3):182–186CrossRefGoogle Scholar
  48. Tofighy MA, Mohammadi T (2011) Adsorption of divalent heavy metal ions from water using carbon nano tube sheets. J Hazard Mater 185(1):140–147CrossRefGoogle Scholar
  49. Wang Y, Iqbal Z, Mitra S (2006) Rapidly functionalized, water-dispersed carbon nano tubes at high concentration. J Am Chem Soc 128(1):95–99CrossRefGoogle Scholar
  50. Xiong C, Li Y, Wang G, Fang L, Zhou S, Yao C, Chen Q, Zheng X, Qi D, Fu Y, Zhu Y (2015) Selective removal of Hg(II) with polyacrylonitrile-2-amino-1,3,4-thiadiazole chelating resin: batch and column study. Chem Eng J 259:257–265CrossRefGoogle Scholar
  51. Xu Y-J, Rosa A, Liu X, Su D (2011) Characterization and use of functionalized carbon nano tubes for the adsorption of heavy metal anions. New Carbon Mater 26(1):57–62CrossRefGoogle Scholar
  52. Yang RT (2003) Adsorbents: fundamentals and applications. Wiley, New JerseyCrossRefGoogle Scholar
  53. Zabihi M, Ahmadpour A, Asl AH (2009) Removal of mercury from water by carbonaceous sorbents derived from walnut shell. J Hazard Mater 167(1–3):230–236CrossRefGoogle Scholar
  54. Zhang FS, Nriagu JO, Itoh H (2009) Mercury removal from water using activated carbons derived from organic sewage sludge. Water Res 39(2–3):389–395Google Scholar
  55. Zhang C, Sui J, Li J, Tang Y, Cai W (2012) Efficient removal of heavy metal ions by thiol-functionalized superparamagnetic carbon nano tubes. Chem Eng J 210:45–52CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2017

Authors and Affiliations

  • Farshid Homayoon
    • 1
  • Hossein Faghihian
    • 1
    Email author
  • Firoozeh Torki
    • 1
  1. 1.Department of ChemistryIslamic Azad UniversityShahrezaIran

Personalised recommendations