Environmental Science and Pollution Research

, Volume 22, Issue 18, pp 14201–14208 | Cite as

Directing carbon nanotubes from aqueous phase to o/w interface for heavy metal uptaking

  • Lili Gao
  • Huayi Yin
  • Xuhui Mao
  • Hua Zhu
  • Wei Xiao
  • Dihua Wang
Research Article


Separation and reuse of dispersed nanoparticles are major obstacles to the extensive application of nano-sized absorbents in wastewater treatment. Herein, we demonstrate the capability of directing acid-oxidized carbon nanotubes (CNTs) as the transfer vehicles of heavy metal ions from simulated wastewater. The heavy metal-loaded CNTs can be readily separated from the aqueous phase via the aggregation process at an oil/water (o/w) interface. The minimum surfactant amount to achieve 99 % transfer ratio (T r) of 100 mg/L CNTs from water phase to o/w interface was ∼0.01 mM. The adsorption experiments showed that the removal efficiency of the divalent lead ions increased with an increase in CNT mass, and the subsequent addition of cetyltrimethylammonium bromide (CTAB) surfactant did not negatively impact the removal of soluble divalent lead species (Pb(II)). In a wide region of pH and ionic strength, both the decontamination of Pb(II) and the transfer of CNTs from water phase to o/w interface can be accomplished successively. The method presented in this study may be developed as a generic one for collecting or recycling the pollutant-loaded nano-sized absorbents.


Carbon nanotube Adsorption Wastewater treatment Aggregation o/w interface 



The authors are grateful to the financial support from NSFC (51278386), MOE (NCET-08-0416), Shanxi Scholarship Council of China (2013-041), and Shanxi Province Science Foundation for Youths (2013021011-3). The authors also appreciated Dr. J. F. Dong and Dr. X. F. Li for zeta potential measurements.


  1. Apostoluk W, Drzymala J (2003) An improved estimation of water-organic liquid interfacial tension based on linear solvation energy relationship approach. J Colloid Interface Sci 262:483–488CrossRefGoogle Scholar
  2. Apul OG, Karanfil T (2015) Adsorption of synthetic organic contaminants by carbon nanotubes: A critical review. Water Res 68:34–55CrossRefGoogle Scholar
  3. Bai Y, Wu F, Lin D, Xing B (2014) Aqueous stabilization of carbon nanotubes: effects of surface oxidization and solution chemistry. Environ Sci Pollut Res 21:4358–4365CrossRefGoogle Scholar
  4. Biesaga M, Pyrzynska K (2006) The evaluation of carbon nanotubes as a sorbent for dicamba herbicide. J Sep Sci 29:2241–2244CrossRefGoogle Scholar
  5. Chen CL, Li XL, Wang XK (2007a) Application of oxidized multi-wall carbon nanotubes for Th(IV) adsorption. Radiochim Acta 95:261–266CrossRefGoogle Scholar
  6. Chen W, Duan L, Zhu DQ (2007b) Adsorption of polar and nonpolar organic chemicals to carbon nanotubes. Environ Sci Technol 41:8295–8300CrossRefGoogle Scholar
  7. Das R, Hamid SBA, Ali ME, Ismail AF, Annuar MSM, Ramakrishna S (2014) Multifunctional carbon nanotubes in water treatment: the present, past and future. Desalination 354:160–179CrossRefGoogle Scholar
  8. Du J, Wang ST, You H, Zhao XS (2013) Understanding the toxicity of carbon nanotubes in the environment is crucial to the control of nanomaterials in producing and processing and the assessment of health risk for human: a review. Environ Toxicol Pharmacol 36:451–462CrossRefGoogle Scholar
  9. Elim HI, Ji W, Ma GH, Lim KY, Sow CH, Huan CHA (2004) Ultrafast absorptive and refractive nonlinearities in multiwalled carbon nanotube films. Appl Phys Lett 85:1799–1801CrossRefGoogle Scholar
  10. Fan Q, Li Z, Zhao H, Jia Z, Xu J, Wu W (2009) Adsorption of Pb(II) on palygorskite from aqueous solution: effects of pH, ionic strength and temperature. Appl Clay Sci 45:111–116CrossRefGoogle Scholar
  11. Ganesan P, Kamaraj R, Sozhan G, Vasudevan S (2013) Oxidized multiwalled carbon nanotubes as adsorbent for the removal of manganese from aqueous solution. Environ Sci Pollut Res 20:987–996CrossRefGoogle Scholar
  12. Gao L, Yin H, Wang D (2010) Ionic liquids assisted formation of an oil/water emulsion stabilised by a carbon nanotube/ionic liquid composite layer. Phys Chem Chem Phys 12:2535–2540CrossRefGoogle Scholar
  13. Gao L, Yin H, Zhu H, Mao X, Gan F, Wang D (2014) Separation of dispersed carbon nanotubes from water: effect of pH and surfactants on the aggregation at oil/water interface. Sep Purif Technol 129:113–120CrossRefGoogle Scholar
  14. Gupta VK, Saleh TA (2013) Sorption of pollutants by porous carbon, carbon nanotubes and fullerene- an overview. Environ Sci Pollut Res 20:2828–2843CrossRefGoogle Scholar
  15. Inyang M, Gao B, Zimmerman A, Zhou YM, Cao XD (2015) Sorption and cosorption of lead and sulfapyridine on carbon nanotube-modified biochars. Environ Sci Pollut Res 22:1868–1876CrossRefGoogle Scholar
  16. Kharisov BI, Dias HVR, Kharissova OV, Jimenez-Perez VM, Perez BO, Flores BM (2012) Iron-containing nanomaterials: synthesis, properties, and environmental applications. RSC Adv 2:9325–9358CrossRefGoogle Scholar
  17. Li YH, Wang SG, Wei JQ, Zhang XF, Xu CL, Luan ZK, Wu DH, Wei BQ (2002) Lead adsorption on carbon nanotubes. Chem Phys Lett 357:263–266CrossRefGoogle Scholar
  18. Li YH, Ding J, Luan ZK, Di ZC, Zhu YF, Xu CL, Wu DH, Wei BQ (2003a) Competitive adsorption of Pb2+, Cu2+ and Cd2+ ions from aqueous solutions by multiwalled carbon nanotubes. Carbon 41:2787–2792CrossRefGoogle Scholar
  19. Li YH, Luan ZK, Xiao X, Zhou XW, Xu CL, Wu DH, Wei BQ (2003b) Removal of Cu2+ ions from aqueous solutions by carbon nanotubes. Adsorpt Sci Technol 21:475–485CrossRefGoogle Scholar
  20. Li YH, Wang SG, Luan ZK, Ding J, Xu CL, Wu DH (2003c) Adsorption of cadmium(II) from aqueous solution by surface oxidized carbon nanotubes. Carbon 41:1057–1062CrossRefGoogle Scholar
  21. Li YH, Di ZC, Ding J, Wu DH, Luan ZK, Zhu YQ (2005) Adsorption thermodynamic, kinetic and desorption studies of Pb2+ on carbon nanotubes. Water Res 39:605–609CrossRefGoogle Scholar
  22. Long RQ, Yang RT (2001a) Carbon nanotubes as a superior sorbent for nitrogen oxides. Ind Eng Chem Res 40:4288–4291CrossRefGoogle Scholar
  23. Long RQ, Yang RT (2001b) Carbon nanotubes as superior sorbent for dioxin removal. J Am Chem Soc 123:2058–2059CrossRefGoogle Scholar
  24. Lu CY, Liu CT (2006) Removal of nickel(II) from aqueous solution by carbon nanotubes. J Chem Technol Biotechnol 81:1932–1940CrossRefGoogle Scholar
  25. Peng C, Jin J, Chen GZ (2007) A comparative study on electrochemical co-deposition and capacitance of composite films of conducting polymers and carbon nanotubes. Electrochim Acta 53:525CrossRefGoogle Scholar
  26. Pyrzynska K, Stafiej A, Biesaga M (2007) Sorption behavior of acidic herbicides on carbon nanotubes. Microchim Acta 159:293–298CrossRefGoogle Scholar
  27. Rao GP, Lu C, Su F (2007) Sorption of divalent metal ions from aqueous solution by carbon nanotubes: a review. Sep Purif Technol 58:224–231CrossRefGoogle Scholar
  28. Rosenzweig S, Sorial GA, Sahle-Demessie E, McAvoy DC, Hassan AA (2014) Effect of chloride ions and water chemistry on copper(II) adsorption on functionalized and pristine carbon nanotubes compared to activated carbon F-400. Water Air Soil Pollut 225:1913–1929CrossRefGoogle Scholar
  29. Sheng GD, Shao DD, Ren XM, Wang XQ, Li JX, Chen YX, Wang XK (2010) Kinetics and thermodynamics of adsorption of ionizable aromatic compounds from aqueous solutions by as-prepared and oxidized multiwalled carbon nanotubes. J Hazard Mater 178:505–516CrossRefGoogle Scholar
  30. Shvedova AA, Castranova V, Kisin ER, Schwegler-Berry D, Murray AR, Gandelsman VZ, Maynard A, Baron P (2003) Exposure to carbon nanotube material: assessment of nanotube cytotoxicity using human keratinocyte cells. J Toxicol Env Heal A 66:1909–1926CrossRefGoogle Scholar
  31. Sohrabi B, Poorgholami-Bejarpasi N, Nayeri N (2014) Dispersion of carbon nanotubes using mixed surfactants: experimental and molecular dynamics simulation studies. J Phys Chem B 118:3094–3103CrossRefGoogle Scholar
  32. Srivastava RK, Pant AB, Kashyap MP, Kumar V, Lohani M, Jonas L, Rahman Q (2011) Multi-walled carbon nanotubes induce oxidative stress and apoptosis in human lung cancer cell line-A549. Nanotoxicology 5:195–207CrossRefGoogle Scholar
  33. Stafiej A, Pyrzynska K (2007) Adsorption of heavy metal ions with carbon nanotubes. Sep Purif Technol 58:49–52CrossRefGoogle Scholar
  34. Sun W-L, Xia J, Shan Y-C (2014) Comparison kinetics studies of Cu(II) adsorption by multi-walled carbon nanotubes in homo and heterogeneous systems: effect of nano-SiO2. Chem Eng J 250:119–127CrossRefGoogle Scholar
  35. Tang DD, Wang YX, Zhao YW, Yang YJ, Zhang LY, Mao XH (2014) Effect of the composition of Ti alloy on the photocatalytic activities of Ti-based oxide nanotube arrays prepared by anodic oxidation. Appl Surf Sci 319:181–188CrossRefGoogle Scholar
  36. Theron J, Walker JA, Cloete TE (2008) Nanotechnology and water treatment: applications and emerging opportunities. Crit Rev Microbiol 34:43–69CrossRefGoogle Scholar
  37. Wang H, Zhou A, Peng F, Yu H, Yang J (2007a) Mechanism study on adsorption of acidified multiwalled carbon nanotubes to Pb(II). J Colloid Interface Sci 316:277–283CrossRefGoogle Scholar
  38. Wang SG, Gong WX, Liu XW, Yao YW, Gao BY, Yue QY (2007b) Removal of lead(II) from aqueous solution by adsorption onto manganese oxide-coated carbon nanotubes. Sep Purif Technol 58:17–23CrossRefGoogle Scholar
  39. Weng B, Liu SQ, Tang ZR, Xu YJ (2014) One-dimensional nanostructure based materials for versatile photocatalytic applications. RSC Adv 4:12685–12700CrossRefGoogle Scholar
  40. Xu WJ, Chen HZ, Shi MM, Huang YG, Wang M (2006) Poly(triphenylamine) related copolymer noncovalently coated MWCNT nanohybrid: fabrication and observation of enhanced photoconductivity. Nanotechnology 17:728–733CrossRefGoogle Scholar
  41. Yang ST, Wang HF, Wang YX, Wang YW, Nie HY, Liu YF (2011) Removal of carbon nanotubes from aqueous environment with filter paper. Chemosphere 82:621–626CrossRefGoogle Scholar
  42. Zelmanov G, Semiat R (2008) Iron(3) oxide-based nanoparticles as catalysts in advanced organic aqueous oxidation. Water Res 42:492–498CrossRefGoogle Scholar
  43. Zhang J, Zou HL, Qing Q, Yang YL, Li QW, Liu ZF, Guo XY, Du ZL (2003) Effect of chemical oxidation on the structure of single-walled carbon nanotubes. J Phys Chem B 107:3712CrossRefGoogle Scholar
  44. Zhang Y, Shen Y, Kuehner D, Wu S, Su Z, Ye S, Niu L (2008) Directing single-walled carbon nanotubes to self-assemble at water/oil interfaces and facilitate electron transfer. Chem Commun 36:4273–4275CrossRefGoogle Scholar
  45. Zhang GL, Zhang JW, Wang L, Meng Q, Wang JH (2012) Fouling mechanism of low-pressure hollow fiber membranes used in separating nanosized photocatalysts. J Membr Sci 389:532–543CrossRefGoogle Scholar
  46. Zhao D, Yang X, Zhang H, Chen C, Wang X (2010) Effect of environmental conditions on Pb(II) adsorption on β-MnO2. Chem Eng J 164:49–55CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2015

Authors and Affiliations

  1. 1.School of Resource and Environmental ScienceWuhan UniversityWuhanPeople’s Republic China
  2. 2.School of Environmental Science and EngineeringTaiyuan University of TechnologyTaiyuanPeople’s Republic China

Personalised recommendations