Skip to main content
SpringerLink
Log in

Influence of graphene oxide sheets on the pore structure and filtration performance of a novel graphene oxide/silica/polyacrylonitrile mixed matrix membrane

  • Composites
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

The novel graphene oxide (GO)/silica (SiO2)/polyacrylonitrile (PAN) mixed matrix membranes (MMMs) with high filtration flux and excellent antifouling performance were designed and fabricated in situ by the method of non-solvent induced phase separation (NIPS) from the precursor of PAN hybridized with GO, tetraethoxysilane and 3-aminopropyltriethoxysilane. The influences of GO sheets on the pore and chemical structure, hydrophilic nature and filtration performance of derived GO/SiO2/PAN MMMs were investigated by the scanning electron microscopy, field emission scanning electron microscopy, atomic force microscopy, energy-dispersive X-ray, Fourier transform infrared spectrometer, pure water contact angles and filtration performance. Results indicated that in situ incorporation of GO sheets and SiO2 molecules into PAN matrix via NIPS reconstructs the porous structure of derived GO/SiO2/PAN MMMs with the upright finger-like holes, porous bottom, thinner top layer and high porosity. The spontaneous surface migration or segregation of hydrophilic GO sheets and SiO2 molecules as well as their synergistic interaction occurred during NIPS greatly ameliorate the top surface structure and property of derived membranes with smoother surface, uniform pore structure and good hydrophilicity. The derived GO/SiO2/PAN MMMs exhibit a high water filtration flux of 387 L m−2 h−1 with the bull serum albumin rejection rate up to 99% and significant enhancement of antifouling performance.

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.

Institutional subscriptions

Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
Figure 7
Figure 8
Figure 9
Figure 10
Figure 11
Figure 12

Similar content being viewed by others

References

  1. Ma Y, Di H-H, Yu Z-X, Liang L, Lv L, Pan Y, Zhang Y-Y, Yin D (2016) Fabrication of silica-decorated graphene oxide nanohybrids and the properties of composite epoxy coatings research. Appl Surf Sci 360:936–945

    Article  CAS  Google Scholar 

  2. Gao S, Sun J, Liu P, Zhang F, Zhang W, Yuan S, Li J, Jin J (2016) A Robust polyionized hydrogel with an unprecedented underwater anti-crude-oil-adhesion property. Adv Mater 28:5307–5314

    Article  CAS  Google Scholar 

  3. Yin J, Deng B (2015) Polymer-matrix nanocomposite membranes for water treatment. J Membr Sci 479:256–275

    Article  CAS  Google Scholar 

  4. Chatterjee S, De S (2015) Adsorptive removal of arsenic from groundwater using a novel high flux polyacrylonitrile (PAN)–laterite mixed matrix ultrafiltration membrane. Environ Sci Water Res Technol 1:227–243

    Article  CAS  Google Scholar 

  5. Yin J, Deng B (2015) Polymer-matrix nanocomposite membranes for water treatment. J Membr Sci 479:256–275

    Article  CAS  Google Scholar 

  6. Ng LY, Mohammad AW, Leo CP, Hilal N (2013) Polymeric membranes incorporated with metal/metal oxide nanoparticles: a comprehensive review. Desalination 308:15–33

    Article  CAS  Google Scholar 

  7. Asatekin A, Kang S, Elimelech M, Mayes AM (2007) Anti-fouling ultrafiltration membranes containing polyacrylonitrile-graft-poly(ethylene oxide) comb copolymer additives. J Membr Sci 298:136–146

    Article  CAS  Google Scholar 

  8. Kochkodan V, Hilal N (2015) A comprehensive review on surface modified polymer membranes for biofouling mitigation. Desalination 356:187–207

    Article  CAS  Google Scholar 

  9. Zhang F, Zhang W-B, Yu Y, Deng B, Li J-Y, Jin J (2013) Sol–gel preparation of PAA-g-PVDF/TiO2 nanocomposite hollow fiber membranes with extremely high water flux and improved antifouling property. J Membr Sci 432:25–32

    Article  CAS  Google Scholar 

  10. Pang R, Li J, Wei K, Sun X, Shen J, Han W, Wang J (2011) In situ preparation of Al-containing PVDF ultrafiltration membrane via sol-gel process J Colloid Interf Sci 364:373–378

    CAS  Google Scholar 

  11. Deng B, Yu M, Yang X-X, Zhang B-W, Li L-F, Xie L-D, Li J-Y, Lu X-F (2010) Antifouling microfiltration membranes prepared from acrylic acid or methacrylic acid grafted poly(vinylidene fluoride) powder synthesized via pre-irradiation induced graft polymerization. J Membr Sci 350:252–258

    Article  CAS  Google Scholar 

  12. Shi Q, Su Y-L, Zhu S-P, Li C, Zhao Y-Y, Jiang Z-Y (2007) A facile method for synthesis of pegylated polyethersulfone and its application in fabrication of antifouling ultrafiltration membrane. J Membr Sci 303:204–212

    Article  CAS  Google Scholar 

  13. Shannon MA, Bohn PW, Elimelech M, Georgiadis JG, Marinas BJ, Mayes AM (2008) Science and technology for water purification in the coming decades. Nature 452:301–310

    Article  CAS  Google Scholar 

  14. Liang H-Q, Wu Q-Y, Wan L-S, Huang X-J, Xu Z-K (2014) Thermally induced phase separation followed by in situ sol-gel process: a novel method for PVDF/SiO2 hybrid membranes. J Membr Sci 465:56–67

    Article  CAS  Google Scholar 

  15. Li X, Fang X-F, Pang R-Z, Li J-S, Sun X-Y, Shen J-Y, Han W-Q, Wang L-J (2014) Self-assembly of TiO2 nanoparticles around the pores of PES ultrafiltration membrane for mitigating organic fouling. J Membr Sci 467:226–235

    Article  CAS  Google Scholar 

  16. Park S-Y, Chung J-W, Chae Y-K, Kwak S-Y (2013) Amphiphilic thiol functional linker mediated sustainable anti-biofouling ultrafiltration nanocomposite comprising a silver nanoparticles and poly(vinylidene fluoride) membrane. ACS Appl Mater Interf 5:10705–10714

    Article  CAS  Google Scholar 

  17. Chen W-J, Su Y-L, Zhang L, Shi Q, Peng J-M, Jiang Z-Y (2010) In situ generated silica nanoparticles as pore-forming agent for enhanced permeability of cellulose acetate membranes. J Membr Sci 348:75–83

    Article  CAS  Google Scholar 

  18. Wu L-S, Sun J-F, Lv Z-Y, Chen Y (2016) In-situ preparation of poly(ether imide)/amino functionalized silica mixed matrix membranes for application in enzyme separation. Mater Des 92:610–620

    Article  CAS  Google Scholar 

  19. Wu H, Mansouri J, Chen V (2013) Silica nanoparticles as carriers of antifouling ligands for PVDF ultrafiltration membranes. J Membr Sci 433:135–151

    Article  CAS  Google Scholar 

  20. Joshi RK, Carbone P, Wang F-C, Kravets VG, Su Y, Grigorieva IV, Wu HA, Geim AK, Nair R-R (2014) Precise and ultrafast molecular sieving through graphene oxide membranes. Science 343:752–754

    Article  CAS  Google Scholar 

  21. Zhang J-Q, Pan X-L, Xue Q-Z, He D-L, Zhu L, Guo Q-K (2017) Antifouling hydrolyzed polyacrylonitrile/graphene oxide membrane with spindle-knotted structure for highly effective separation of oil-water emulsion. J Membr Sci 532:38–46

    Article  CAS  Google Scholar 

  22. Jhaveri JH, Patel CM, Murthy ZVP (2017) Preparation, characterization and application of GO-TiO2/PVC mixed matrix membranes for improvement in performance. J Ind Eng Chem 52:138–146

    Article  CAS  Google Scholar 

  23. Ho KC, Teow YH, Ang WL, Mohammad AW (2017) Novel GO/OMWCNTs mixed-matrix membrane with enhanced antifouling property for palm oil mill effluent treatment. Sep Purif Technol 177:337–349

    Article  CAS  Google Scholar 

  24. Kumar M, Gholamvand Z, Morrissey A, Nolan K, Ulbricht M, Lawler J (2016) Preparation and characterization of low fouling novel hybrid ultrafiltration membranes based on the blends of GO-TiO2 nanocomposite and polysulfone for humic acid removal. J Membr Sci 506:38–49

    Article  CAS  Google Scholar 

  25. Xia S-J, Yao L-J, Zhao Y, Li N-N, Zheng Y (2015) Preparation of graphene oxide modified polyamide thin film composite membranes with improved hydrophilicity for natural organic matter removal. Chem Eng J 280:720–727

    Article  CAS  Google Scholar 

  26. Wu H-Q, Tang B-B, Wu P-Y (2014) Development of novel SiO2–GO nanohybrid/polysulfone membrane with enhanced performance. J Membr Sci 451:94–102

    Article  CAS  Google Scholar 

  27. Li Z-K, Lang W-Z, Miao W, Yan X, Guo Y-J (2016) Preparation and properties of PVDF/SiO2@GO nanohybrid membranes via thermally induced phase separation method. J Membr Sci 511:151–161

    Article  CAS  Google Scholar 

  28. Nina IK, Patricia JO, Benjamin RM, Thomas EM, Sergey AC, Eugenia VB, Alexandr DG (1999) Layer-by-layer assembly of ultrathin composite films from micron-sized graphite oxide sheets and polycations. Chem Mater 11:771–778

    Article  Google Scholar 

  29. Vanegas ME, Quijada R, Serafini D (2009) Microporous membranes prepared via thermally induced phase separation from metallocenic syndiotactic polypropylenes. Polymer 50:2081–2086

    Article  CAS  Google Scholar 

  30. Vatanpour V, Madaeni SS, Khataee AR, Salehi E, Zinadini S, Monfared H-A (2012) TiO2 embedded mixed matrix PES nanocomposite membranes: influence of different sizes and types of nanoparticles on antifouling and performance. Desalination 292:19–29

    Article  CAS  Google Scholar 

  31. Choi J-H, Jegal J, Kim W-N (2006) Fabrication and characterization of multi-walled carbon nanotubes/polymer blend membranes. J Membr Sci 284:406–415

    Article  CAS  Google Scholar 

  32. Zhao H, Wu L, Zhou Z, Zhang L, Chen H (2013) Improving the antifouling property of polysulfone ultrafiltration membrane by incorporation of isocyanate-treated graphene oxide. Phys Chem Chem Phys 15:9084–9092

    Article  CAS  Google Scholar 

  33. Vatanpour V, Madaeni SS, Moradian R, Zinadini S, Astinchap B (2011) Fabrication and characterization of novel antifouling nanofiltration membrane prepared from oxidized multiwalled carbon nanotube/polyethersulfone nanocomposite. J Membr Sci 375:284–294

    Article  CAS  Google Scholar 

  34. Schaefer DM, Carpenter M, Gady B, Reifenberger R, Demejo LP, Rimai DS (1995) Surface roughness and its influence on particle adhesion using atomic force techniques. J Adhes Sci Technol 9:1049–1062

    Article  CAS  Google Scholar 

  35. Zhu Z-Y, Jiang J-L, Wang X-D, Huo X-N, Xu Y-W, Li Q-Q, Wang L (2017) Improving the hydrophilic and antifouling properties of polyvinylidene fluoride membrane by incorporation of novel nanohybrid GO@SiO2 particles. Chem Eng J 314:266–276

    Article  CAS  Google Scholar 

Download references

Acknowledgements

The authors gratefully acknowledge the financial support under National Key R&D Program of China (2017YFB0603403) and National Natural Science Foundation of China (21506020, 21576035, 21436009, 21376037, 21676044); the Fundamental Research Funds for the Central Universities of China (DUT16RC(4)05); China Postdoctoral Science Foundation (2014M561232); and State Key Laboratory of Separation Membranes and Membrane Processes (Tianjin Polytechnic University) (M2-201509). Much thanks to Dr. and Prof. Xianshe Feng for his English polishing.

Author information

Authors and Affiliations

  1. State key Laboratory of Fine Chemicals, Carbon Research Laboratory, School of Chemical Engineering, Dalian University of Technology, 2 Linggong Road, Dalian, 116024, China

    Qiao Liu, Lin Li, Xin Jin, Chunlei Wang & Tonghua Wang

Authors
  1. Qiao Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Lin Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xin Jin
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Chunlei Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Tonghua Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Lin Li or Tonghua Wang.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liu, Q., Li, L., Jin, X. et al. Influence of graphene oxide sheets on the pore structure and filtration performance of a novel graphene oxide/silica/polyacrylonitrile mixed matrix membrane. J Mater Sci 53, 6505–6518 (2018). https://doi.org/10.1007/s10853-018-1990-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-018-1990-4

Search

Navigation