Skip to main content
Log in

Controlled reduction and fabrication of graphene oxide membrane for improved permeance and water purification performance

  • Chemical routes to materials
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

It has been found that moderately reduced graphene oxide (RGO) membrane which was applicable to the field of nanofiltration had both good hydrophilicity and appropriate layer spacing. However, existing GO reduction technologies are usually toxic, complex and uncontrollable. Therefore, it is necessary to seek a green and controllable method to develop the partially RGO membrane (RGOM) which has outstanding water purification ability. In this work, GO laminar membranes (GOM) were prepared via vacuum filter, and L ( +)-ascorbic acid (LAA) was employed as a reduction agent to prepare the RGOM. Subsequently, SEM, XPS, Raman and XRD tests were conducted to characterize the physical and chemical properties of RGOM. Furthermore, the effect of reduction degree on water purification performance was determined. Owing to the combined effect of D-spacing and sp2 domains with ultralow friction, GOM treated in LAA for 10 min (10-RGOM) exhibited a great water flux of 27.62 L m−2 h−1 bar−1 which was 238% higher than that of GOM and also showed excellent dye rejection. Furthermore, compared with GO, 10-RGOM exhibited better structural stability and superior separation performance in different pH environments.

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

Access this article

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

Similar content being viewed by others

References

  1. Mi B (2014) Graphene oxide membranes for ionic and molecular sieving. Science 343(6172):740–742

    Article  CAS  Google Scholar 

  2. Mohmood I, Lopes CB, Lopes I et al (2013) Nanoscale materials and their use in water contaminants removal-a review. Environ Sci Pollut Res 20:1239–1260

    Article  CAS  Google Scholar 

  3. Du Y, Huang L, Wang Y et al (2020) Preparation of graphene oxide / silica hybrid composite membranes and performance studies in water treatment. J Mater Sci 55:11188–11202. https://doi.org/10.1007/s10853-020-04774-5

    Article  CAS  Google Scholar 

  4. Agenson KO, Oh JI, Urase T (2003) Retention of a wide variety of organic pollutants by different nanofiltration/reverse osmosis membranes: controlling parameters of process. J Memb Sci 225:91–103

    Article  CAS  Google Scholar 

  5. Naono H, Hakuman M, Shimoda M et al (1996) Separation of water and ethanol by the adsorption technique: selective desorption of water from micropores of active carbon. J Colloid Interface Sci 182:230–238

    Article  CAS  Google Scholar 

  6. Mehta GD (1982) Comparison of membrane processes with distillation for alcohol/water separation. J Memb Sci 12:1–26

    Article  CAS  Google Scholar 

  7. Neves CMSS, Granjo JFO, Freire MG et al (2011) Separation of ethanol–water mixtures by liquid–liquid extraction using phosphonium-based ionic liquids. Green Chem 13:1517–1526

    Article  CAS  Google Scholar 

  8. Pendergast MM, Hoek EMV (2011) A review of water treatment membrane nanotechnologies. Energy Environ Sci 4:1946–1971

    Article  CAS  Google Scholar 

  9. Van der Bruggen B, Mänttäri M, Nyström M (2008) Drawbacks of applying nanofiltration and how to avoid them: a review. Sep Purif Technol 63:251–263

    Article  Google Scholar 

  10. Daufin G, Escudier JP, Carrére H et al (2001) Recent and emerging applications of membrane processes in the food and dairy industry. Food Bioprod Process Trans Inst Chem Eng Part C 79:89–102

    Article  CAS  Google Scholar 

  11. Sun SP, Hatton TA, Chan SY, Chung TS (2012) Novel thin-film composite nanofiltration hollow fiber membranes with double repulsion for effective removal of emerging organic matters from water. J Memb Sci 401–402:152–162

    Article  Google Scholar 

  12. Choi W, Choi J, Bang J, Lee JH (2013) Layer-by-layer assembly of graphene oxide nanosheets on polyamide membranes for durable reverse-osmosis applications. ACS Appl Mater Interfaces 5:12510–12519

    Article  CAS  Google Scholar 

  13. Ma J, He Y, Shi H et al (2019) Stable graphene oxide-based composite membranes intercalated with montmorillonite nanoplatelets for water purification. J Mater Sci 54(3):2241–2255. https://doi.org/10.1007/s10853-018-2997-6

    Article  CAS  Google Scholar 

  14. Cohen-Tanugi D, Grossman JC (2012) Water desalination across nanoporous graphene. Nano Lett 12:3602–3608

    Article  CAS  Google Scholar 

  15. Boukhvalov DW, Katsnelson MI, Son YW (2013) Origin of anomalous water permeation through graphene oxide membrane. Nano Lett 13:3930–3935

    Article  CAS  Google Scholar 

  16. Nair R, Wu H, Jayaram P, Grigorieva I, Geim A (2012) Unimpeded permeation of water through helium-leak–tight graphene-based membranes. Science 335(6067):442–444

    Article  CAS  Google Scholar 

  17. Lerf A, Buchsteiner A, Pieper J et al (2006) Hydration behavior and dynamics of water molecules in graphite oxide. J Phys Chem Solids 67:1106–1110

    Article  CAS  Google Scholar 

  18. Zheng S, Tu Q, Urban JJ et al (2017) Swelling of graphene oxide membranes in aqueous solution: characterization of interlayer spacing and insight into water transport mechanisms. ACS Nano 11:6440–6450

    Article  CAS  Google Scholar 

  19. Baskoro F, Wong CB, Kumar SR et al (2018) Graphene oxide-cation interaction: Inter-layer spacing and zeta potential changes in response to various salt solutions. J Memb Sci 554:253–263

    Article  CAS  Google Scholar 

  20. Hung WS, Tsou CH, De Guzman M et al (2014) Cross-linking with diamine monomers to prepare composite graphene oxide-framework membranes with varying d-spacing. Chem Mater 26:2983–2990

    Article  CAS  Google Scholar 

  21. Jia Z, Wang Y (2015) Covalently crosslinked graphene oxide membranes by esterification reactions for ions separation. J Mater Chem A 3:4405–4412

    Article  CAS  Google Scholar 

  22. Pei S, Zhao J, Du J et al (2010) Direct reduction of graphene oxide films into highly conductive and flexible graphene films by hydrohalic acids. Carbon N Y 48:4466–4474

    Article  CAS  Google Scholar 

  23. Chua CK, Pumera M (2014) Chemical reduction of graphene oxide: A synthetic chemistry viewpoint. Chem Soc Rev 43:291–312

    Article  CAS  Google Scholar 

  24. Yang E, Ham M-H, Park HB et al (2018) Tunable semi-permeability of graphene-based membranes by adjusting reduction degree of laminar graphene oxide layer. J Membr Sci 547:73–79

    Article  CAS  Google Scholar 

  25. Fan X, Cai C, Gao J et al (2020) Hydrothermal reduced graphene oxide membranes for dyes removing. Sep Purif Technol 241:116730–116737

    Article  CAS  Google Scholar 

  26. Li S, Wang M, Lian Y (2016) Electrochemical capacitors based on the composite of graphene and nickel foam. Sci Chian-Chem 59:405–411

    Article  CAS  Google Scholar 

  27. Qiu L, Zhang X, Yang W et al (2011) Controllable corrugation of chemically converted graphene sheets in water and potential application for nanofiltration. Chem Commun 47:5810–5812

    Article  CAS  Google Scholar 

  28. Maddinedi SB, Mandal BK, Vankayala R et al (2014) Casein mediated green synthesis and decoration of reduced graphene oxide. Spectrochim Acta— Part A Mol Biomol Spectrosc 126:227–231

    Article  CAS  Google Scholar 

  29. Yu H, He Y, Xiao G et al (2019) Weak-reduction graphene oxide membrane for improving water purification performance. J Mater Sci Technol 39:106–112. https://doi.org/10.1016/j.jmst.2019.08.024

    Article  Google Scholar 

  30. De Silva KKH, Huang HH, Joshi RK, Yoshimura M (2017) Chemical reduction of graphene oxide using green reductants. Carbon N Y 119:190–199

    Article  Google Scholar 

  31. Fernández-Merino MJ, Guardia L, Paredes JI et al (2010) Vitamin C is an ideal substitute for hydrazine in the reduction of graphene oxide suspensions. J Phys Chem C 114:6426–6432

    Article  Google Scholar 

  32. Iskandar F, Hikmah U, Stavila E et al (2017) Microwave-assisted reduction method under nitrogen atmosphere for synthesis and electrical conductivity improvement of reduced graphene oxide (rGO). RSC Adv 7(83):52391–52397

    Article  CAS  Google Scholar 

  33. Sui Z, Zhang X, Lei Y, Luo Y (2011) Easy and green synthesis of reduced graphite oxide-based hydrogels. Carbon N Y 49:4314–4321

    Article  CAS  Google Scholar 

  34. Dua V, Surwade SP, Ammu S et al (2010) All-organic vapor sensor using inkjet-printed reduced graphene oxide. Angew Chemie—Int Ed 49:2154–2157

    Article  CAS  Google Scholar 

  35. Ding H, Zhang S, Chen JT et al (2015) Reduction of graphene oxide at room temperature with vitamin C for RGO-TiO<inf>2</inf> photoanodes in dye-sensitized solar cell. Thin Solid Films 584:29–36

    Article  CAS  Google Scholar 

  36. Li Y, Zhao W, Weyland M et al (2019) Thermally reduced nanoporous graphene oxide membrane for desalination. Environ Sci Technol 53:8314–8323

    Article  CAS  Google Scholar 

  37. Fan X, Peng W, Li Y et al (2008) Deoxygenation of exfoliated graphite oxide under alkaline conditions: a green route to graphene preparation. Adv Mater 20:4490–4493

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51774245), the Applied Basic Research Program of Science and Technology Department of Sichuan Province (2018JY0517) and Open Fund (PLN161) of State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation.

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Yi He, Siming Yan or Yi Fan.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Gao, Y., He, Y., Yan, S. et al. Controlled reduction and fabrication of graphene oxide membrane for improved permeance and water purification performance. J Mater Sci 55, 15130–15139 (2020). https://doi.org/10.1007/s10853-020-05073-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-020-05073-9

Navigation