Skip to main content
SpringerLink
Log in

An antifouling catechol/chitosan-modified polyvinylidene fluoride membrane for sustainable oil-in-water emulsions separation

  • Research Article
  • Published:
Frontiers of Environmental Science & Engineering Aims and scope Submit manuscript

Abstract

Low-pressure membrane filtrations are considered as effective technologies for sustainable oil/water separation. However, conventional membranes usually suffer from severe pore clogging and surface fouling, and thus, novel membranes with superior wettability and antifouling features are urgently required. Herein, we report a facile green approach for the development of an underwater superoleophobic microfiltration membrane via one-step oxidant-induced ultrafast co-deposition of naturally available catechol/chitosan on a porous polyvinylidene fluoride (PVDF) substrate. Membrane morphology and surface chemistry were studied using a series of characterization techniques. The as-prepared membrane retained the original pore structure due to the ultrathin and uniform catechol/chitosan coating. It exhibited ultrahigh pure water permeability and robust chemical stability under harsh pH conditions. Moreover, the catechol/chitosan hydrophilic coating on the membrane surface acting as an energetic barrier for oil droplets could minimize oil adhesion on the surface, which endowed the membrane with remarkable antifouling property and reusability in a cyclic oil-in-water (O/W) emulsion separation. The modified membrane exhibited a competitive flux of ~428 L/(m2·h·bar) after three filtration cycles, which was 70% higher than that of the pristine PVDF membrane. These results suggest that the novel underwatersuperoleophobic membrane can potentially be used for sustainable O/W emulsions separation, and the proposed green facile modification approach can also be applied to other water-remediation materials considering its low cost and simplicity.

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

Similar content being viewed by others

References

  • Akhtar S, Khalid N, Ahmed I, Shahzad A, Suleria H A R (2014). Physicochemical characteristics, functional properties, and nutritional benefits of peanut oil: A review. Critical Reviews in Food Science and Nutrition, 54(12): 1562–1575

    Article  CAS  Google Scholar 

  • Behboodi-Sadabad F, Zhang H, Trouillet V, Welle A, Plumeré N, Levkin P A (2017). UV-triggered polymerization, deposition, and patterning of plant phenolic compounds. Advanced Functional Materials, 27 (22): 1700127

    Article  Google Scholar 

  • Bera B, Carrier O, Backus E H G, Bonn M, Shahidzadeh N, Bonn D (2018). Counteracting interfacial energetics for wetting of hydro-phobic surfaces in the presence of surfactants. Langmuir, 34(41): 12344–12349

    Article  CAS  Google Scholar 

  • Cao C, Kim E, Liu Y, Kang M, Li J, Yin J J, Liu H, Qu X, Liu C, Bentley W E, Payne G F (2018). Radical scavenging activities of biomimetic catechol-chitosan films. Biomacromolecules, 19(8): 3502–3514

    Article  CAS  Google Scholar 

  • Chen Y, Liu Q (2019). Oxidant-induced plant phenol surface chemistry for multifunctional coatings: Mechanism and potential applications. Journal of Membrane Science, 570–571: 176–183

    Article  Google Scholar 

  • Chew N, Zhao S, Malde C, Wang R (2018). Polyvinylidene fluoride membrane modification via oxidant-induced dopamine polymerization for sustainable direct-contact membrane distillation. Journal of Membrane Science, 563: 31–42

    Article  CAS  Google Scholar 

  • Chew N G P, Zhao S, Malde C, Wang R (2017). Superoleophobic surface modification for robust membrane distillation performance. Journal of Membrane Science, 541: 162–173

    Article  CAS  Google Scholar 

  • Chew N G P, Zhao S, Loh C H, Permogorov N, Wang R (2017). Surfactant effects on water recovery from produced water via direct-contact membrane distillation. Journal of Membrane Science, 528: 126–134

    Article  CAS  Google Scholar 

  • Cui J, Zhou Z, Xie A, Meng M, Cui Y, Liu S, Lu J, Zhou S, Yan Y, Dong H (2019). Bio-inspired fabrication of superhydrophilic nanocomposite membrane based on surface modification of SiO2 anchored by polydopamine towards effective oil-water emulsions separation. Separation and Purification Technology, 209: 434–142

    Article  CAS  Google Scholar 

  • Gao S, Zhu Y, Wang J, Zhang F, Li J, Jin J (2018). Layer-by-Layer construction of Cu2+/alginate multilayer modified ultrafiltration membrane with bioinspired superwetting property for high-efficient crude-oil-in-water emulsion separation. Advanced Functional Materials, 28(49): 1801944

    Article  Google Scholar 

  • Guo D, Xiao Y, Li T, Zhou Q, Shen L, Li R, Xu Y, Lin H (2020). Fabrication of high-performance composite nanofiltration membranes for dye wastewater treatment: mussel-inspired layer-by-layer self-assembly. Journal of Colloid and Interface Science, 560: 273–283

    Article  CAS  Google Scholar 

  • Guo X, Li C, Li C, Wei T, Tong L, Shao H, Zhou Q, Wang L, Liao Y (2019). G-CNTs/PVDF mixed matrix membranes with improved antifouling properties and filtration performance. Frontiers of Environmental Science & Engineering, 13(6): 81

    Article  Google Scholar 

  • He M, Gao K, Zhou L, Jiao Z, Wu M, Cao J, You X, Cai Z, Su Y, Jiang Z (2016). Zwitterionic materials for antifouling membrane surface construction. Acta Biomaterialia, 40: 142–152

    Article  Google Scholar 

  • Kolesnyk I, Konovalova V, Kharchenko K, Burban A, Kujawa J, Kujawski W (2020). Enhanced transport and antifouling properties of polyethersulfone membranes modified with α-amylase incorporated in chitosan-based polymeric micelles. Journal of Membrane Science, 595: 117605

    Article  CAS  Google Scholar 

  • Lee H, Dellatore S M, Miller W M, Messersmith P B (2007). Mussel-inspired surface chemistry for multifunctional coatings. Science, 318 (5849): 426–430

    Article  CAS  Google Scholar 

  • Lee M, Lee S H, Oh I K, Lee H (2017). Microwave-accelerated rapid, chemical oxidant-free, material-independent surface chemistry of poly(dopamine). Small, 13(4): 1600443

    Article  Google Scholar 

  • Li D, Yang X, Zhou Z, Jiang B, Tawfik A, Zhao S, Meng F (2019). Molecular traits of phenolic moieties in dissolved organic matter: Linkages with membrane fouling development. Environment International, 133: 105202

    Article  CAS  Google Scholar 

  • Liao Y, Wang R, Fane A G (2014). Fabrication of bioinspired composite nanofiber membranes with robust superhydrophobicity for direct contact membrane distillation. Environmental Science & Technology, 48(11): 6335–6341

    Article  CAS  Google Scholar 

  • Liao Y, Tian M, Wang R (2017). A high-performance and robust membrane with switchable super-wettability for oil/water separation under ultralow pressure. Journal of Membrane Science, 543: 123–132

    Article  CAS  Google Scholar 

  • Luo C, Liu Q (2017). Oxidant-induced high-efficient mussel-inspired modification on pvdf membrane with superhydrophilicity and underwater superoleophobicity characteristics for oil/water separation. ACS Applied Materials & Interfaces, 9(9): 8297–8307

    Article  CAS  Google Scholar 

  • Meng F, Song F, Yao Y, Liu G, Zhao S (2020). Ultrastable nanofiltration membranes engineered by polydopamine-assisted polyelectrolyte layer-by-layer assembly for water reclamation. ACS Sustainable Chemistry & Engineering, 8(29): 10928–10938

    CAS  Google Scholar 

  • Miller D J, Dreyer D R, Bielawski C W, Paul D R, Freeman B D (2017). Surface modification of water purification membranes. Angewandte Chemie International Edition, 56(17): 4662–4711

    Article  CAS  Google Scholar 

  • Qiu W Z, Zhong Q Z, Du Y, Lv Y, Xu Z K (2016). Enzyme-triggered coatings of tea catechins/chitosan for nanofiltration membranes with high performance. Green Chemistry, 18(23): 6205–6208

    Article  CAS  Google Scholar 

  • Qu J, Wang H, Wang K, Yu G, Ke B, Yu H Q, Ren H, Zheng X, Li J, Li W W, Gao S, Gong H (2019). Municipal wastewater treatment in China: Development history and future perspectives. Frontiers of Environmental Science & Engineering, 13(6): 88

    Article  Google Scholar 

  • Ryu J H, Messersmith P B, Lee H (2018). Polydopamine surface chemistry: A decade of discovery. ACS Applied Materials & Interfaces, 10(9): 7523–7540

    Article  CAS  Google Scholar 

  • Shin M, Park E, Lee H (2019). Plant-inspired pyrogallol-containing functional materials. Advanced Functional Materials, 29(43): 1903022

    Article  CAS  Google Scholar 

  • Tian M, Liao Y, Wang R (2020). Engineering a superwetting thin film nanofibrous composite membrane with excellent antifouling and self-cleaning properties to separate surfactant-stabilized oil-in-water emulsions. Journal of Membrane Science, 596: 117721

    Article  CAS  Google Scholar 

  • Wu Z, Zhang C, Peng K, Wang Q, Wang Z (2018). Hydrophilic/underwater superoleophobic graphene oxide membrane intercalated by TiO2 nanotubes for oil/water separation. Frontiers of Environmental Science & Engineering, 12(3): 15

    Article  Google Scholar 

  • Xu Y, Guo D, Li T, Xiao Y, Shen L, Li R, Jiao Y, Lin H (2020). Manipulating the mussel-inspired co-deposition of tannic acid and amine for fabrication of nanofiltration membranes with an enhanced separation performance. Journal of Colloid and Interface Science, 565: 23–34

    Article  CAS  Google Scholar 

  • Xu Y C, Wang Z X, Cheng X Q, Xiao Y C, Shao L (2016). Positively charged nanofiltration membranes via economically mussel-substance-simulated co-deposition for textile wastewater treatment. Chemical Engineering Journal, 303: 555–564

    Article  CAS  Google Scholar 

  • Yi G, Fan X, Quan X, Chen S, Yu H (2019). Comparison of CNT-PVA membrane and commercial polymeric membranes in treatment of emulsified oily wastewater. Frontiers of Environmental Science & Engineering, 13(2): 23

    Article  Google Scholar 

  • Yang H C, Waldman R Z, Wu M B, Hou J, Chen L, Darling S B, Xu Z K (2018). Dopamine: Just the right medicine for membranes. Advanced Functional Materials, 28(8): 1705327

    Article  Google Scholar 

  • Yu Z, Pan Y, He Y, Zeng G, Shi H, Di H (2015). Preparation ofa novel anti-fouling β-cyclodextrin-PVDF membrane. RSC Advances, 5 (63): 51364–51370

    Article  CAS  Google Scholar 

  • Zhang C, Ou Y, Lei W X, Wan L S, Ji J, Xu Z K (2016). CuSO4/H2O2-induced rapid deposition of polydopamine coatings with high uniformity and enhanced stability. Angewandte Chemie International Edition, 55(9): 3054–3057

    Article  CAS  Google Scholar 

  • Zhang H, Shen Y, Li M, Zhu G, Feng H, Li J (2019). Egg shell powders-coated membrane for surfactant-stabilized crude oil-in-water emulsions efficient separation. ACS Sustainable Chemistry & Engineering, 7(12): 10880–10887

    Article  CAS  Google Scholar 

  • Zhang J, Zhang F, Song J, Liu L, Si Y, Yu J, Ding B (2019). Electrospun flexible nanofibrous membranes for oil/water separation. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 7 (35): 20075–20102

    Article  CAS  Google Scholar 

  • Zhang W, Zhu Y, Liu X, Wang D, Li J, Jiang L, Jin J (2014). Salt-induced fabrication of superhydrophilic and underwater super-oleophobic PAA-g-PVDF membranes for effective separation of oil-in-water emulsions. Angewandte Chemie International Edition, 53(3): 856–860

    Article  CAS  Google Scholar 

  • Zhao S, Minier-Matar J, Chou S, Wang R, Fane A G, Adham S (2017). Gas field produced/process water treatment using forward osmosis hollow fiber membrane: Membrane fouling and chemical cleaning. Desalination, 402: 143–151

    Article  CAS  Google Scholar 

  • Zolfaghari R, Fakhru’l-Razi A, Abdullah L C, Elnashaie S S E H, Pendashteh A (2016). Demulsification techniques of water-in-oil and oil-in-water emulsions in petroleum industry. Separation and Purification Technology, 170: 377–407

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 51808564 and 51878675), the State Key Laboratory of Separation Membranes and Membrane Processes (Tiangong University, Grant No. M1-201803) and the National Key R&D Program of China (Grant No. 2017YFE0114300). The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Author information

Authors and Affiliations

  1. School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510006, China

    Shanshan Zhao, Zhu Tao, Muqiao Han & Fangang Meng

  2. State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin, 300387, China

    Shanshan Zhao, Bin Zhao, Liang Wang & Fangang Meng

  3. Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Guangzhou, 510006, China

    Shanshan Zhao, Zhu Tao, Muqiao Han & Fangang Meng

  4. School of Material Science and Engineering, Sun Yat-sen University, Guangzhou, 510006, China

    Liwei Chen & Xuelin Tian

Authors
  1. Shanshan Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Zhu Tao
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Liwei Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Muqiao Han
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Bin Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Xuelin Tian
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Liang Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Fangang Meng
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Liang Wang or Fangang Meng.

Additional information

Highlights

• Underwater superoleophobic membrane was fabricated by deposition of catechol/chitosan.

• The membrane had ultrahigh pure water flux and was stable under harsh pH conditions.

• The membrane exhibited remarkable antifouling property in O/W emulsion separation.

• The hydration layer on the membrane surface prevented oil droplets adhesion.

Supplementary materials

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhao, S., Tao, Z., Chen, L. et al. An antifouling catechol/chitosan-modified polyvinylidene fluoride membrane for sustainable oil-in-water emulsions separation. Front. Environ. Sci. Eng. 15, 63 (2021). https://doi.org/10.1007/s11783-020-1355-5

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s11783-020-1355-5

Keywords

Search

Navigation