Elsevier

Journal of Membrane Science

Volume 640, 15 December 2021, 119863
Journal of Membrane Science

Tailored thin film nanocomposite membrane incorporated with Noria for simultaneously overcoming the permeability-selectivity trade-off and the membrane fouling in nanofiltration process

https://doi.org/10.1016/j.memsci.2021.119863Get rights and content

Highlights

  • A novel TFN membrane was fabricated by incorporating Noria.

  • PIP-Noria-TMC membrane possessed a wrinkled structure and a thinner PA layer.

  • Incorporation of Noria enhanced hydrophilicity and negative charge of membranes.

  • Permeability-selectivity trade-off and membrane fouling was addressed jointly.

  • Mono/divalent salt selectivity of PIP-Noria-TMC membrane can be as high as 47.

Abstract

Membrane fouling as well as the “trade-off effect” between water permeability and selectivity are the grand challenges for nanofiltration (NF) membranes. In this study, a macrocyclic molecule, Noria, was embedded in the polyamide layer to fabricate a thin film nanocomposite (TFN) membrane with high performances of separation and antifouling. Noria was first synthesized and dissolved in a piperazine (PIP) aqueous solution. Then the TFN membrane (i.e., PIP-Noria-TMC membrane, TMC is the abbreviation of 1,3,5-benzenetricarbonyl trichloride) was prepared by interfacial polymerization using PIP-Noria mixture as aqueous phase. The optimal PIP-Noria-TMC membrane reached 147.6 L m-2h-1MPa-1 of water permeability, which was almost twice that of the pristine NF membrane (i.e., PIP-TMC membrane). Meanwhile, the PIP-Noria-TMC membrane exhibited comparable Na2SO4 rejection (∼98%) to the PIP-TMC membrane and outstanding mono/divalent salt selectivity. Besides, static adsorption tests using E.coli and bovine serum albumin (BSA) as the model foulants revealed that the surface of PIP-Noria-TMC membranes with high hydrophilicity and electronegative charge could effectively resist foulant attachment, which was also exhibited in the dynamic BSA filtration tests. Therefore, this work provided a practicable pathway to simultaneously overcome the permeability-selectivity trade-off and membrane fouling problems for the NF process.

Introduction

Besides the essential role of water for social development and human health, more than 30% of the global population does not have access to clean water today, and there is a prediction that the proportion will reach 60% in 2025 [1]. Hitherto, 2.5 billion people are in need of adequate sanitation, and the water-related disease causes the death of a child every minute [2]. Therefore, desalination of brackish water or reuse of wastewater is an effective way to address the water scarcity issue. Due to its high efficiency, environmentally friendly, and low operation cost, membrane technology is widely regarded as a promising technology for augmenting freshwater supply [3]. Nanofiltration (NF) membranes are typically polyamide (PA) thin film composite (TFC) membranes fabricated by interfacial polymerization (IP) using piperazine (PIP) as aqueous phase and 1,3,5-benzenetricarbonyl trichloride (TMC) as organic phase. As a membrane technology between reverse osmosis (RO) and ultrafiltration (UF) in regard to pore size, NF membranes are capable of allowing water molecules and most of the monovalent ions to pass through, while rejecting multivalent ions and larger molecules [4]. Several exclusion forces including Donnan equilibrium, steric exclusion, and potentially dielectric exclusion exist at the interface between the NF membrane surface and the feed [[5], [6], [7], [8]]. It can be seen that the NF technology can separate small molecules more effectively compared to UF and is less expensive to produce high-quality drinking water than RO [9,10]. Therefore, NF has attracted significant attention towards the treatment of drinking water over the past decades.

As NF has the distinct advantages of sieving monovalent/divalent ions and small organic molecules with different molecular weight compared with UF and RO, extensive efforts are needed to further improve the selectivity of NF membranes. However, narrowing the pore size to enhance membrane selectivity is usually accompanied by a decline in water permeability. This “trade-off effect” between water permeability and selectivity is one of the pervasive and main obstacles that limit the further enhancement of NF membranes. Therefore, exploring NF membranes with both high water permeability and selectivity has become an important research topic to break the “trade-off effect”. On the one hand, the representative strategies for improving water permeability of membranes include making a thin selective layer, tailoring surface morphology to increase membrane effective area, improving membrane hydrophilicity, and reducing mass-transfer resistance [[11], [12], [13]]. On the other hand, membrane selectivity enhancement mainly involves in tuning pore size/pore size distribution and manipulating charge distribution [14]. Based on these knowledge, various membrane fabrication approaches have been successful for the enhancement of both water permeability and selectivity by tailoring desirable membrane properties. Particularly, the interlayer-thin film composite (i-TFC) membrane has been developed due to the formation of thinner PA layers with desired nanostructures, which significantly improves the water permeability and selectivity [15]. However, the fabrication process of the i-TFC membrane consists of constructing an interlayer on a support membrane by dip-coating polymeric materials or vacuum filtration with nanomaterials, and subsequently implementing IP. The extra interlayer coating process of i-TFC membranes results in the low reproducibility and capital cost problems for the industrial scaling-up [16]. Due to the simplicity and reliability, incorporating nanomaterials into the PA layer by one-step IP has become a promising route to get both ultra-permeable and highly selective TFC membranes, named as thin film nanocomposite (TFN) membrane. This concept proposed by Hoek et al. [17] has motivated many materials-oriented researches to explore the effect of various embedded nanomaterials such as carbon nanotube [[18], [19], [20]], graphene oxide [21], silica [22], silver [23], metal-organic frameworks (MOF) [24], zeolite nanoparticles [17,25], and polyhedral oligomeric silsesquioxane (POSS) [26] on the membrane performance. Several advantages of the TFN membrane contribute to overcoming the “trade-off effect”, including faster water transport within the porous nanomaterials, increased membrane affinity to water, and improved PA layer properties such as tunable charge density, pore structure, and thermal, chemical, and mechanical stability.

Another huge challenge of the NF membrane is the occurrence of membrane fouling. The organics and microorganisms in aqueous systems (e.g., wastewater, seawater et al.) may deposit and then aggregate on the membrane surface, which ultimately causes severe flux decline, increases operating pressure, and shortens the lifespan of NF membranes [27]. In general, membrane fouling is influenced by a nonspecific interaction between foulants and membrane surface properties. According to literatures, surface hydrophilicity as well as surface charge have major effect on membrane fouling. On the one hand, membrane surfaces with high hydrophilicity can prevent fouling effectively due to the formation of a hydration layer [[28], [29], [30]]. On the other hand, as most organics and microorganisms are negatively charged, membrane surfaces with neutral or negative charges are employed to repel the foulant attachment because of the electrostatic repulsion [31]. Therefore, both enhancing surface hydrophilicity and adjusting surface charge are effective strategies for improving the antifouling propensity of NF membranes.

Noria is a macrocyclic molecule, possessing 24 hydroxyl groups, 6 shallow cavities in the side, and a large central cavity. This well-defined pore structure of Noria could act as the water transport channel in the PA layer, meanwhile the plentiful hydroxyl groups could enhance membrane hydrophilicity and negative charge. Based on these advantages of Noria, tailoring a TFC membrane containing Noria might be effective for simultaneously overcoming the permeability-selectivity trade-off and the membrane fouling in NF process. So far, Noria has been applied to construct an interlayer for i-TFC fabrication [32] and amination Noria has been synthesized to serve as the aqueous phase monomer alone in the IP process for TFC membrane preparation [33]. But there is no study on doping Noria into PIP aqueous phase for TFN membrane fabrication. In this study, we synthesized Noria by a one-pot condensation reaction of resorcinol and 1,5-pentanedial, and then the TFN NF membrane embedded with Noria (hereafter, called as “PIP-Noria-TMC membrane”) was prepared by one-step IP via doping Noria into the PIP aqueous phase. The effect of Noria doping concentration on membrane characterizations and performances was systematically investigated. The physicochemical properties of as-prepared membranes were characterized by Attenuated Total Reflection-Fourier Transform Infrared Spectroscopy (ATR-FTIR), water contact angle, and ζ-potential. The membrane morphology was observed by scanning electron microscope (SEM) and atomic force microscope (AFM). For the membrane performance, the separation parameters of fabricated membranes including water permeability and salt rejection were tested in a crossflow system. The antifouling propensity of membranes was evaluated by static adsorption experiments as well as dynamic filtration tests.

Section snippets

Materials

Polysulfone (PSF) UF membranes were used as the support film for IP process which were provided by Vontron Co., Ltd. (Beijing, China). PIP and TMC, two reactive monomers for IP, were purchased in Tokyo Chemical Industry (Tokyo, Japan). Resorcinol (Shanghai Adamas Reagent Co., Ltd., Shanghai, China) and glutaraldehyde (50% in water, Shanghai Aladdin Bio-Chem Technology Co., Ltd., Shanghai, China) were used to synthesize the Noria. Escherichia coli (E.coli) and bovine serum albumin (BSA,

Membrane characterizations

In this study, Noria was synthesized through a simple condensation reaction of resorcinol and glutaraldehyde, and this molecule is known to have a large central cavity with multi-hydroxyl groups. The chemical composition of the synthesized Noria was confirmed by ATR-FTIR and 1H NMR as shown in Figs. S1(a) and S1(b). The solubility of Noria was demonstrated in Fig. S2. Precipitation appeared after 24 h when Noria was dissolved by water, which suggested that the Noria can be suspended in water

Conclusion

In this study, a PIP-Noria-TMC membrane integrating excellent separation performance and antifouling propensity was prepared by a one-step IP process using PIP-Noria mixture as the aqueous phase. Noria was successfully synthesized and soluble in the PIP aqueous solution. The incorporation content of Noria in the PA layer was controllable by adjusting the Noria doping concentration in the PIP-Noria aqueous phase. The optimal PIP-Noria-TMC membrane reached 147.6 L m-2h-1MPa-1 of water

Author contributions

Zhe Yang: Conceptualization, Methodology, Writing-Original draft, Funding acquisition.

Longting Li: Investigation, Formal analysis.

Chi Jiang: MD simulation operation.

Na Zhao: Investigation.

Shenghao Zhang: Investigation.

Yaoli Guo: Visualization.

Yi Chen: Investigation.

Shuangmei Xue: Visualization.

Chenhao Ji: Software, Data Curation.

Shuzhen Zhao: Resources.

Ralph Rolly Gonzales: Writing - Review & Editing.

Hideto Matsuyama: Writing - Review & Editing.

Jianzhong Xia: Project administration.

Q. Jason Niu:

Declaration of competing interest

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.

Acknowledgements

The authors would like to acknowledge the National Natural Science Foundation of China (NO. U2006230) and the China Postdoctoral Science Foundation (NO. 2021M692190) for the financial support.

References (61)

  • Q. Li et al.

    Enhancing nanofiltration performance by incorporating tannic acid modified metal-organic frameworks into thin-film nanocomposite membrane

    Environ. Res.

    (2020)
  • J. Duan et al.

    High-performance polyamide thin-film-nanocomposite reverse osmosis membranes containing hydrophobic zeolitic imidazolate framework-8

    J. Membr. Sci.

    (2015)
  • X. You et al.

    Enhancing the permeation flux and antifouling performance of polyamide nanofiltration membrane by incorporation of PEG-POSS nanoparticles

    J. Membr. Sci.

    (2017)
  • Z. Yang et al.

    Improved anti-biofouling performance of polyamide reverse osmosis membranes modified with a polyampholyte with effective carboxyl anion and quaternary ammonium cation ratio

    J. Membr. Sci.

    (2020)
  • Z. Yang et al.

    Zwitterionic polymer modification of polyamide reverse-osmosis membranes via surface amination and atom transfer radical polymerization for anti-biofouling

    J. Membr. Sci.

    (2018)
  • Z. Yang et al.

    Effect of polymer structure modified on RO membrane surfaces via surface-initiated ATRP on dynamic biofouling behavior

    J. Membr. Sci.

    (2019)
  • Z. Yang et al.

    Engineering a dual-functional sulfonated polyelectrolyte-silver nanoparticle complex on a polyamide reverse osmosis membrane for robust biofouling mitigation

    J. Membr. Sci.

    (2021)
  • L. Ren et al.

    Construction of high selectivity and antifouling nanofiltration membrane via incorporating macrocyclic molecules into active layer

    J. Membr. Sci.

    (2020)
  • A.K. Ghosh et al.

    Impacts of support membrane structure and chemistry on polyamide–polysulfone interfacial composite membranes

    J. Membr. Sci.

    (2009)
  • Y. Ren et al.

    High flux thin film nanocomposite membranes based on porous organic polymers for nanofiltration

    J. Membr. Sci.

    (2019)
  • M.B.M.Y. Ang et al.

    A facile and versatile strategy for fabricating thin-film nanocomposite membranes with polydopamine-piperazine nanoparticles generated in situ

    J. Membr. Sci.

    (2019)
  • Y.-L. Ji et al.

    Mussel-inspired zwitterionic dopamine nanoparticles as building blocks for constructing salt selective nanocomposite membranes

    J. Membr. Sci.

    (2019)
  • Z. Yao et al.

    Preparation of nanocavity-contained thin film composite nanofiltration membranes with enhanced permeability and divalent to monovalent ion selectivity

    Desalination

    (2018)
  • S. Xiong et al.

    Thin film composite membranes containing intrinsic CD cavities in the selective layer

    J. Membr. Sci.

    (2018)
  • Y. Zeng et al.

    An acid resistant nanofiltration membrane prepared from a precursor of poly (s-triazine-amine) by interfacial polymerization

    J. Membr. Sci.

    (2018)
  • J. Zhu et al.

    High-flux thin film composite membranes for nanofiltration mediated by a rapid co-deposition of polydopamine/piperazine

    J. Membr. Sci.

    (2018)
  • S. Yang et al.

    Electrosprayed polyamide nanofiltration membrane with intercalated structure for controllable structure manipulation and enhanced separation performance

    J. Membr. Sci.

    (2020)
  • X. Li et al.

    Design and development of layer-by-layer based low-pressure antifouling nanofiltration membrane used for water reclamation

    J. Membr. Sci.

    (2019)
  • L. Chen et al.

    High performance graphene oxide nanofiltration membrane prepared by electrospraying for wastewater purification

    Carbon

    (2018)
  • Y.-S. Guo et al.

    High-flux zwitterionic nanofiltration membrane constructed by in-situ introduction method for monovalent salt/antibiotics separation

    J. Membr. Sci.

    (2020)
  • Cited by (53)

    View all citing articles on Scopus
    View full text