Construction of highly water-stable metal-organic framework UiO-66 thin-film composite membrane for dyes and antibiotics separation
Graphical abstract
Introduction
Over the past few decades, emission of organic contaminants into the environment was seriously excessive owing to the accelerated urbanization and overgrew population [1], [2], [3]. Environmental remediation, especially water purification, attracted much attention in the whole world [4], [5]. Among many organic contaminants, synthetic dyes and antibiotics are the main pollutants, possessing intrinsic bio-toxicity and recalcitrance, that may lead to detrimental effect on the aquatic environment and human health [6], [7]. Compared to conventional liquid purification methods such as distillation, evaporation, adsorption, and ion exchange, membrane-based separation processes are known as promising and advanced technologies for water purification. This is due to their low energy consumption, convenient compact operation, and environmentally friendly [8], [9], [10]. Nanofiltration (NF), as the most attractive pressure-driven membrane separation technology, has been gained great concentration on organic contaminants separation [11], [12]. However, commercially available NF membranes are generally adopted polymers as the dominant materials, including polyimide (PI), polyamide (PA), poly(ethyleneimine) (PEI), and polydimethylsiloxane (PDMS) [13]. And these materials show some inevitable shortcomings, especially the barrier between high permeability and good selectivity, which limits NF membrane’s large-scale application [10], [13].
Therefore, tremendous efforts have been devoted to developing advanced membranes to improve the NF separation performance [14], [15], [16]. For example, Bai et al. integrated cellulose nanocrystals into the polyamide layer to achieve high rejection efficiency for divalent and monovalent ions [8]. Shao and his group fabricated composite membranes using interfacial polymerization technique, which exhibited over 90% retention ratios for safranin o and aniline blue [14]. Moreover, Chen and co-workers successfully constructed ultrathin polyamide membranes with additional passageways to recycle and remove organic solutes [11]. Based on these researches, thin-film composite (TFC) membrane comprised of an ultrathin selective layer is the most popular and energy efficient membrane in the field of NF [17], [18]. This is because that their selective layer and support layer can be independently designed and optimized to meet the requirements for target separation [17], [19]. Although water permeability and solute rejection of conventional TFC membrane have gradually improved, their low hydrophilicity, fouling-prone, as well as high cost hampered their large-scale applications [20]. Hence, the development of advanced TFC membrane with effective anti-fouling and high stability is highly desirable for direct treatment synthetic dyes and antibiotics in wastewater.
Metal-organic frameworks (MOFs), as a new generation porous crystalline material consisted of organic linkers and inorganic metal or clusters, have been driven intensive interest on environmental remediation, including adsorption [21], [22], degradation [23], catalysis [24], and membrane separation [25], [26], [27]. Since their intrinsic well-defined porous structure, distinct chemical versatility, and tailored functionality, MOFs are considered as an ideal candidate for advanced TFC membrane preparation [10], [13], [25], [27]. For instance, Liu et al. constructed ultrathin MOFs nanosheets as gutter layer in high efficiency, flexible thin-film composite membranes (TFCMs) for CO2 separation [28]. Zhang and co-workers prepared ultrathin reduced graphene oxide/MOF composite membrane for dye and heavy metal ions separation [29]. And precious metal recovery also realized through fibrous MOFs membranes synthesized by Liu’s group [30]. Among these MOFs, UiO-66 or its derivatives have been verified with superior performance serving as the molecular sieve for selective permeation [31], [32]. It stemmed from the fact that UiO-66 has tailored nanometer pore sizes that their aperture size (~6.0 Å) much bigger than water molecules (~2.8 Å), accelerating water transportation efficiency [33]. Besides, high pore volume, surface areas, and functional groups of UiO-66 increased defects and active sites during the synthetic process, promoting organic contaminants adsorption [34]. Last, the existence of the highest coordination between zirconium atom and carboxyl linkers, UiO-66 had superior hydrothermal and water-stable stability [35].
Herein, highly water-stable UiO-66 selective layer was vacuum-assisted filtrated on a polydopamine (PDA) modified graphene oxides (GO)-polyacrylonitrile (PAN) flexible porous support layer for dye and antibiotic separation. As mentioned in the previous researches [36], GO was a kind nanofiller to enhance polymeric substrate hydrophilicity due to abundant oxygen functional groups on their basal planes and edges. And the well-constructed lamellar structure of GO could achieve controllable pore channels and robust stability [37]. Meanwhile, PDA was used to further strengthen the combination and stability between polymeric support layer and UiO-66 selective layer. This is because that PDA can be easily deposited on many polymeric membranes owing to its strong adhesion ability [38], [39]. Under this configuration, water permeability and separation experiments of the UiO-66/PGP membrane were conducted. Both antifouling and stability performance of the prepared TFC membrane were evaluated. It was also attempted to explore the separation mechanism of the UiO-66/PGP membrane for dye and antibiotic.
Section snippets
Materials and chemicals
All reagents and chemicals were commercially available and used as received. Zirconium tetrachloride (ZrCl4), terephthalate (H2BDC), and anhydrous copper sulfate (CuSO4) were purchased from Shanghai Yien Chemical Reagent Co., Ltd. (China) Polyacrylonitrile (PAN, MW = 85000), polyethylene glycol (PEG, MW = 800), and dopamine hydrochloride (DA) were provided by Shanghai Macklin Biochemical Co., Ltd. (China) N, N-dimethylformamide (DMF), N-methylpyrrolidone (NMP), sodium dodecyl sulfate (SDS),
Characterization
All the characterizations were performed on partial materials (GO, PDA, and UiO-66), PAN substrate, GP substrate, PGP substrate, and the UiO-66/PGP TFC membrane.
Conclusions
In this study, highly water-stable UiO-66 selective layer was vacuum-assisted filtrated on mussel-inspired porous PGP support layer for dye and antibiotic separation. The FESEM, AFM, FTIR, XRD, XPS and CA results revealed that the incorporation of GO and PDA into the PAN substrate can effectively enhance the membrane surface compatibility and hydrophilicity. Notably, the thermal stability and wastewater treatment performance of the UiO-66/PGP TFC membrane were remarkably improved after UiO-66
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 are grateful for the financial supports from National Natural Science Foundation of China (51579095, 51579096, 51521006, 51378190 and 21675043), Hunan Province university innovation platform open fund project (14K020).
References (65)
- et al.
Cross-linking to prepare composite graphene oxide-framework membranes with high-flux for dyes and heavy metal ions removal
Chem. Eng. J.
(2017) - et al.
Fabrication of new composite membrane filled with UiO-66 nanoparticles and its application to nanofiltration
Sep. Purif. Technol.
(2017) - et al.
Enhanced permeability of rGO/S-GO layered membranes with tunable inter-structure for effective rejection of salts and dyes
Sep. Purif. Technol.
(2019) - et al.
Exploiting synergetic effects of graphene oxide and a silver-based metal-organic framework to enhance antifouling and anti-biofouling properties of thin-film nanocomposite membranes
ACS Appl. Mater. Interfaces
(2018) - et al.
Enhanced hydrophilicity and water flux of poly(ether sulfone) membranes in the presence of aluminum fumarate metal-organic framework nanoparticles: preparation and characterization
ACS Appl. Mater. Interfaces
(2019) - et al.
Mussel-inspired synthesis of polydopamine-functionalized graphene hydrogel as reusable adsorbents for water purification
ACS Appl. Mater. Interfaces
(2013) - et al.
Antifouling properties of Cu(tpa)@GO/PES composite membranes and selective dye rejection
J. Membr. Sci.
(2018) - et al.
Incorporation of cellulose nanocrystals (CNCs) into the polyamide layer of thin-film composite (TFC) nanofiltration membranes for enhanced separation performance and antifouling properties
Environ. Sci. Technol.
(2018) - et al.
High-flux thin film composite membranes for nanofiltration mediated by a rapid co-deposition of polydopamine/piperazine
J. Membr. Sci.
(2018) - et al.
Metal−organic framework composite membranes: synthesis and separation applications
Chem. Eng. Sci.
(2015)
Building additional passageways in polyamide membranes with hydrostable metal organic frameworks to recycle and remove organic solutes from various solvents
ACS Appl. Mater. Interfaces
Fabrication of a loose nanofiltration candidate from Polyacrylonitrile/Graphene oxide hybrid membrane via thermally induced phase separation
J. Hazard. Mater.
Metal–organic framework membranes: production, modification, and applications
Prog. Mater Sci.
Newly developed nanofiltration (NF) composite membranes by interfacial polymerization for Safranin O and Aniline blue removal
J. Membr. Sci.
Nano-ZnO embedded mixed matrix polyethersulfone (PES) membrane: influence of nanofiller shape on characterization and fouling resistance
Appl. Surf. Sci.
Composite ultrafiltration membrane tailored by MOF@GO with highly improved water purification performance
Chem. Eng. J.
Preparation and characterization of new PA-MOF/PPSU-GO membrane for the separation of KHI from water
Chem. Eng. J.
Graphene oxide-in-polymer nanofiltration membranes with enhanced permeability by interfacial polymerization
J. Membr. Sci.
Graphene oxide quantum dots incorporated into a thin film nanocomposite membrane with high flux and antifouling properties for low-pressure nanofiltration
ACS Appl. Mater. Interfaces
Thin film nanocomposite forward osmosis membrane embedded with amine-functionalized ordered mesoporous silica
Appl. Surf. Sci.
The application of different typological and structural MOFs-based materials for the dyes adsorption
Coord. Chem. Rev.
Mn-doped zirconium metal-organic framework as an effective adsorbent for removal of tetracycline and Cr(VI) from aqueous solution
Microporous Mesoporous Mater.
Insight into electro-Fenton and photo-Fenton for the degradation of antibiotics: mechanism study and research gaps
Chem. Eng. J.
Metal-organic framework supported palladium nanoparticles: applications and mechanisms
Part. Part. Syst. Char.
Metal-organic frameworks for separations
Chem. Rev.
Iron containing metal-organic frameworks: structure, synthesis, and applications in environmental remediation
ACS Appl. Mater. Interfaces
Metal-organic frameworks based membranes for liquid separation
Chem. Soc. Rev.
Ultrathin metal-organic framework nanosheets as a gutter layer for flexible composite gas separation membranes
ACS Nano
Ultrathin reduced graphene oxide/MOF nanofiltration membrane with improved purification performance at low pressure
Chemosphere
Super-stable, highly efficient, and recyclable fibrous metal-organic framework membranes for precious metal recovery from strong acidic solutions
Small
Highly water-stable zirconium metal-organic framework UiO-66 membranes supported on alumina hollow fibers for desalination
J. Am. Chem. Soc.
High flux thin film nanocomposite membranes based on metal-organic frameworks for organic solvent nanofiltration
J. Am. Chem. Soc.
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