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Nanoscale · 2020 ·Vol. 12 ·期 34 ·17812-17820 · IF 6.895

Superhydrophobic graphene-coated sponge with microcavities for high efficiency oil-in-water emulsion separation

Longxiang Han,Hengchang Bi,Xiao Xie,Shi Su,Peng Mao,Litao Sun

Materials for emulsion separation with low pressure, high flux and high stability are of great interest in the treatment of oily wastewater. Herein, we report a facile strategy for the fabrication of PDMS and graphene coated melamine sponge (PG-MS), which can efficiently separate oil-in-water emulsions. In PG-MS, melamine sponge (MS) provides a three-dimensional porous structure, graphene constructs hydrophobic microcavities, and PDMS enhances the hydrophobic property of the material, forming a superhydrophobic material. The PG-MS shows high flux (experimentally 10 000 L m−2 h−1, and the effective flux increases with the thickness of the filter layer), high separation efficiency (oil content of the filtered water ∼4.7 mg L−1 can be discharged directly, with oil separation efficiency >99%), low pressure (applied to overcome water's gravity), and high stability (no obvious change in 20 cycles). Our study indicates that PG-MS has a wide range of applications in oil-in-water emulsion separation in industry and environmental sciences.

CAS / MDL: 56-23-5 112-40-3
研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Robust translucent superhydrophobic PDMS/PMMA film by facile one-step spray for self-cleaning and efficient emulsion separation

Hui Liu,Jianying Huang,Zhong Chen,Guoqiang Chen,Ke-Qin Zhang,Salem S. Al-Deyab,Yuekun Lai

In this work, a translucent superhydrophobic coating was fabricated by a simple spray-coating technique using fluorine-free and easily available materials, viz , the hybrids of PDMS and PMMA in THF solution, without any pre-/post-treatment. The combination of the microscale roughness of the sprayed-PMMA, along with the low surface energy PDMS, has contributed to the observed superhydrophobicity. The as-prepared PDMS/PMMA@superhydrophobic surface has displayed a water contact angle of 157.5° and sliding angle of 2.8°. Furthermore, the liquids with various surface tension, ranging from water to various organic liquids, displayed nearly spherical shapes on the superhydrophobic substrate. In addition, this coating has also shown significant stability against sand abrasion and water droplet impact, and was able to maintain its superhydrophobicity after being soaked in strong acid and salkali solutions. Moreover, the superhydrophobic coating was found to be translucent with good visibility of the characters through the coated glass substrate. The transformation from a superhydrophobic state to superhydrophilic state can be realized via a hot-press process, and such a facile technique can be easily applied to potential applications in surface patterning. Additionally, the super-antiwetting surface has been demonstrated for applications in highly efficient oil-water emulsion separation, anti-fouling, and self-cleaning.

CAS / MDL: 109-99-9
研究领域: 材料科学 · 表面工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Multifunctional membranes with super-wetting interface and in-situ Fenton-like sites for efficient oil-in-water emulsion separation

Juan Zhai,Zihan Li,Hengyang Mao,Xiuyang Zou,Shouyong Zhou,Meisheng Li,Minghui Qiu,Yan Zhang,Shanshan Xia,Yijiang Zhao

The surge in oil-in-water (O/W) emulsions poses a threat to the ecological environment. Membrane separation technology can achieve complete O/W emulsion separation through size sieving; however, its efficiency is limited by membrane fouling. In this study, an efficient O/W separation membrane with passive and positive anti-fouling properties was fabricated using Fe 3 O 4 functionalized attapulgite (ATP) nanofibers. The anti-fouling mechanism of the multifunctional membranes for the separation of various O/W emulsions was studied. During separation process, a hydration layer, which mitigates oil adhesion with binding energy as low as −169 kcal·mol −1 , forms on the interface of Fe 3 O 4 -ATP. When a cationic surfactant is present, positively charged oil droplets are attracted to the membrane surface, where they compress against each other, leading to demulsification and escape. Synergistic effects including electrostatic shielding, interaction energy, and steric hindrance were demonstrated through characterization and simulation. Our findings showed that the membrane exhibited a high filtration efficiency with an oil rejection of over 99 % and a steady flux of over 73 % of its initial value. After filtration, oil fouling degraded into smaller sizes and escaped from the membrane structure through the Fenton-like catalytic function of Fe 3 O 4 , resulting in a flux recovery ratio of up to 90 %. This study provides a reference for the construction of multifunctional membranes for efficient separation processes and advancing anti-fouling research on membrane interfaces.

研究领域: 环境科学 · 材料科学
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Scientific Reports · 2017 ·Vol. 7 ·期 1 ·1-12 · IF 4.259

Flexible PVDF membranes with exceptional robust superwetting surface for continuous separation of oil/water emulsions

Xiong Zhu,Lin Haibo,Liu Fu,Xiao Peng,Wu Ziyang,Li Tiantian,Li Dehong

Instability of superwetting surface is the stumbling block of flexible polymeric membranes for continuous separation of water-in-oil or oil-in-water emulsions. Manipulation of rigid superwetting nano-TiO 2 on hierarchical poly(vinylidene fluoride) (PVDF) membrane by mimicking the plant roots holding soil behaviour enabled the generation of robust superwetting surface withstanding the harshly physical and chemical torture. The unique interface combination, which fabricated by a compacted nano-layer with the thickness of ~20 μm, was disclosed by systematic structure characterization. As demonstrated by SEM, LSCM and nano-CT, the pristine PVDF membrane with large quantities of cilia-like micro/nano-fibrils can function as the plant roots to capture, cage and confine the nanoparticles to form a robustly rigid nano-coating. The as-prepared membranes showed excellent durable separation performance both in varieties of stabilized water-in-oil and oil-in-water emulsion separation for a long term with few nanoparticles loss in a continuous crossflow mode. The strategy of assembling rigid inorganic nano-particles on flexible surface offers a window of opportunity for preparation of robust organic-inorganic hybrid membranes not only for continuous oil/water emulsion separation, but also for other functional application, such as electric conduction, heat conduction, ion exchange, and in membrane catalytic reactors etc.

研究领域: 材料科学 · 环境工程
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Self-Locked and Self-Cleaning Membranes for Efficient Removal of Insoluble and Soluble Organic Pollutants from Water

Kai Wang,Huaqiang He,Tian C. Zhang,Ying Liang,Shaojun Yuan

A feasible and efficient membrane for long-term treatment of complex oily wastewater is especially in demand, but its development still remains a challenge because of serious membrane fouling and incomplete/destructive reclamation methods. Herein, an interpenetrating TiO2 nanorod-decorated membrane with self-locked and self-cleaning properties is rationally fabricated via coaxial electrospinning and hydrothermal synthesis. The self-locked membrane shows full reinstatement of the original state and exhibits satisfactory mechanical strength, superhydrophilicity, underwater superoleophobicity, and robust solvent resistance, which endow the membrane with successful separation for 16 types of highly emulsified oil-in-water emulsions (e.g., surfactant-free; anionic, cationic, and nonionic surfactant-stabilized). Moreover, successful sequencing treatment of soluble organic emulsions using the separated “bait–hook–destroy” strategy indicates that the pristine membrane can be used to treat multipollutant wastewater with various limits. Most importantly, the fouled membrane can easily be reinstated by light irradiation without reduction of both mechanical strength and separation performance. As a proof of concept, the as-synthesized membrane shows an ultrahigh flux over 5000 L m–2 h–1 with a removal efficiency of >99.92%. The present development would provide a highly efficient strategy for the fabrication of an inorganic–organic revivable electrospinning membrane for various applications.

研究领域: 环境科学 · 材料科学
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY · 2020 · IF 1.701

Scalable and rapid preparation of Janus fabric by trans-printing method for efficient oil/water emulsion separation

Hai-Feng Liu,Zhu Wang,Cheng-Jun Sun

The old-fashioned yet effective trans-printing method was adopted to prepare Janus fabric in the study. Nonwoven cotton fabric was firstly immersed in tetrahydrofuran solution containing P(DMAEMA-co-TMSPMA), a polymer synthesized by copolymerization between N, N-dimethylaminoethyl methacrylate (DMAEMA) and 3-(trimethoxysilyl)propylmethacrylate (TMSPMA), followed by thermal treatment, thus endowing the fabric with the demulsification property. Next, one side of the above prepared fabric was overlapped and rolled with donor fabric containing PDMS-g-TMOS, a polymer synthesized by thiol/ene click reaction between multi-vinyl poly(dimethylsiloxane) (vinyl-PDMS) and 3-mercaptopropyltrimethoxysilane (MPTMOS). The PDMS-g-TMOS polymer infiltrated into the fabric cured with P(DMAEMA-co-TMSPMA) to a certain depth, followed by thermal treatment. Thus, the resultant fabric had both the superhyrophilic side for oil coalescence and the superhyrophobic side for oil permeation. The Janus fabric structure was confirmed by metalloscope, unidirectional water transport property (UDWT), scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). When the prepared fabric was used to separate model oil hexadecane (HD) from oil-in-water emulsion, the maximum separation speed was 134.5 kg h−1 m−2. The recovery rate of HD respectively reached 96.0% after 60 min and 99.9% after 150 min. The Janus fabric prepared by the trans-printing method is particularly suitable for industrial production and of great industrial value.

研究领域: 材料科学 · 环境工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Hierarchical architectures of Ag clusters deposited biomimetic membrane: Synthesis, emulsion separation, catalytic and antibacterial performance

Na Liu,Xiangyu Li,Jiakai Li,Yingze Cao,Lin Feng

The synthesis of high-performance materials for purifying oily wastewater, especially stable oil-in-water emulsions that aromatic pollutants present in water, is of growing scientific and technological significance. Novel hierarchical architectures of Ag clusters deposited biomimetic membrane have been synthesized by ingeniously selecting the mussel-inspired polydopamine coatings as an intermedium layer followed by a facile wet chemical reduction method. The target micro-scaled Ag clusters which are composed of innumerable nanoparticles, firmly load on the surface of sub-micrometer polydopamine spheres (PDSs) benefiting from the chelating capacity and benign reduction ability of PDSs. The resultant Ag@PDSs deposited membrane with enormous specific surface area exhibits superhydrophilicity and underwater superoleophobicity, making it highly promising for efficient separation of various surfactant-stabilized oil-in-water emulsions and synchronously excellent catalytic reduction of water-soluble aromatic dyes. Moreover, such a construction mode can effectively prevent the aggregation and possible leaching of Ag particles, which greatly contributes to the outstanding cyclic performance and good antibacterial activity. All these features demonstrate that the two-step strategy is a facile approach to design and exploit the deposited Ag@PDSs composites for diverse actual applications in oil/water emulsion separation, catalysis and antibacterial agent.

CAS / MDL: 1336-21-6
研究领域: 材料科学 · 环境科学 · 化学工程
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Science China-Technological Sciences · 2021 ·Vol. 64 ·期 10 ·2211-2219 · IF 3.572

Selective separation of oil-in-water emulsion with high efficiency by bio-inspired Janus membrane

Cai YaHui,Chen DongYun,Li NaJun,Xu QingFeng,Li Hua,He JingHui,Lu JianMei

The efficient and rapid separation of oil from stabilized oil-in-water emulsions with micro/nanometer size is a global challenge. Owing to the low oil content in oil-in-water emulsions, separating the oil by simply controlling the surface wettability is difficult. Controlling the pore size of the membrane surface to achieve separation will lead to a sharp decrease in flux. Herein, inspired by cell membrane transportation, a hydrophilic/hydrophobic bifunctional Janus membrane for stable oil-in-water separation was prepared by simple surface polymerization and vapor diffusion. The prepared Janus membrane contained a hydrophobic side and hydrophilic polyamine layer. When used for oil-in-water emulsion separation, the polyamine layer accumulated micro/nanometer oil droplets, forming an oil layer on the hydrophobic surface. Water was retained by the 1 H ,1 H ,2 H ,2 H -perfluorooctyl trichlorosilane layer, allowing oil droplets to selectively permeate through the membrane, achieving the separation effect. As the pore size of the modified fabric was basically unchanged, the permeation flux was fast (1.53×10 3 Lm −2 h −1 ). Furthermore, the poly( N,N -dimethylaminoethyl methacrylate) layer destroyed the emulsion stability, making the emulsion droplets aggregate without affecting the separation efficiency with fast permeation flux. Therefore, the prepared bifunctional Janus membrane shows great potential for actual wastewater treatment.

研究领域: 材料科学 · 环境工程
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2021 · IF 3.171

Fabrication of magnetically responsive anti-fouling and easy-cleaning nanofiber membrane and its application for efficient oil-water emulsion separation

Yajie Wang,Zhiwei Guo,Yujie Yang,Yanxiang Li,Qingchun Guo,Peilin Cui,Wangliang Li

The magnetically responsive anti-fouling nanofiber membrane (MRANM) was fabricated for efficient oil-water emulsion separation, which could be cleaned using oscillating magnetic field. MRANM was prepared by grafting superparamagnetic Fe 3 O 4 nanoparticles onto the surface of electrospun polyacrylonitrile nanofiber membrane (PANM). Compared with PANM, the water contact angle of MRANM decreased from 104° to 0°, indicating that the hydrophilicity of the membrane was significantly improved. For the emulsions of hexadecane, octane and rapeseed oil, the separation efficiency was 98.04%, 96.59% and 92.67%, respectively. After the treatments in oscillating magnetic field, the separation efficiency kept above 95% after 8 times recycling, which indicated that the MRANM had good regenerability and reusability. The as-fabricated membrane with magnetic responsiveness facilitated an effective method for solving the membrane fouling problem during practical applications of separation high viscosity oil-water emulsion.

研究领域: 材料科学 · 环境工程
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

High-flux whisker layer ceramic membrane prepared by gel spin-coating method for low-pressure oil/water emulsion filtration

Yuanhui Gao,Guogang Xu,Peng Zhao,Lulu Liu,Enliang Zhang,Shaowei Jin

Insufficient permeability and membrane fouling significantly influence the efficiency of ceramic microfiltration (MF) membranes in oil/water emulsion treatment. In this study, a high-flux whisker layer ceramic MF membrane with super-hydrophilicity was successfully fabricated through gel-spin coating method and a low-temperature oxidation method, which was used to separate oil/water emulsion. The effects of the whisker layer and surface wettability were systematically investigated, and the mechanism of in-situ gelling and pore size distribution was proposed. The super-hydrophilic ceramic MF membrane with an average pore size of 250 nm exhibited a high gas flux of 934 m 3 /(m 2 ·h·bar) and excellent pure water flux of 9754 L/(m 2  h bar). Even after a long-term circulating filtration process, the super-hydrophilic ceramic MF membrane still maintained a high water flux of over 50 L/(m 2 ·h) at a transmembrane pressure of 5 KPa during the treatment of oil-in-water emulsion with a concentration of 1000 mg/L. Overall, the developed ceramic MF membrane demonstrated high permeability and excellent anti-fouling performance, making it a promising candidate for oil/water emulsion wastewater treatment.

研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

In-situ electrostatic self-assembly superhydrophilic UiO-66-NH2@h-PPS membranes for highly efficient oil-water emulsion separation

Shiwei Tian,Yaqi Zhang,Qiankun Sha,Tian Yang,Yan Huang,Xingxiang Zhang,Wei Wang,Na Han

Highly efficient treatment of oil-water emulsions in severe environments (organic solvents, strong acids) is recognized as a challenging subject. Polyphenylene sulfide (PPS) is an ideal membrane material with superior thermal stability as well as chemical resistance that is expected to settle this challenge. However, the hydrophobicity of PPS (h-PPS) membrane inherently prevents its efficient treatment of oil-in-water (O/W) emulsions. In this study, superhydrophilic modification of PPS substrates was achieved by in situ electrostatic self-assembly of hydrophilic Zr-MOFs to obtain UiO-66-NH 2 @h-PPS membranes. The introduction of UiO-66-NH 2 crystals constructed the micro/nanoscale hierarchical structure for the substrate, which transforms the PPS substrate from a hydrophobic to a superhydrophilic state (water droplets require only 0.6 s to be completely immersed in the membrane). Meanwhile, the UiO-66-NH 2 @h-PPS membranes gain under-water superhydrophobicity (the under-water oil contact angle exceeds 150° for toluene, hexane , dichloromethane , and carbon tetrachloride , of which toluene reaches 163.1°), thereby improving wettability selectivity and decreasing oil adhesion, permitting the fabricated UiO-66-NH 2 @h-PPS membranes to effectively separate different types of O/W emulsions. The UiO-66-NH 2 @h-PPS membranes acquire excellent permeate fluxes (for the surfactant-free toluene-in-water emulsion, it reaches up to 7638.1 L m −2  h −1 ) and separation accuracy (99.1% oil rejection). Moreover, the UiO-66-NH 2 @h-PPS membrane exhibited outstanding harsh environment resistance. Interestingly, the combination of UiO-66-NH 2 and h-PPS substrate was applicable to degrade the organic compound in water, and the degradation efficiency of the methylene blue achieved 85.7% under visible light within 120 min. In summary, loading Zr-MOFs onto h-PPS substrates provides a novel strategy for the efficient treatment of wastewater under complex conditions with great potential for practical applications.

研究领域: 材料科学 · 环境工程
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LANGMUIR · 2023 · IF 3.9

Rapid Construction of Caffeic Acid/p-Phenylenediamine Antifouling Hydrophilic Coating on a PVDF Membrane for Emulsion Separation

Yujia Tong,Changing Miao,Wenlong Ding,Fiona Hammond Quarcoo,Xiao Xiao,Hongjun Ji,Weixing Li,Xiaohui Ju

The current methods of constructing modification strategies for hydrophilic membranes are time-consuming, complex in operation, and poor in universality, which limit their application on membranes. In this work, inspired by the adhesion properties and versatility of caffeic acid (CA) and p-phenylenediamine (PPDA), a simple, rapid, and universal method was designed for the separation of oil-in-water emulsion by preparing a stable hydrophilic coating separation membrane. The preparation time of the membrane was shortened to 40 min. The developed PVDF–PCA/PPDA membrane showed superhydrophilic and underwater superoleophobic properties. When applied to petroleum ether-in-water emulsion, isooctane-in-water emulsion, and dodecane-in-water emulsion separation, the oil rejection was more than 99.0%. In the circulating separation of 10 g/L soybean oil-in-water emulsion, the oil rejection was more than 99.3%, and the highest flux was 1036 L·m–2·h–1. The prepared PVDF–PCA/PPDA membrane performed well in the separation test of oily wastewater. The proposed strategy is simple and rapid; it may become a universal method for preparing membranes with super strong antifouling properties against viscous oil and accelerate the research progress of membrane separation of oil-in-water emulsions.

CAS / MDL: 9048-46-8 77-86-1
研究领域: 材料科学 · 环境工程 · 界面化学
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