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JOURNAL OF APPLIED POLYMER SCIENCE · 2022 ·Vol. 139 ·期 21 ·52205 · IF 3.057

Fabrication and characterization of transparent underwater superoleophobic coatings based chitin nanofibers and polyvinyl alcohol

Qian Wang,Peizhuang Wang,Lvheng Kou,Hongyuan Wei,Jiang Zhou

Transparent underwater superoleophobic coatings were prepared by blending chitin nanofibers (ChNFs) and polyvinyl alcohol (PVA) and then cross-linked with glutaraldehyde (GA). The interactions among ChNFs, PVA, and GA in the coatings were analyzed via FT-IR and XPS. Results of SEM observation and AFM analysis showed that higher concentrations of ChNFs and GA gave rise to rougher surface and lower transmittance of the coatings. By adjusting ratios of ChNFs, PVA, and GA, the coating surface could possess underwater superoleophobicity with oil (1, 2-dichloroethane) contact angle up to 159.2° and slide angle ~3°, meanwhile, transmittance of the coatings in the wavelength range of 400–800 nm could be maintained between 40% and 90%. This work provides a new route to prepare environmentally friendly transparent underwater superoleophobic coatings.

CAS / MDL: 1398-61-4 108-31-6
研究领域: 材料科学 · 表面化学
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ACS Applied Polymer Materials · 2022 · IF 4.855

Robust and Versatile Cellulose Aerogel with a Self-Wettable Surface for Efficient Dual Separations of Oil-in-Water and Water-in-Oil Emulsions

Yucong Yu,Xiaolong Shi,Lin Liu,Wenli Gong,Xiangdong Kong,Juming Yao

Separation materials with unique surface wettability have been regarded as promising candidates for oily sewage treatment. However, simple and facile fabrication of superwettable materials integrating robust and tunable surface features is still a challenge. Inspired by the unique molecular structure of cellulose with a rigid skeleton and abundant hydroxyl groups, this work proposed high-strength, superhydrophilic, and underwater superoleophobic cellulose aerogels prepared via facile chemical cross-linking without any surface modification. Benefiting from the superporous microstructure and unique surface wettability, the cellulose aerogels exhibited on-demand separation performances for oil-in-water (O/W), water-in-oil (W/O) emulsions, and crude oil. The superior separation flux of 19,602 L/(m2 h) and a rejection of 99.5% were acquired for O/W emulsion, while 5158 L/(m2 h) of flux and 98.9% of rejection were acquired for W/O emulsions. Importantly, the cellulose aerogels show an outstanding efficiency for crude oil/water emulsions with flux from 7815 to 26,648 L/(m2 h) based on water content. Moreover, owing to the rigid skeleton and cross-linked cellular architecture, the aerogels displayed significant flexibility and toughness with tiny deformation of 0.15% after 60 cycles underwater, endowing it with excellent reusability. Thereby, this proposed cellulose aerogel with unique advantages of a robust, superhydrophilic, and underwater superoleophobic surface exhibits a promising application in versatile and efficient dual oil/water separation.

研究领域: 材料科学 · 环境工程 · 化学工程
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Journal of Water Process Engineering · 2021 · IF 5.485

Underwater superoleophobic graphene oxide-connected cotton fibers membrane for antifouling oil/water separation

Shaolin Yang,Jinze Li,Na Yang,Simiao Sha,Cheng Yang,Jiayu Zhao,Aijian Duoerkun,Yu Hong,Caiqin Wu

Underwater superoleophobic membranes constructed by coating superhydrophilic materials on various porous substrates have been widely used for oil/water separation. However, most of these membranes suffer from high-cost, non-green and complex fabrication process. Herein, a novel graphene oxide-connected cotton fibers (GOCCF) membrane was fabricated by simply soaking cotton in graphene oxide (GO) aqueous-alcoholic suspension followed by air-drying. The synergistic effect of the rough surface and the hydrophilic polar groups on the GO nanosheets endows the GOCCF membrane with superhydrophilicity and underwater superoleophobicity. The GOCCF membrane can be applied to oil/water separation, and exhibits high separation efficiency for separating water from various oils driven by gravity. The GOCCF membrane also shows remarkable antifouling behavior and recyclability with maintaining a high separation efficiency over 99.8% and an ultra-high flux about 95,000 L m −2  h −1 in the whole separation processes repeated for 30 cycles. These results suggest that the GOCCF membrane could be a potential material for practical oil/water separation.

研究领域: 材料科学 · 环境科学
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Polymers · 2023 ·Vol. 15 ·期 14 ·3042 · IF 5

Preparation of Superhydrophilic/Underwater Superoleophobic and Superhydrophobic Stainless Steel Meshes Used for Oil/Water Separation

Yu-Ping Zhang,Ya-Ning Wang,Hong-Li Du,Ling-Bo Qv,Jun Chen

Robust membrane materials with high efficiency have attracted extensive attention in oil/water separation. In this work, carbon particles via candle combustion were firstly adsorbed on the surface of stainless steel meshes (SSMs), which formed a thin hydrophobic coating, and a rough structure was then constructed through chemical vapor deposition and high temperature calcination, with the resultant SSM surface wrapped with uniform silica coating possessing the characteristic of superoleophobicity underwater. Scanning electron microscope (SEM), energy dispersive spectroscopy (EDS), and X-ray powder diffraction (XRD) were used to characterize the modified SSMs. The prepared SSMs were superhydrophilic in air, and they had superoleophobicity underwater (157.4°). The separation efficiency of five oil/water mixtures was above 98.8%, and the separation flux was 46,300 L·m−2·h−1. After it was immersed in 1 mol/L NaOH, 1 mol/L HCl and 3.5 wt% NaCl for 24 h, respectively, the efficiency was still above 97.3%. Further immersion in the solution of dopamine and octadecylamine resulted in the transformation of superhydrophililc/superoleophobicity-underwater SSMs to superhydrophobic SSMs, and the resultant SSMs with reverse surface wettability was also used for the oil/water separation with good separation efficiency and separation flux.Keywords:stainless steel mesh;underwater superoleophobicity;chemical vapor deposition;superhydrophobicity;oil/water separation

研究领域: 材料科学 · 表面工程 · 环境科学
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Preparation of superhydrophilic-underwater superoleophobic silica nanorods modified fiber membrane for efficient oil-in-water emulsion separation

Feiyang Yan,Liangcheng Tong,Hang Qin,Wenming Guo,Jingxiong Liu,Wen Xie,Pengzhao Gao,Hanning Xiao

Silica nanorods modified fiber membranes were successfully fabricated for the separation of emulsions by filtration deposition method. Compared to the unmodified membranes, the arithmetic mean and root mean square of the membranes were 5.69 μm and 9.71 μm, with an improvement of 39.8% and 46.0%, respectively. Roughness increases improved hydrophilicity and underwater oleophobicity of the membrane. The instantaneous water contact angle (WCA) and underwater oil contact angle (UOCA) reached 0° and 151.92°, showing excellent superhydrophilic and underwater superoleophobic properties. The structural stability of the membranes was demonstrated by testing the mass and microstructural changes after continuous ultrasonic treatment, where the mass loss was only 5.42% and no significant changes in the microstructure were observed. Moreover, following immersion treatment with acid, alkali, and saline solutions, the maximum loss of membrane mass was only 1.20% and it remained underwater oleophobic, displaying excellent chemical stability. The separation efficiency of the silica nanorods modified fiber membrane for oil-in-water emulsions was as high as 96%, and the separation flux was above 1900 L m −2  h −1 ·bar −1 . The separation efficiency of the membranes was consistently maintained above 96% for 5 cycles.

CAS / MDL: 64-17-5 7647-14-5
研究领域: 材料科学 · 环境工程
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Sugarcane-based superhydrophilic and underwater superoleophobic membrane for efficient oil-in-water emulsions separation

Yanhua Liu,Tianbin Bai,Shixing Zhao,Zhuanli Zhang,Meijun Feng,Jianbin Zhang,Dianming Li,Libang Feng

The development of ecological, low cost, easy preparation, especially high performance materials for emulsions separation is of great importance due to the rise in pollution of oil-water emulsions from industrial production and domestic waste. Straws as agricultural wastes, including plenty of hydrophilic groups and multi-level pore structures, can be prepared as biomass membranes for oil-water emulsion separation. Herein, a novel super-hydrophilic sugarcane-based (SHS) membrane was prepared using a facile and eco-friendly method including chemical treatment and freeze-drying. The as-prepared SHS membrane has unique wettabilities due to the hydrophilic property of the internal cellulose and the micro-nano pores, including superhydrophilicity (water contact angle of 0°) and underwater superoleophobicity (underwater oil contact angles of over 150°). The SHS membrane has good durability and stability against ultraviolet (UV) irradiation, corrosion by acids and alkalis, mechanical abrasion and especially mould adhesion. Importantly, the SHS membrane can be used for separation of various oil-in-water emulsions, and exhibits excellent separation performances such as high separation efficiency (> 99 %) and good separation flux (above 891 L m −2 h −1 bar −1 ). The SHS membrane also exhibits excellent recyclability over 10 continuous separation cycles. Furthermore, the SHS membrane can be utilized to selectively absorb water from oils as a water absorbent material. Hence, SHS membrane is a promising and practical material for applications in treatment of wastewater containing oil-water emulsions.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Bi-functional super-hydrophilic/underwater super-oleophobic 2D lamellar Ti3C2Tx MXene/poly (arylene ether nitrile) fibrous composite membrane for the fast purification of emulsified oil and photodegradation of hazardous organics

Qingying Feng,Yingqing Zhan,Wei Yang,Ao Sun,Hongyu Dong,Yu-Hsuan Chiao,Yucheng Liu,Ximin Chen,Yiwen Chen

Developing the multi-functional membranes including oil/water emulsion separation and removal of hazardous organic pollutants is essential to the purification of the complicated wastewater. However, it remains a daunting challenge to combine these intended functions while maintaining high separation efficiency. Herein, we developed a new 2D lamellar MXene/poly (arylene ether nitrile) (PEN) fibrous composite membrane through the self-assembly of TiO 2 nanoparticles intercalated MXene nanosheets onto the porous PEN nanofibrous mats and bioinspired polydopamine triggered chemical-crosslinking with polyethyleneimine (PEI). Such nano-intercalation and mussel-inspired crosslinking could effectively regulate the interlayer spacing of the MXene nanosheet skin layer and surface wettability of the composite membrane, which also further contributed to the fast separation and unique bifunctional feature. It was found that the MXene@TiO 2 /PEN fibrous composite membrane exhibited low oil-adhesion and superhydrophilic (WCA = 0°)/underwater superoleophobic (UOCA > 155°) properties, which could efficiently separate various surfactant-stabilized oil-in-water emulsions under low pressure of 0.04 MPa while keeping good stability (Under 1 M HCl and 2 M NaOH solutions) and recyclability. Interestingly, the fibrous composite membrane achieved favorable permeation flux of 908–1003 Lm −2 h −1 (2270–2507.5 Lm −2 h −1 bar −1 ) in comparison to other reported MXene based multifunctional composite membranes. Moreover, owing to the synergistic effect of MXene nanosheets and TiO 2 nanoparticles, the MXene@TiO 2 /PEN membrane showed excellent photocatalytic degradation performance for various dyes under visible light, i.e. the photocatalytic degradation efficiency for 15 ppm MB, MO, CV, and MeB solutions achieved 92.31%, 93.50%, 98.06%, and 99.30% within 60 min, respectively. Such 2D MXene bio-functional composite membranes with outstanding oil/water emulsions separation and photocatalytic degradation of dyes pave an avenue for treating complicated oily wastewater.

研究领域: 材料科学 · 环境科学 · 纳米技术
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NEW JOURNAL OF CHEMISTRY · 2024 · IF 2.7

Simple temperature-regulated polymerization for the fabrication of a tea polyphenols-modified PVDF membrane for emulsion separation

Atian Xie,Lei Lu,Can Wei,Jirong Luo,Tong Tian,Feiyan Wang,Quan Li,Jiaheng Pu,Jiuyun Cui,Chengcai Li

Surface modification of membranes through facile coating methods is a promising way to improve their pollution resistance and separation performance. Herein, a tea polyphenol (TP)-coated PVDF membrane (PVDF-TP) was prepared via a simple temperature-regulated oxidative polymerization. The obtained membrane exhibited a water contact angle of 0° and underwater oil contact angle of 168.2°. This superhydrophilic/underwater superoleophobic membrane showed good separation capabilities with fluxes of 88.3–169.9 L m−2 h−1 and separation efficiencies of over 98.7% for various oil-in-water emulsions under a gravity-driven process. The PVDF-TP membrane exhibited excellent stability and was capable of withstanding ultrasonic waves, bending, and agitation. Even after recycling for more than 15 times, the separation efficiency of the membrane was still above 98.7% and the flux decreased by approximately 37%, demonstrating a good antifouling performance. Considering the characteristics of its simple preparation, good antifouling performance, high separation efficiency, and good stability, the PVDF-TP membrane has broad application prospects in the field of oil–water separation.

研究领域: 材料科学 · 环境工程
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MATERIALS CHEMISTRY AND PHYSICS · 2024 · IF 4.3

Synthesis of ZrO2/CeO2 composite coating with self-cleaning property for oil-water separation

Yao Wang,Ziyan Shen,Liang Zhang,Bing Xu,Kangkang Wang,Zhixian He,Shengnan Zhang

In the context of the escalating global water scarcity issue and the growing awareness of environmental protection, the purification and decontamination of wastewater from different sources have become of utmost necessity. This study was dedicated to fabricating a material capable of effectively mitigating membrane contamination for oil-water separation applications. A superhydrophilic/underwater superoleophobicitic cerium oxide/zirconia composite coating (CeO 2 /ZrO 2 ) was synthesized on a stainless-steel substrate by the sol-gel method. The distinctive rough network structure of the coating enables a water contact angle of 0° and an underwater oil contact angle as high as 169°. The coating not only effectively segregates various oil-water mixtures but also transcends the service life limitations associated with traditional ceramic membranes. Upon 80 min of visible light irradiation, the contact angle of this coating diminishes from 58° to 15°, signifying its self-cleaning ability. It can be considered that this durable and easily repairable coating has a promising application prospect in the field of oil-water separation.

CAS / MDL: 13520-92-8
研究领域: 材料科学 · 环境科学 · 表面化学
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SURFACE & COATINGS TECHNOLOGY · 2020 · IF 3.784

Facile surface coating of metal-tannin complex onto PVDF membrane with underwater Superoleophobicity for oil-water emulsion separation

Jie Yang,Lulu Wang,Atian Xie,Xiaohui Dai,Yongsheng Yan,Jiangdong Dai

In this study, inspired by self-cleaning property of fish scale in water, a novel superhydrophilic and underwater superoleophobic tannin-metal complex@polyvinylidene fluoride (TA-Fe@PVDF) nanocomposite membrane was prepared by a facile and one-pot surface coating technology at room temperature using the ferric nitrate and tannic acid as the building blocks. The as-fabricated TA-Fe@PVDF nanocomposite membrane was characterized by scanning electron microscopy (SEM), attenuated total reflection fourier transform infrared spectroscopy (ATR-IR), atomic force microscope (AFM) and contact angle measuring instrument. It was found that the TA-Fe complexes improved the surface wetting, separation efficiency and repeatability. The optimal TA-Fe@PVDF-1 composite membrane was obtained at the concentration ratio of TA and Fe 3+ of 1:3, which show underwater oil contact angle of 155°, and low oil adhesion. The separation efficiencies of TA-Fe@PVDF-1 composite membrane for various oil-water mixtures and oil-in-water emulsions are higher than 99.5%. The membrane flux can reach 2551 L m −2  h −1  bar −1 for surfactant-stabilized petroleum ether-in-water emulsion separation, and 4505 L m −2  h −1  bar −1 for petroleum ether/water mixture. This nanocomposite membrane exhibits excellent repeatability and good chemical stability (salt/acid/alkali resistance), to be potentially applied for the treatment of oily wastewater.

CAS / MDL: 9005-65-6 28983-56-4
研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Ultra-robust superwetting hierarchical membranes constructed by coordination complex networks for oily water treatment

Yuanyuan Zhao,Yanqiu Zhang,Feiran Li,Yongping Bai,Yunlu Pan,Jun Ma,Sui Zhang,Lu Shao

Superhydrophilic and underwater superoleophobic (SHL&UWSOB) membranes possess unique advantages in treating oily wastewater. The hydrophilic surface coating and the hierarchical microstructure is significant for the fabrication of SHL&UWSOB membrane, however, the stability of the surface coating remain challenging. In this study, the hydrophilic hierarchical structure was first constructed based on amino-functionalized polyhedral oligosiloxane/proanthocyanidins (POSS-NH 2 /PC) surface coating. Then metal-phenol networks (MPN) was quickly derived from Fe (Ⅲ) and PC networks (FPN). The coordination complex networks formed by POSS-NH 2 /PC cross-linking and FPN synergy construct a hydrophilic hierarchical hybrid layer on poly (vinylidene fluoride) (PVDF) microfiltration (MF) membrane surface. Physicochemical characterizations demonstrate that FPN can greatly restrain the oxidation of phenolic hydroxyl group and reduce the electrostatic repulsion force and enhance the interaction between chain segments, hence, the stability of the coating in strong acidic or alkaline conditions was achieved. The synthesized membrane shows robust superhydrophilicity and underwater superoleophobicity, revealing high efficiency for separation of oil-in-water emulsion in harsh environment, and the oil rejections are over 99.0%. In addition, the resulted membrane has good anti-oil fouling performance even after three-cycles of oil/water separation. The designed membrane lights new prospects in the design of the facile and universality for other superwetting materials.

研究领域: 材料科学 · 环境工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Engineering a superwetting membrane with spider-web structured carboxymethyl cellulose gel layer for efficient oil-water separation based on biomimetic concept

Jing Yang,Ligang Lin,Qi Wang,Wensong Ma,Xinyang Li,Zitian Liu,Xu Yang,Meina Xu,Qi Cheng,Kongyin Zhao,Junqiang Zhao

Superhydrophilic and underwater superoleophobic membranes have recently attracted significant interest as materials for effective oil-water emulsion separation. In this work, a superwetting membrane with a spider web structured gel layer was designed for efficient oil-water separation. Biomaterial, carboxymethyl cellulose (CMC), was used as the raw material, a spider web structured gel layer was constructed on the PVDF membrane surface by heat-treatment and chemical cross-linking. The hydrophilic gel layer imparted excellent superhydrophilic and underwater superoleophobic properties to the membrane, while the special spider web structure improved the membrane mechanical stability. The fabricated membrane exhibited superhydrophilicity and underwater superoleophobicity. Among different CMC concentration-modified membranes, the M-0.5 membrane containing 0.5 wt% CMC exhibited a flux of 612 L·m −2  h −1 during dichloromethane oil-water emulsion separation, which was 4.2-fold higher than that of the pristine PVDF membrane, while the membrane showed efficient oil-water separation capacity. Additionally, the water flux recovery reached as high as 93.3 %, and oil rejection attained 99.1 %. Meanwhile, the spiderweb-structured gel layer on the membrane surface displayed good mechanical stability. In summary, this novel membrane-modification method, inspired by the spider web structure, was simple, cost effective and environmentally friendly, thereby making it promising for future preparation of highly efficient oil-water emulsion separation membranes.

CAS / MDL: 9004-32-4
研究领域: 材料科学 · 环境工程
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