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MILP synthesis of separation processes for waste oil-in-water emulsions treatment

Zorka N. Pintarič,Gorazd P. Škof,Zdravko Kravanja

《化学科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 120-130 doi: 10.1007/s11705-016-1559-1

摘要： This paper presents a novel synthesis method for designing integrated processes for oil-in-water (O/W) emulsions treatment. General superstructure involving alternative separation technologies is developed and modelled as a mixed integer linear programming (MILP) model for maximum annual profit. Separation processes in the superstructure are divided into three main sections of which the pretreatment and final treatment are limited to the selection of one alternative (or bypass) only, while within the intermediate section various combinations of different technologies in series can be selected. Integrated processes composed of selected separation techniques for given ranges of input chemical oxygen demand (COD) can be proposed by applying parametric analyses within the superstructure approach. This approach has been applied to an existing industrial case study for deriving optimal combinations of technologies for treating diverse oil-in-water emulsions within the range of input COD values between 1000 mg?L and 145000 mg?L . The optimal solution represents a flexible and profitable process for reducing the COD values below maximal allowable limits for discharging effluent into surface water.

关键词： oil-in-water emulsion     chemical oxygen demand     superstructure     process synthesis     MILP    

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

Shanshan Zhao, Zhu Tao, Liwei Chen, Muqiao Han, Bin Zhao, Xuelin Tian, Liang Wang, Fangang Meng

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1355-5

摘要： Abstract • 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. 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 underwater superoleophobic 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.

关键词： Antifouling     Catechol/chitosan co-deposition     Oil-in-water emulsions separation     Underwater superoleophobic    

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Biodegradable, superhydrophobic walnut wood membrane for the separation of oil/water mixtures

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1377-1386 doi: 10.1007/s11705-022-2157-z

摘要： The preparation of environmentally friendly oil/water separation materials remains a great challenge. Freeze-drying of wood after lignin removal yields wood aerogels, which can be used as substrates to prepare fluorine-free environmentally friendly superhydrophobic materials, However, they are more suitable for absorption rather than filtration applications due to their poor strength. A study using cross-sections of pristine wood chips as substrates retains the original strength of wood, but the use of the cross-sectional of wood pieces limits their thickness, strength, and size. In this paper, a degradable fluorine-free superhydrophobic film (max. water contact angle of approximately 164.2°) with self-cleaning and abrasion resistance characteristics was prepared by a one-step method using pristine and activated walnut longitudinal section films as the substrate, with tetraethyl orthosilicate as a precursor and dodecyltriethoxysilane as a modifier. The tensile strength results show that superhydrophobic films with pristine or activated wood substrates maintained the strength of pristine wood and were 2.2 times stronger than the wood aerogel substrate. In addition, after cross-laminating the two samples, the films had the ability to separate oil and water by continuous filtration with high efficiency (98.5%) and flux (approximately 1.3 × 103 L∙m‒2∙h‒1). The method has potential for the large-scale fabrication of degradable superhydrophobic filtration separation membranes.

关键词： wood nanotechnology     superhydrophobic     biodegradable     surface modification     oil/water separation    

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Highly hydrophobic oil−water separation membrane: reutilization of waste reverse osmosis membrane

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1606-1615 doi: 10.1007/s11705-022-2200-0

摘要： The increasing applications of seawater desalination technology have led to the wide usage of polyamide reverse osmosis membranes, resulting in a large number of wasted reverse osmosis membranes. In this work, the base nonwoven layer of the wasted reverse osmosis membrane was successfully modified into the hydrophobic membrane via surface deposition strategy including TiO2 and 1H,1H,2H,2H-perfluorooctyltrichlorosilane (PFOTS), respectively. Various techniques were applied to characterize the obtained membranes, which were then used to separate the oil–water system. The optimally modified membrane displayed good hydrophobicity with a contact angle of 135.2° ± 0.3°, and its oil–water separation performance was as high as 97.8%. After 20 recycle tests, the oil–water separation performance remained more than 96%, which was attributed to the film adhesion of the anchored TiO2 and PFOTS layer on the surface. This work might provide a new avenue for recycling the wasted reverse osmosis membrane used in oily wastewater purification.

关键词： oil–water separation     wasted reverse osmosis membrane     hydrophobic modification    

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Fabrication of a superhydrophilic/underwater superoleophobic stainless steel mesh for oil/water separation

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 46-55 doi: 10.1007/s11705-022-2170-2

摘要： Because of the increasing amount of oily wastewater produced each day, it is important to develop superhydrophilic/underwater superoleophobic oil/water separation membranes with ultrahigh flux and high separation efficiency. In this paper, a superhydrophilic/underwater superoleophobic N-isopropylacrylamide-coated stainless steel mesh was prepared through a simple and convenient graft polymerization approach. The obtained mesh was able to separate oil/water mixtures only by gravity. In addition, the mesh showed high-efficiency separation ability (99.2%) and ultrahigh flux (235239 L∙m–2∙h–1). Importantly, due to the complex cross-linked bilayer structure, the prepared mesh exhibited good recycling performance and chemical stability in highly saline, alkaline and acidic environments.

关键词： oil/water separation     N-isopropylacrylamide     stainless steel mesh     ultrahigh flux    

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Functional flax fiber with UV-induced switchable wettability for multipurpose oil-water separation

《环境科学与工程前沿（英文）》 2022年 第16卷 第12期 doi: 10.1007/s11783-022-1588-6

摘要：

● A PAA-ZnO-HDTMS flax fiber with UV-induced switchable wettability was developed.

关键词： Flax fiber     Switchable wettability     ZnO-HDTMS coating     Oil-water separation    

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properties of a silver particle-coated and 1-dodecanethiol-modified superhydrophobic melamine sponge for oil/water separation

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1237-1246 doi: 10.1007/s11705-022-2140-8

摘要： A Ag particle-coated and 1-dodecanethiol-modified melamine sponge (Ag-DDT-MS) was prepared through surface roughness by coating silver particles and subsequent grafting of a hydrophobic long hydrocarbon chain. Superhydrophobic and 3D porous Ag-DDT-MS was characterized by Fourier transform infrared spectroscopy, scanning electron microscope, energy-dispersive X-ray spectroscopy, and X-ray diffraction. The water contact angle of Ag-DDT-MS reached 159.2°. Ag-DDT-MS exhibited excellent absorption capacity for high viscous oils and organic solvents, ranging from 42.8 to 105.2 g∙g−1. The absorbed oils can be easily collected by the mechanical pressing process, and the oil recovery rate was satisfactory, more than 90% after 20 recycles. Ag-DDT-MS material also demonstrated good stability and excellent compression-recovery ability, keeping 88.6% of the initial height after ten compression-release cycles.

关键词： melamine sponge     oil-absorbing material     hydrophobic     oil-water separation     oil absorption capacity    

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construction of pseudo-Janus silica/surfactant assembly and their application to stabilize Pickering emulsionsand enhance oil recovery

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1101-1113 doi: 10.1007/s11705-021-2095-1

摘要： Nanoparticles with high surface energy and chemical activity have drawn substantial attention in petroleum industry. Recently, Janus nanoparticles exhibited tremendous potential in enhanced oil recovery (EOR) due to their asymmetric structures and properties. In this study, a series of amphiphilic pseudo-Janus@OTAB (PJ@C18) nanoparticles with different concentrations of stearyltrimethylammoium bromide (OTAB) were successfully fabricated. The structures and properties of PJ@C18 were characterized by Fourier transform infrared spectroscopy and ζ-potential measurements. Based on the emulsification experimental results, the interaction models and the self-assembly behavior between hydrophilic nanoparticles (SiO2@NH2) and OTAB molecules at the oil/water interface were proposed, which was further confirmed via the measurements of the contact angle and dynamic interfacial tension. Interestingly, it was found that the change of pH value from 7.5 to 4.0 caused the type reversal of the PJ@C18-1000 stabilized Pickering emulsions. Furthermore, the PJ@C18-1000 stabilized Pickering emulsion system with excellent salt and temperature tolerances (10000 mg∙L–1, 90 °C) significantly improved the oil recovery in the single-tube (more than 17%) and double-tube (more than 25%) sand pack model flooding tests. The findings of this study could help to better understand the construction mechanism of pseudo-Janus silica/surfactant assembly and the potential application of PJ@C18-1000 stabilized Pickering emulsions for EOR.

关键词： Janus nanoparticles     surfactant     double phase inversion     self-assembly     enhanced oil recovery    

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Optimising the oil phases of aluminium hydrogel-stabilised emulsions for stable, safe and efficient vaccine

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 973-984 doi: 10.1007/s11705-021-2123-1

摘要： To increase antibody secretion and dose sparing, squalene-in-water aluminium hydrogel (alum)-stabilised emulsions (ASEs) have been developed, which offer increased surface areas and cellular interactions for higher antigen loading and enhanced immune responses. Nevertheless, the squalene (oil) in previous attempts suffered from limited oxidation resistance, thus, safety and stability were compromised. From a clinical translational perspective, it is imperative to screen the optimal oils for enhanced emulsion adjuvants. Here, because of the varying oleic to linoleic acid ratio, soybean oil, peanut oil, and olive oil were utilised as oil phases in the preparation of aluminium hydrogel-stabilised squalene-in-water emulsions, which were then screened for their stability and immunogenicity. Additionally, the underlying mechanisms of oil phases and emulsion stability were unravelled, which showed that a higher oleic to linoleic acid ratio increased anti-oxidative capabilities but reduced the long-term storage stability owing to the relatively low zeta potential of the prepared droplets. As a result, compared with squalene-in-water ASEs, soybean-in-water ASEs exhibited comparable immune responses and enhanced stability. By optimising the oil phase of the emulsion adjuvants, this work may offer an alternative strategy for safe, stable, and effective emulsion adjuvants.

关键词： pickering emulsion     vaccine adjuvant     alum-stabilised emulsion     oleic to linoleic acid ratio     stability    

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Easily-manufactured paper-based materials with high porosity for adsorption/separation applications in

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 830-839 doi: 10.1007/s11705-022-2267-7

摘要： A multi-functional porous paper-based material was prepared from grass pulp by simple pore-forming and green cross-linking method. As a pore-forming agent, calcium citrate increased the porosity of the paper-based material from 30% to 69% while retaining the mechanical strength. The covalent cross-linking of citric acid between cellulose fibers improved both the wet strength and adsorption capacity. In addition, owing to the introduction of high-content carboxyl groups as well as the construction of hierarchical micro-nano structure, the underwater oil contact angle was up to 165°. The separation efficiency of the emulsified oil was 99.3%, and the water flux was up to 2020 L·m–2·h–1. The theoretical maximum adsorption capacities of cadmium ion, lead ion and methylene blue reached 136, 229 and 128.9 mg·g–1, respectively. The continuous purification of complex wastewater can be achieved by using paper-based materials combined with filtration technology. This work provides a simple, low cost and environmental approach for the treatment of complex wastewater containing insoluble oil, organic dyes, and heavy metal ions.

关键词： adsorption     oil–water separation     underwater superoleophobicity     wastewater treatment    

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A novel composite coating mesh film for oil-water separation

Futao QIN, Zhijia YU, Xinhui FANG, Xinghua LIU, Xiangyu SUN

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 112-118 doi: 10.1007/s11705-009-0149-x

摘要： Polytetrafluoroethylene-polyphenylene sulfide composite coating mesh film was successfully prepared by a simple layered transitional spray-plasticizing method on a stainless steel mesh. It shows super-hydrophobic and super-oleophilic properties. The contact angle of this mesh film is 156.3° for water, and close to 0° for diesel oil and kerosene. The contact angle hysteresis of water on the mesh film is 4.3°. The adhesive force between the film and substrate is grade 0, the flexibility is 1 mm and the pencil hardness is 4H. An oil-water separation test was carried out for oil-contaminated water in a six-stage super-hydrophobic film separator. The oil removal rate can reach about 99%.

关键词： super-hydrophobic     super-oleophilic     composite coating     mesh film     separation of oil and water    

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Superhydrophobic, mechanically flexible and recyclable reduced graphene oxide wrapped sponge for highly efficient oil/water separation

Lijuan Qiu, Ruiyang Zhang, Ying Zhang, Chengjin Li, Qian Zhang, Ying Zhou

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 390-399 doi: 10.1007/s11705-018-1751-6

摘要：

Water pollution has become an urgent issue for our modern society, and it is highly desirable to rapidly deal with the water pollution without secondary pollution. In this paper, we have prepared a reduced graphene oxide (RGO) wrapped sponge with superhydrophobicity and mechanically flexibility via a facile low-temperature thermal treatment method under a reducing atmosphere. The skeleton of this sponge is completely covered with RGO layers which are closely linked to the skeleton. This sponge has an abundant pore structure, high selectivity, good recyclability, low cost, and outstanding adsorption capacity for floating oil or heavy oil underwater. In addition, this sponge can maintain excellent adsorption performance for various oils and organic solvents over 50 cycles by squeezing, and exhibits extremely high separation efficiencies, up to 6 × 106 and 3.6 × 106 L·m−3·h−1 in non-turbulent and turbulent water/oil systems, respectively. This superhydrophobic adsorbent with attractive properties may find various applications, especially in large-scale removal of organic contaminants and oil spill cleanup.

关键词： superhydrophobicity     mechanically flexibility     water/oil separation     reduced graphene oxide wrapped sponge    

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膜接触破乳——用于油包水乳液分离的超疏水ZIF-8@rGO膜 Article

顾佳慧, 瞿周, 张祥宁, 范红玮, 李春喜, Jürgen Caro, 孟洪

《工程（英文）》 2023年 第23卷 第4期   页码 73-81 doi: 10.1016/j.eng.2022.02.017

摘要：

水-油界面不平衡是实现油包水乳液破乳的关键。传统膜通常是依赖较高的跨膜压力破坏界面平衡而实现破乳。本文提出了可自然、快速地破坏水-油界面平衡的“接触破乳”的概念，开发了一种对有机组分具有高通量的新型破乳分离膜。具体制备过程分为两步，首先通过真空辅助抽滤法在聚四氟乙烯（PTFE）基底上组装ZIF-8@rGO微球（ZGS）层，再采用聚二甲基硅氧烷（PDMS）交联溶液进行固定化处理。由于ZGS表面为微纳米阶层结构，所制备的ZIF-8@rGO@PDMS/PTFE（ZGPP）膜表面展现出超疏水性特性，当表面活性剂稳定的油包水乳液接触到膜表面时，微纳结构的超疏水膜表面会引起水-油界面不平衡。ZGPP膜对油包水乳液具有良好的分离破乳性能，在0.15 bar（15 kPa）的低跨膜压力下，分离效率可以达到99.57%，通量可达到2254 L·m‒2·h‒1，且对于表面活性剂稳定的纳米级甲苯水乳液（平均液滴尺寸为57 nm）的体系也可以实现破乳分离。“接触破乳”概念的提出有望为开发新一代油包水乳液分离的破乳膜提供新的思路。

关键词： 油包水乳液     破乳     油水分离     超疏水膜    

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membranes with micro-nano composite structure using a facile atomization-assisted nonsolvent induced phase separation

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1268-1280 doi: 10.1007/s11705-022-2143-5

摘要： The micro-nano composite structure can endow separation membranes with special surface properties, but it often has the problems of inefficient preparation process and poor structural stability. In this work, a novel atomization-assisted nonsolvent induced phase separation method, which is also highly efficient and very simple, has been developed. By using this method, a bicontinuous porous microfiltration membrane with robust micro-nano composite structure was obtained via commercially available polymers of polyacrylonitrile and polyvinylpyrrolidone. The formation mechanism of the micro-nano composite structure was proposed. The microphase separation of polyacrylonitrile and polyvinylpyrrolidone components during the atomization pretreatment process and the hydrogen bonding between polyacrylonitrile and polyvinylpyrrolidone molecules should have resulted in the nano-protrusions on the membrane skeleton. The membrane exhibits superhydrophilicity in air and superoleophobicity underwater. The membrane can separate both surfactant-free and surfactant-stabilized oil-in-water emulsions with high separation efficiency and permeation flux. With excellent antifouling property and robust microstructure, the membrane can easily be recycled for long-term separation. Furthermore, the scale-up verification from laboratory preparation to continuous production has been achieved. The simple, efficient, cost-effective preparation method and excellent membrane properties indicate the great potential of the developed membranes in practical applications.

关键词： atomization     nonsolvent induced phase separation     bicontinuous porous structure     micro-nano composite structure     oil-water separation    

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Bioinspired cellulose-based membranes in oily wastewater treatment

《环境科学与工程前沿（英文）》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1515-2

摘要：

• Cellulose-based membrane separates oily wastewater mimicking the living things.

关键词： Cellulose     Bioinspired membrane     Superhydrophobic surface     Underwater superoleophobic surface     Oil-water separation    

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标题 作者 时间 类型 操作

MILP synthesis of separation processes for waste oil-in-water emulsions treatment

Zorka N. Pintarič,Gorazd P. Škof,Zdravko Kravanja

期刊论文

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

Shanshan Zhao, Zhu Tao, Liwei Chen, Muqiao Han, Bin Zhao, Xuelin Tian, Liang Wang, Fangang Meng

期刊论文

Biodegradable, superhydrophobic walnut wood membrane for the separation of oil/water mixtures

期刊论文

Highly hydrophobic oil−water separation membrane: reutilization of waste reverse osmosis membrane

期刊论文

Fabrication of a superhydrophilic/underwater superoleophobic stainless steel mesh for oil/water separation

期刊论文

Functional flax fiber with UV-induced switchable wettability for multipurpose oil-water separation

期刊论文

properties of a silver particle-coated and 1-dodecanethiol-modified superhydrophobic melamine sponge for oil/water separation

期刊论文

construction of pseudo-Janus silica/surfactant assembly and their application to stabilize Pickering emulsionsand enhance oil recovery

期刊论文

Optimising the oil phases of aluminium hydrogel-stabilised emulsions for stable, safe and efficient vaccine

期刊论文

Easily-manufactured paper-based materials with high porosity for adsorption/separation applications in

期刊论文

A novel composite coating mesh film for oil-water separation

Futao QIN, Zhijia YU, Xinhui FANG, Xinghua LIU, Xiangyu SUN

期刊论文

Superhydrophobic, mechanically flexible and recyclable reduced graphene oxide wrapped sponge for highly efficient oil/water separation

Lijuan Qiu, Ruiyang Zhang, Ying Zhang, Chengjin Li, Qian Zhang, Ying Zhou

期刊论文

膜接触破乳——用于油包水乳液分离的超疏水ZIF-8@rGO膜

顾佳慧, 瞿周, 张祥宁, 范红玮, 李春喜, Jürgen Caro, 孟洪

期刊论文

membranes with micro-nano composite structure using a facile atomization-assisted nonsolvent induced phase separation

期刊论文

Bioinspired cellulose-based membranes in oily wastewater treatment

期刊论文