Excellent Antifouling Properties Research Articles

Green Solvent-Based Antifouling Polymer Brushes Demonstrate Excellent Hemocompatibility.

Medical devices are crucial for patient care, yet even the best biomaterials lead to infections and unwanted activation of blood coagulation, potentially being life-threatening. While hydrophilic polymer brushes are the best coatings to mitigate these issues, their reliance on fossil raw materials underscores the urgency of bio-based alternatives. In this work, we introduce polymer brushes of a green solvent-based monomer, prohibiting protein adsorption, bacterial colonization, and blood clot formation at the same level as fossil-based polymer brushes. The polymer brushes are composed of N,N-dimethyl lactamide acrylate (DMLA), can be polymerized in a controlled manner, and show strong hydrophilicity as determined by thermodynamic analysis of the surface tension components. The contact of various challenging protein solutions results in repellency on the poly(DMLA) brushes. Furthermore, the poly(DMLA) brushes completely prevent the adhesion and colonization of Escherichia coli. Remarkably, upon blood contact, the poly(DMLA) brushes successfully prevent the formation of a fibrin network and leukocyte adhesion on the surface. While showcasing excellent antifouling properties similar to those of N-hydroxypropyl methacrylamide (HPMA) polymer brushes as one of the best antifouling coatings, the absence of hydroxyl groups prevents activation of the complement system in blood. We envision the polymer brushes to contribute to the future of hemocompatible coatings.

Precisely engineered bionic Cu-doped titanium dioxide nanoarrays/fluorine-doped tin oxide with excellent antibacterial and antifouling properties

Precisely engineered bionic Cu-doped titanium dioxide nanoarrays/fluorine-doped tin oxide with excellent antibacterial and antifouling properties

Thermoresponsive and Photocrosslinkable Poly(2-alkyl-2-oxazoline) Toolbox - Customizable Ultralow-Fouling Hydrogel Coatings for Blood Plasma Environments.

This study focuses on developing surface coatings with excellent antifouling properties, crucial for applications in the medical, biological, and technical fields, for materials and devices in direct contact with living tissues and bodily fluids such as blood. This approach combines thermoresponsive poly(2-alkyl-2-oxazoline)s, known for their inherent protein-repellent characteristics, with established antifouling motifs based on betaines. The polymer framework is constructed from various monomer types, including a novel benzophenone-modified 2-oxazoline for photocrosslinking and an azide-functionalized 2-oxazoline, allowing subsequent modification with alkyne-substituted antifouling motifs through copper(I)-catalyzed azide-alkyne cycloaddition. From these polymers surface-attached networks are created on benzophenone-modified gold substrates via photocrosslinking, resulting in hydrogel coatings with several micrometers thickness when swollen with aqueous media. Given that poly(2-alkyl-2-oxazoline)s can exhibit a lower critical solution temperature in water, their temperature-dependent solubility is compared to the swelling behavior of the surface-attached hydrogels upon thermal stimulation. The antifouling performance of these hydrogel coatings in contact with human blood plasma is further evaluated by surface plasmon resonance and optical waveguide spectroscopy. All surfaces demonstrate extremely low retention of blood plasma components, even with undiluted plasma. Notably, hydrogel layers with sulfobetaine moieties allow efficient penetration by plasma components, which can then be easily removed by rinsing with buffer.

Superhydrophilic/superoleophobic GO@CoSx photocatalytic membranes with excellent antifouling properties for efficient oil-water separation and organic pollutant degradation

With the development of industry, water resources have been seriously polluted, posing a great threat to human health and ecological development, and it is urgent to realize the efficient treatment of sewage-containing wastewater. The CoSx modified by thioacetamide grew in the interlayer of graphene oxide, which provided the composite membrane with self-cleaning ability, and at the same time enlarged the interlayer channels, which resulted in the flux and hydrophilicity significantly better than that of GO, and the retention rate of different types of oil-in-water emulsions was above 99 %. Encouragingly, the GO@CoSx-activated PMS system exhibited extremely high degradation performance for methylene blue. After 5 cycles, the flux of the composite membrane to the oil red-petroleum ether-oil-in-water emulsion under the light condition was higher than that under the dark condition, and the retention rate was kept at 99.93 %, with excellent antifouling performance. The composite membrane showed good degradation of methylene blue under alkaline conditions (99.84 %) and excellent removal of oil red-petroleum ether-oil-in-water emulsion under strong acid/alkaline conditions (99.37 %). The composite membrane has good chemical stability and mechanical properties for long-term use. This study will provide a new idea for the separation of oil-water emulsions, which has a broad application prospect.

Development of Janus membranes with asymmetric wettability for desalination of impaired seawater by direct contact membrane distillation

Membrane distillation (MD) is an emerging technology for direct seawater desalination. The widely employed hydrophobic membranes are susceptible to pore wetting/ fouling in the presence of organic contaminants in seawater. Here, we demonstrate a facile method of preparing Janus membranes with hydrophilic/hydrophobic faces having excellent anti-fouling and anti-wetting properties. The hydrophobic substrate is a PVDF-co-HFP membrane incorporating fluoroalkylsilane (FAS) grafted hydrophobic MIL-53(Al)- a form of metal organic framework (h-MIL-53(Al)), and the hydrophilic coating is prepared by the direct deposition of polydopamine (PDA) (top layer). The optimum membrane exhibited a stable flux of 11 L/m2h and permeate conductivity ∼10 µS/cm for up to 60 h of seawater desalination. The anti-wetting property of the Janus membrane was demonstrated from the stable performance when challenging the membrane with impaired seawater containing low surface tension compounds such as sodium dodecyl sulphate (SDS) and propylene glycol (PG), and oil (hexadecane). The prepared membrane exhibited wetting resistance of 45 h and 18 h when feed was seawater containing 0.3 mM SDS and 3 wt% PG, respectively. The membrane displayed excellent resistance to fouling for desalination from SDS-stabilized hexadecane (500 ppm)/seawater feeds for up to 50 h (5 cycles). The membrane fabricated in this study holds the potential for seawater desalination.

Fabrication of an electrically conductive separation layer with stable nanonetworks for efficient removal of heavy metals under an external voltage

Positively charged nanofiltration membrane shows great potentials in removing heavy metal ions from wastewater, but excellent separation and antifouling properties remain a challenge. Herein, a novel nanocomposite membrane with a dual-charged electrically conductive separation layer was fabricated by combining phase inversion, vacuum filtration and chemical crosslinking. The microstructure of PSF/sodium styrene-maleic anhydride copolymer (SMANa) composite membranes was systematically manipulated by adjusting the intermolecular binding state of SMA. Subsequently, various deposition layers were generated on the membrane surface by tuning the CNT/rGO ratios, and polyethylenimine (PEI) was also introduced by crosslinking with tannic acid (TA). The optimized membrane possessed a dual-charged separation layer with excellent conductivity and stable three-dimensional (3D) nanonetworks, and acted as cathode to achieve outstanding rejections of Cu2+(92.9%), Ni2+ (99.0%), Pb2+ (99.9%) and Cd2+ (99.5%) at a -3V voltage, with the permeate fluxes of 14.4～18.6 L/m2 h bar. This is ascribed to the synergistic effect among the electroreduction of metal ions, the chemical reaction with OH− to form hydroxides, the chelation with –OH and –NH2 groups, and the adsorption-induced electrostatic repulsion. Importantly, it also displayed superior stability over multiple runs and outstanding antifouling performances owing to the superposition of electrochemistry effect and stable hydration layers.

Photothermal Superhydrophobic Cotton Fabric Based on Silver Nanoparticles Cross-Linked by Polydopamine and Polyethylenimide.

Photothermal materials that can convert solar energy into heat energy through photothermal conversion have attracted extensive attention, but these materials are easily polluted by the environment. Here, we propose a simple and effective strategy for constructing photothermal superhydrophobic cotton fabrics with self-cleaning ability. The PDA@PEI@GA@Ag@PDMS-coated cotton fabric can achieve good superhydrophobicity (water contact angle: 159.6°) by a simple dipping method and mussel-inspired dopamine surface modification, which is regulated by the mass of dopamine, the mass of silver nitrate, and the concentration of polydimethylsiloxane (PDMS). The coated cotton fabric has good physical and chemical stability. Meanwhile, the coated cotton fabric has excellent self-cleaning and antifouling properties. The superhydrophobic PDA@PEI@GA@Ag@PDMS fabric exhibits excellent and stable photothermal properties, with the surface temperature reaching 70.4 °C under simulated sunlight with a current of 20 A. This photothermal superhydrophobic fabric with self-cleaning properties is expected to be applied in the field of photothermal conversion.

Multifunctional Ti3C2Tx MXene/Silver Nanowire Membranes with Excellent Catalytic, Antifouling, and Antibacterial Properties for Nitrophenol-Containing Water Purification.

The uncontrolled release of nitrophenol and dye pollutants into water systems is an increasingly serious worldwide concern, and thus efficient wastewater treatment technologies are urgently needed. Herein we report a novel two-dimensional (2D) transition metal carbides and/or nitrides (Ti3C2Tx MXene) membrane modified with silver nanowires (AgNWs) by vacuum assisted filtration technology for the ultrafast nitrophenol catalysis and water purification applications. Regular and controllable membrane transport channels were constructed by stacking Ti3C2Tx MXene nanosheets. Furthermore, the intercalation of AgNWs into the Ti3C2Tx MXene interlayer greatly enlarged the interlayer spacing, resulting in more gaps for fast and selective molecular transport. The optimized Ti3C2Tx MXene@AgNWs (M@A) membrane exhibited a water flux up to ∼191.9 L/(m2 h) while maintaining a high bovine serum albumin (BSA) rejection of ∼95.4%. We emphatically used M@A membranes as efficient catalysts for the reduction of 4-nitrophenol (4-NP), and the results indicated that M@A-12% membrane exhibited the greatest catalytic reduction ability, and recycling utilization. M@A-12% membrane also had an antibacterial rate of more than 99% against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). This work provides a possibility to expand the application of 2D multifunctional M@A membranes in wastewater treatment and pollutant catalytic degradation.

Superhydrophobic Fe-based amorphous alloy coatings with excellent anti-fouling and anti-corrosion properties by picosecond laser texturing

Producing superhydrophobic surfaces on the amorphous alloy coatings with excellent anti-corrosion and anti-fouling properties offers a promising strategy to broaden the applications of amorphous alloys in marine fields. In this work, the superhydrophobic surfaces on the Fe-based amorphous alloy coatings with micro-nano hierarchical structures were fabricated using picosecond pulsed laser texturing (LT) and surface chemical modification. The fabricated superhydrophobic coating surfaces have achieved a maximum contact angle of 166.5°and a minimum sliding angle of 3.6°. Additionally, these produced coatings also demonstrate outstanding self-cleaning and anti-fouling properties for preventing surface contamination. The superhydrophobicity originated from the formation of micro-nano hierarchical structures and the grafting of organic compounds with low surface free energy on the LT fabricated surfaces. The changes in wettability were attributed to the differences in the solid–liquid interfacial area fractions. The electrochemistry tests revealed that the corrosion resistance of the produced coatings with superhydrophobic surfaces had improved considerably compared with the as-sprayed amorphous alloy coatings, which could broaden the functional applications of the Fe-based amorphous alloy coatings.

One-step separation of fat globules based on size from bovine milk using a cross-flow microfiltration

Milk microfiltration has gained attention in the dairy industry due to its ability to selectively separate and concentrate bioactive components from milk and its further application in food fortification. One such compound is milk fat globules, a bioactive component with potential health benefits, which undergoes structural and functional damage, membrane phospholipids loss, experience longer processing time, and higher recovery cost due to its current multi-step separation process. We developed a single-step approach based on size for the separation of smaller-size milk fat globules from cow and buffalo milk using a porous polysulfone membrane through a cross-flow microfiltration system. An asymmetric polysulfone membrane with an average pore size of 0.8 ± 0.03 µm was synthesized via phase inversion and subsequently characterized for surface morphology, hydrophilicity, porosity, thermo-mechanical properties, and water contact angle. The membrane demonstrated good performance, with initial milk permeate flux ranging from 296 to 613 L/m2h at different transmembrane pressures (e.g., 0.2, 0.4, 0.6 bar) for both animal groups, with a gradual decline due to concentration polarization, and eventually reaching a steady state. Notably, at lower transmembrane pressure, the membrane exhibited excellent antifouling properties (flux recovery of 81.56–83 %) and reusability over three cycles. Microscopic examination of milk fat globules confirmed the successful size-based separation with intact globule membrane, high phospholipid yield, and mass balance. The results, to the best of our knowledge, demonstrate for the first time an in-depth analysis of membrane fouling and reusability for selective isolation of milk fat globules.

Flow injection analysis coupled with photoelectrochemical immunoassay for simultaneous detection of anti-SARS-CoV-2-spike and anti-SARS-CoV-2-nucleocapsid antibodies in serum samples

A thin-layer flow cell of low internal volume (12 μL) is incorporated in a flow injection analysis (FIA) system for simultaneous and real-time photoelectrochemical (PEC) immunoassay of anti-SARS-CoV-2 spike 1 (S1) and anti-SARS-CoV-2 nucleocapsid (N) antibodies. Covalent linkage of S1 and N proteins to two separate polyethylene glycol (PEG)-covered gold nanoparticles (AuNPs)/TiO2 nanotube array (NTA) electrodes affords 10 consecutive analyses with surface regenerations in between. An indium tin oxide (ITO) allows visible light to impinge onto the two electrodes. The detection limits for anti-S1 and anti-N antibodies were estimated to be 177 and 97 ng mL−1, respectively. Such values compare well with those achieved with other reported methods and satisfy the requirement for screening convalescent patients with low antibody levels. Additionally, our method exhibits excellent intra-batch (RSD = 1.3%), inter-batch (RSD = 3.4%), intra-day (RSD = 1.0%), and inter-day (RSD = 1.6%) reproducibility. The obviation of an enzyme label and continuous analysis markedly decreased the assay cost and duration, rendering this method cost-effective. The excellent anti-fouling property of PEG enables accuracy validation by comparing our PEC immunoassays of patient sera to those of ELISA. In addition, the simultaneous detection of two antibodies holds great potential in disease diagnosis and immunity studies.

Biomimetic hydrophilic modification of poly (vinylidene fluoride) membrane for efficient oil-in-water emulsions separation

Membrane separation is one of the simple and efficient methods for treating oily wastewater. To improve the efficiency of oil-in-water emulsion separation, alkali treatment was used to promote the deposition of Fe (III) on poly (vinylidene fluoride) (PVDF) membranes, and the tannic acid (TA)-glutathione (GSH) hydrophilic coating was produced on the membrane surface by biomimetic coating method under weak alkaline conditions. The PVDF membrane with hydrophilic coating and multi-layered surface structure showed hydrophilic/ underwater superoleophobic. Meanwhile, the permeability and antifouling properties were significantly enhanced. According to the experimental results, the optimized modified membrane (MF-3) had excellent pure water flux (3368.0 ± 94.2 L·m−2·h−1), and oil rejection was 99.3 ± 0.2 % for toluene-in-water emulsion. In addition, after simulated fouling and regeneration by bovine serum albumin (BSA) solution, the flux recovery rate reached 97.0 %. Excellent underwater anti-oil adhesion and antifouling properties help maintain high separation efficiency during multiple filtration cycles. The chemical stability of the modified membranes was demonstrated after 7 d immersion in acid, alkali, and salt solutions, respectively. The superior performances of the membrane are attributed to the constructed hydrophilic coating. This environmentally friendly PVDF membrane modification strategy has great potential for application in oil-in-water emulsion separation and provides a reliable solution for sustainable development.

Covalent codeposition modification of reverse osmosis membranes with Noria and zwitterionic copolymers for antifouling in reclaimed water production

Reverse osmosis (RO) has been recognized as a promising technology to treat municipal wastewater. However, membrane fouling is still an important hurdle in the RO membrane operation. The present work demonstrates the facile and high-effective fabrication of a robust antifouling RO membrane by the codeposition of Noria with zwitterionic copolymers. This modified coating is irreversibly bound to the membrane during typical membrane operational conditions. Compared with the pristine membrane, the modified membrane (that is, the TFC-Co-8 membrane) possesses improved hydrophilicity, reduced roughness, and lower negative charge. Our results illustrate that the TFC-Co-8 membrane displays an excellent antifouling property with milder flux decline and higher flux recovery during protein and alginate filtrations. Additionally, the TFC-Co-8 membrane is applied in the treatment of actual secondary effluent and also exhibits a superior antifouling property, which is consistent with the results of the simulated solution. This work provides a reference for the design of antifouling RO membrane in reclaimed water production.

Antifouling and Injectable Granular Hydrogel for the Prevention of Postoperative Intrauterine Adhesion.

Postoperative intrauterine adhesion (IUA), caused by endometrial basal layer injury, is one of the main causes of female infertility. The excessive deposition of fibrin as well as fibroblast is considered the root cause of IUA. However, few clinical strategies are effective in preventing extracellular matrix (ECM) deposition at endometrial wounds that include protein and cell deposits. Herein, the injectable granular poly(N-(2-hydroxyethyl) acrylamide) (PHEAA) hydrogel (granular PHEAA gel), which presents excellent antifouling properties and remarkably prevents protein and cell adhesions, is used to prevent postoperative IUA. The granular PHEAA gel with a jammed network structure exhibits outstanding injectability and superior stability. Compared with the IUA group, the granular PHEAA gel can promote regeneration of the endometrium while reducing the area of endometrial fibrosis. Immunohistochemical staining experiments indicate that the granular PHEAA gel can improve the proliferation of the endometrium, promote vascularization, and enhance anti-inflammatory effect in IUA rats. And the granular PHEAA gel can effectively slow down the fibrosis of uterine tissue. Importantly, the number of embryos is significantly increased after injecting granular PHEAA gel, inferring that there is an obvious reproductive function recovery of injured endometrium.

Eco-friendly polysaccharide coatings for antifouling and drag-reduction and potential application for marine devices

Traditional antifouling agents usually have a certain toxic effect on marine environments and non-target organisms. In this study, Dictyophora indusiata polysaccharide (DIP) was applied as a natural antifouling surface modifier to prepare the surface coating for marine antifouling. Three DIP coatings were prepared: D. indusiata spore polysaccharide (DISP), D. indusiata volva polysaccharide (DIVP), and D. indusiata embryonic body polysaccharide (DIEP). The antifouling, tribological, and anticorrosion behavior of the coatings were examined. Results revealed that the three kinds of DIP coatings had excellent antifouling properties, which could effectively prevent the adhesion of Chlorella and the attachment of water-based and oily stains on the surface. Additionally, the coatings showed great mechanical stability and could maintain an extremely low coefficient of friction (COF < 0.05) after continuous wear. The drag reduction rate of the coated surfaces reached 5%, showing a powerful lubrication performance. Furthermore, the DIP coatings presented an outstanding corrosion resistance, where the equivalent circuit impedances were 4–9 orders of magnitude higher than the control groups. This research showed a promising prospect of surface coating fabrication with DIP for marine devices to achieve the purpose of antifouling and drag reduction.

Cinnamaldehyde grafted porous Aerogel-Organ gel liquid infused surface for achieving difunctional long-term dynamic antifouling

Marine biofouling caused a number of questions about energy consumption and safety. While there were still some challenges in developing an environmentally friendly, non-toxic and long-term antifouling slippery liquid-infused porous surface (SLIPS). Here, we proposed a difunctional antifouling strategy via constructing porous polydimethylsiloxane (PDMS) surface with a layer of aerogel by sol-gel method and grafted cinnamaldehyde chemically. The improvement in structure enhanced the liquid storage stability of coating, which in turn increases its anti-bioadhesive ability. In addition, the grafted cinnamaldehyde could also be used to act as a chemical antibacterial and is intelligently released in the face of harsh fouling environments, which played a key role in prolonging the antibacterial lifespan of the coating. After the 120-hour anti-bacteria experiment and the 25-day anti-algae experiment, the anti-Escherichia coli (anti-E. coli) rate and the anti-algae rate of the coating reached 99.6% and 99.9%, respectively, which was attributed to the excellent long-term antifouling properties of the coating. The combination of physical and chemical antifouling property made the coating achieve long-term fouling prevention for marine engineering equipment.

Preparation and characterization of a silicone RAFT-modified aqueous acrylic resin coating for wood antifouling

Anionic emulsifiers, synthesized from novel silicone RAFT reagents (RAFT-PDMS), acrylic acid, lauryl methacrylate, and methyl methacrylate, were used to create a macromolecular silicone-modified polyacrylate aqueous emulsion. This emulsion was prepared by copolymerizing the custom-made anionic emulsifier with hydroxyethyl acrylate and other monomers. The emulsion underwent crosslinking with isocyanate, leading to a novel aqueous wood varnish incorporating polydimethylsiloxane chain segments. The structural features of RAFT-PDMS were characterized using 1HNMR, Fourier Transform Infrared Spectroscopy (FTIR), Ultraviolet-Visible Absorption Spectroscopy (UV–VIS), and Energy-Dispersive X-ray Spectroscopy (EDS). By adjusting the degree of polymerization and content of RAFT-PDMS, emulsions with a core-shell structure were generated. The impact of RAFT-PDMS on the molecular weight, particle size, and thermal properties of the latex was evaluated. Studies demonstrated that the applied wood coatings reduced surface roughness while enhancing gloss and hydrophobicity. Further tests revealed excellent antifouling properties and resistance to both acid and alkali for the coating. This type of wood paint could address challenges associated with the difficulty of combining large molecule organosilicones with wood, thereby offering a novel approach for wood paint applications.

Ti3C2Tx-Au hybrid composites-based electrochemical biosensors for calreticulin biomarker detection

A sensitive biosensor is critical for early breast cancer treatment and prognosis. Herein, a label-free electrochemical immunosensor is proposed for the sensitive detection of calreticulin (CALR), a new breast cancer biomarker. The biosensor relied upon an electroactive hybrid of ultra-thin Ti3C2Tx nanosheets preadsorbed with Au NPs and methylene blue (MB)(MB–Ti3C2Tx–Au), which served as redox-active centers and an electroactive probe to detect CALR biomarkers respectively. The detection mechanism followed a simple inhibition strategy, where the optimal differential pulse voltammetry (DPV) response of preadsorbed MB over the Ti3C2Tx–Au electrode decreased in proportion to the concentration of CALR biomarkers owing to the formation of the antibody-antigen immunocomplex. The biosensor could detect CALR-biomarker in the concentration range of 0.0015 to 0.94 ng mL−1 with a limit of detection (LOD) of 0.28 pg mL−1 and showed excellent antifouling properties against commonly encountered biomolecules such as hemoglobin (Ig), immunoglobulin G (IgG), neuron-specific enolase (NSE), and tumor necrosis factor-alpha (TNF). The proposed strategy provides an efficient method for utilizing MXene nanosheets to construct advanced biosensors with promising clinical applications.

High-performance CPES nanofiltration membrane decorated by cinnamon extract with efficient antibacterial/anti-fouling property for post treatment of biologically treated industrial wastewater

In this work, cinnamon extract/ coupling modified polyether sulfone (CiE/CPES) mixed matrix membrane with excellent anti-fouling and antibacterial properties was synthesized by the phase inversion method. To characterize the modified membrane, SEM, AFM, ATR – FTIR, EDX, WCA and porosity measurements were performed. SEM images showed the wider finger-like pores compared to the unfilled-CPES membrane. AFM images exhibited that with the addition of CiE to the polymer matrix the surface of CiE/CPES membranes has been significantly smoothed. BSA was used as a foulant to evaluate the anti-fouling properties and the results showed excellent flux recovery ratio (more than 95%) in all weight percentages of CiE, which indicates the significant improvement of self-cleaning property of fabricated membranes. To confirm the antibacterial properties of CiE, agar diffusion test was performed. A clear large halo around the CiE was observed for both model bacteria. The average halo radius was 41.63 mm for E. coli and 47.25 mm for S. aureus, which showed better performance compared to other routine studies. Also, the bacteria suspension immersion test and SEM analysis were investigated. The results showed a significant reduction of bacteria on the membrane surface compared to the control sample, which confirmed the excellent performance of CiE in the membrane. Besides, to measure the separation performance of the membranes, the biologically treated soft drink industrial wastewater (BTW) rejection was evaluated. The results provided very good efficiency in BTW purification. For further study, the desalination performance of the membranes was evaluated by examining the rejection of different salt solutions, and the order of rejection in all prepared membranes followed MgSO4 > MgCl2 > NaCl.

In situ reaction enabled surface segregation toward dual-heterogeneous antifouling membranes for oil-water separation

Fabricating membranes with superior antifouling property and long-term high performance is in great demand for efficient oil-water separation. Herein, we reported a reaction enabled surface segregation method for antifouling membrane fabrication, in which the pre-synthesized fluorinated ternary copolymer Pluronic F127 was coordinated with Ti4+ as segregation additive in the membrane casting bath. Additionally, tannic acid was utilized to enhance the self-assembly of the copolymer in the coagulation bath, and freshly-biomineralized TiO2 was anchored into the membrane surface through hydrogen bond. A hydrogel layer was constructed onto the membrane surface with synergistically tailored heterogeneous chemical composition and heterogeneous geometrical roughness. The dual-heterogeneous membrane exhibited hydrophilic and underwater superoleophobic features, resulting in high water flux (621.7 L m−2 h−1) at low operation pressure of 0.05 MPa and an excellent antifouling property (only 4.8% flux decline during 24-hour filtration). In situ reaction enabled surface segregation method will accelerate the development of antifouling membranes for oil-in-water emulsion separation.