Biodegradable electrospinning superhydrophilic nanofiber membranes for ultrafast oil-water separation.

Although membrane technology has attracted considerable attention for oily wastewater treatment, the plastic waste generated from discarded membranes presents an immediate challenge for achieving eco-friendly separation. We designed on-demand biodegradable superhydrophilic membranes composed of polylactic acid nanofibers in conjunction with polyethylene oxide hydrogels using electrospinning technology for ultrafast purification of oily water. Our results showed that the use of the polyethylene oxide hydrogels increased the number of hydrogen bonds formed between the membrane surface and water molecules by 357.6%. This converted hydrophobic membranes into superhydrophilic ones, which prevented membrane fouling and accelerated emulsion penetration through the membranes. The oil-in-water emulsion permeance of our newly designed nanofiber membranes increased by 61.9 times (2.1 × 104 liters per square meter per hour per bar) with separation efficiency >99.6%, which was superior to state-of-the-art membranes. Moreover, the formation of hydrogen bonds was found to accelerate polylactic acid biodegradation into lactic acid by over 30%, offering a promising approach for waste membrane treatment.

Surface manipulation for prevention of migratory viscous crude oil fouling in superhydrophilic membranes.

Here, we present a proactive fouling prevention mechanism that endows superhydrophilic membranes with antifouling capability against migratory viscous crude oil fouling. By simulating the hierarchical architecture/chemical composition of a dahlia leaf, a membrane surface is decorated with wrinkled-pattern microparticles, exhibiting a unique proactive fouling prevention mechanism based on a synergistic hydration layer/steric hindrance. The density functional theory and physicochemical characterizations demonstrate that the main chains of the microparticles are bent towards Fe3+ through coordination interactions to create nanoscale wrinkled patterns on smooth microparticle surfaces. Nanoscale wrinkled patterns reduce the surface roughness and increase the contact area between the membrane surface and water molecules, expanding the steric hindrance between the oil molecules and membrane surface. Molecular dynamic simulations reveal that the water-molecule densities and strengths of the hydrogen bonds are higher near the resultant membrane surface. With this concept, we can successfully inhibit the initial adhesion, migration, and deposition of oil, regardless of the viscosity, on the membrane surface and achieve migratory viscous crude oil antifouling. This research on the PFP mechanism opens pathways to realize superwettable materials for diverse applications in fields related to the environment, energy, health, and beyond.

Electrically Induced Underwater Superaerophilicity/Superaerophobicity Switching on Polypyrrole-Coated Mesh Films for Selective Bubble Permeation.

Recently, materials with controllable superwettability have attracted much attention. However, almost all studies focused on controlling wetting of water and oil; research on underwater gas bubble wetting control is still rare. Herein, we report a mesh film prepared by coating polypyrrole (PPy) film on Ti mesh. Briefly, the film mesh is underwater superaerophilic when PPy is doped with perfluorooctanesulfonate ions (PFOS- ), and becomes underwater superaerophobic as the PFOS- are removed. The transition of the wettability can be triggered by electrical stimuli, which is attributed to the cooperative effect between the rough structure and chemical components variation. The controllable wettability allows adjustable bubble permeation. It can be envisioned that the film will provide potential applications in the future, such as underwater bubble capture/release and microfluidic devices.

Constructing Scalable Superhydrophobic Membranes for Ultrafast Water-Oil Separation.

Superhydrophobic membranes are desirable for separation of water-in-oil emulsions, membrane distillation, and membrane condensation. However, the lack of large-scale manufacture methods of superhydrophobic membranes hampers their widespread applications. Here, a facile method of coaxial electrospinning is provided to manufacture superhydrophobic membranes for the ultrafast separation of water-in-oil emulsions. Under the high-voltage electric field, the polydimethylsiloxane (PDMS)-coated polyvinylidene fluoride (PVDF) nanofibers and PDMS microspheres with PVDF nanobulges were integrated together during the electrospinning process. Moreover, asymmetric composite membranes with selective layers are designed to reduce the resistance of the mass transfer. Consequently, the as-prepared asymmetric composite membrane exhibits an ultrafast permeance and excellent separation efficiency of about 99.6%, outperforming most of the state-of-the-art membranes reported previously. Most importantly, the membrane could be as large as 770 cm2, could be manufactured continuously, and could be easily enlarged further via tailoring the roller receptor, showing strong promise in the separation of water-in-oil emulsions.

Molecular basis of nucleosomal H3K36 methylation by NSD methyltransferases.

Histone methyltransferases of the nuclear receptor-binding SET domain protein (NSD) family, including NSD1, NSD2 and NSD3, have crucial roles in chromatin regulation and are implicated in oncogenesis1,2. NSD enzymes exhibit an autoinhibitory state that is relieved by binding to nucleosomes, enabling dimethylation of histone H3 at Lys36 (H3K36)3-7. However, the molecular basis that underlies this mechanism is largely unknown. Here we solve the cryo-electron microscopy structures of NSD2 and NSD3 bound to mononucleosomes. We find that binding of NSD2 and NSD3 to mononucleosomes causes DNA near the linker region to unwrap, which facilitates insertion of the catalytic core between the histone octamer and the unwrapped segment of DNA. A network of DNA- and histone-specific contacts between NSD2 or NSD3 and the nucleosome precisely defines the position of the enzyme on the nucleosome, explaining the specificity of methylation to H3K36. Intermolecular contacts between NSD proteins and nucleosomes are altered by several recurrent cancer-associated mutations in NSD2 and NSD3. NSDs that contain these mutations are catalytically hyperactive in vitro and in cells, and their ectopic expression promotes the proliferation of cancer cells and the growth of xenograft tumours. Together, our research provides molecular insights into the nucleosome-based recognition and histone-modification mechanisms of NSD2 and NSD3, which could lead to strategies for therapeutic targeting of proteins of the NSD family.

Under-Oil Switchable Superhydrophobicity to Superhydrophilicity Transition on TiO2 Nanotube Arrays.

Recently, smart interfacial materials that can reversibly transit between the superhydrophobicity and superhydrophilicity have aroused much attention. However, all present performances happen in air, and to realize such a smart transition in complex environments, such as oil, is still a challenge. Herein, TiO2 nanotube arrays with switchable transition between the superhydrophobicity and superhydrophilicity in oil are reported. The switching can be observed by alternation of UV irradiation and heating process, and the smart controllability can be ascribed to the cooperative effect between the surface nanostructures and the chemical composition variation. By using the controllable wetting performances, some applications such as under-oil droplet-based microreaction and water-removal from oil were demonstrated on our surface. This paper reports a surface with smart water wettability in oil, which could start some fresh ideas for wetting control on interfacial materials.

In situ hydrogels enhancing postoperative functional recovery by reducing iron overload after intracerebral haemorrhage.

The role of surgery for most patients with spontaneous intracerebral haemorrhage (ICH) remains controversial due to the continuous occurrence of postoperative iron overload induced by low clot clearance rate. In this study, human hair keratose hydrogel (KG) loading with minocycline hydrochloride (MH) were prepared to reduce iron overload for the improvement of the postoperative functional recovery after ICH aspiration surgery. Hemoglobin-induced iron accumulation in rat primary neuronal culture was delayed by the adsorptive capacity of blank KG, while MH-loaded KG displayed a stronger and more thorough cytoprotective effect than blank KG due to the combined effect of absorptive action to iron and sustained release of the iron chelator. Moreover, high iron-chelating efficiency in the hematoma region supplied by MH-loaded KG significantly reduced dose strength of iron chelator. In situ injection of KG with different MH loadings (2, 20, and 200µg) into the hematoma region after aspiration surgery showed a stronger effect on the reduction of ICH-induced iron accumulation, edema, and neurological deficits in rats compared to the postoperative intraperitoneal administration of MH (approximately 15mg). These results suggested that the in situ KG not only could effectively reduce the ICH postoperative iron overload and improve the postoperative functional recovery via the iron adsorption and sustained release of MH, but also has great potential to reduce the systemic adverse effects by decreasing the dose strength of iron chelator.

High Density of Free-Standing Holey Graphene/PPy Films for Superior Volumetric Capacitance of Supercapacitors.

The volumetric performance is a vitally important metric for portable electronic and wearable devices with limited space. However, it is contradictory for the most supercapacitors in the connection between the volumetric and gravimetric capacitances. Herein, we report a simple strategy to prepare a free-standing and binder-free holey graphene/PPy film that possesses a dense microstructure but still high gravimetric capacitances. The holey graphene/PPy film own high-efficiency ion transport channels and big ion-accessible surface area to achieve high-powered supercapacitor electrodes, which have a superior volumetric capacitance (416 F cm-3) and high gravimetric capacitance (438 F g-1) at 1.0 A g-1 in 6 M KOH electrolyte. Meanwhile, it possesses high rate capability and good cycling performance (82.4% capacitance retention even after 2000 cycles). Furthermore, the volumetric energy density of assembled holey graphene/PPy film symmetric supercapacitor can show high as 22.3 Wh L-1. Such densely packed free-standing holey graphene/PPy film is a very significant electrode material for compact and miniaturized energy storage equipment in the further.

Janus Copper Mesh Film with Unidirectional Water Transportation Ability toward High Efficiency Oil/Water Separation.

Inspired by the special asymmetric wettability and controllable permeation function of cell membranes, we report a Janus nanostructured copper mesh film with unidirectional water transportation ability. Water can permeate from the hydrophobic side to the hydrophilic side, but is retained in the opposite direction. Notably, based on this special unidirectional water permeation property, both heavy oil/water mixtures (ρoil >ρwater ) and light oil/water mixtures (ρoil <ρwater ) can be separated. Additionally, the film demonstrates high separation efficiency and good recyclability. This paper reports a new Janus film that achieved highly efficient oil/water separation based on smart control of the wettability of the film. It is believed to have the potential to be used in many practical applications, such as wastewater treatment and oil-spill cleanup.

Feather keratin hydrogel for wound repair: Preparation, healing effect and biocompatibility evaluation.

Keratins are highly attractive for wound healing due to their inherent bioactivity, biocompatibility and physical properties. However, nearly all wound healing studies have focused on human hair keratins, and the wound-repair effects and in vivo biocompatibilities of feather keratins are not clear. Feather keratins are derived from chicken feathers, which are considered to be the major waste in the poultry industry, and the quality of feather keratin is easier to control than that of human hair keratin due to human hair perming and colouring-dyeing. Thus, we extracted keratins from chicken feathers, and a feather keratin hydrogel was then prepared and used to test the in vivo wound-healing properties and biocompatibility. The results indicated that feather keratins displayed wound-healing and biodegradation properties similar to those of human hair keratins and were also highly compatible with those of the tissue and devoid of immunogenicity and systematic toxicity. Collectively, these results suggested that feather keratin hydrogel could be used for biomedical applications, particularly effective wound healing.

The design of underwater superoleophobic Ni/NiO microstructures with tunable oil adhesion.

Controlling oil adhesion in water is a fundamental issue in many practical applications for surfaces. Currently, almost all studies on underwater oil adhesion control are concentrated on regulating surface chemistry on polymer surfaces, and structure-dependent underwater oil adhesion is still rare, especially on inorganic materials. Herein, we report a series of underwater superoleophobic Ni/NiO surfaces with controlled oil adhesions by combining electro-deposition and heating techniques. The adhesive forces between an oil droplet and the surfaces can be adjusted from an extremely low (less than 1 µN) to a very high value (about 60 µN), and the tunable effect can be attributed to different wetting states that result from different microstructures on the surfaces. Moreover, the oil-adhesion controllability for different types of oils was also analyzed and the applications of the surface including oil droplet transportation and self-cleaning were discussed. The results reported herein provide a new feasible method for fabrication of underwater superoleophobic surfaces with controlled adhesion, and improve the understanding of the relationship between surface microstructures, adhesion, and the fabrication principle of tunable oil adhesive surfaces.

Regulating Underwater Oil Adhesion on Superoleophobic Copper Films through Assembling n-Alkanoic Acids.

Controlling liquid adhesion on special wetting surface is significant in many practical applications. In this paper, an easy self-assembled monolayer technique was advanced to modify nanostructured copper substrates, and tunable adhesive underwater superoleophobic surfaces were prepared. The surface adhesion can be regulated by simply varying the chain length of the n-alkanoic acids, and the tunable adhesive properties can be ascribed to the combined action of surfaces nanostructures and related variation in surface chemistry. Meanwhile, the tunable ability is universal, and the oil-adhesion controllability is suitable to various oils including silicon oil, n-hexane, and chloroform. Finally, on the basis of the special tunable adhesive properties, some applications of our surfaces including droplet storage, transfer, mixing, and so on are also discussed. The paper offers a novel and simple method to prepare underwater superoleophobic surfaces with regulated adhesion, which can potentially be applied in numerous fields, for instance, biodetection, microreactors, and microfluidic devices.

pH-controllable on-demand oil/water separation on the switchable superhydrophobic/superhydrophilic and underwater low-adhesive superoleophobic copper mesh film.

Recently, materials with controlled oil/water separation ability became a new research focus. Herein, we report a novel copper mesh film, which is superhydrophobic and superhydrophilic for nonalkaline water and alkaline water, respectively. Meanwhile, the film shows superoleophobicity in alkaline water. Using the film as a separating membrane, the oil/water separating process can be triggered on-demand by changing the water pH, which shows a good controllability. Moreover, it is found that the nanostructure and the appropriate pore size of the substrate are important for realization of a good separation effect. This paper offers a new insight into the application of surfaces with switchable wettability, and the film reported here has such a special ability that allows it to be used in other applications, such as sewage purification, filtration, and microfluidic device.

A molecular threading mechanism underlies Jumonji lysine demethylase KDM2A regulation of methylated H3K36.

The dynamic reversible methylation of lysine residues on histone proteins is central to chromatin biology. Key components are demethylase enzymes, which remove methyl moieties from lysine residues. KDM2A, a member of the Jumonji C domain-containing histone lysine demethylase family, specifically targets lower methylation states of H3K36. Here, structural studies reveal that H3K36 specificity for KDM2A is mediated by the U-shaped threading of the H3K36 peptide through a catalytic groove within KDM2A. The side chain of methylated K36 inserts into the catalytic pocket occupied by Ni(2+) and cofactor, where it is positioned and oriented for demethylation. Key residues contributing to K36me specificity on histone H3 are G33 and G34 (positioned within a narrow channel), P38 (a turn residue), and Y41 (inserts into its own pocket). Given that KDM2A was found to also bind the H3K36me3 peptide, we postulate that steric constraints could prevent α-ketoglutarate from undergoing an "off-line"-to-"in-line" transition necessary for the demethylation reaction. Furthermore, structure-guided substitutions of residues in the KDM2A catalytic pocket abrogate KDM2A-mediated functions important for suppression of cancer cell phenotypes. Together, our results deduce insights into the molecular basis underlying KDM2A regulation of the biologically important methylated H3K36 mark.

A selective jumonji H3K27 demethylase inhibitor modulates the proinflammatory macrophage response.

The jumonji (JMJ) family of histone demethylases are Fe2+- and α-ketoglutarate-dependent oxygenases that are essential components of regulatory transcriptional chromatin complexes. These enzymes demethylate lysine residues in histones in a methylation-state and sequence-specific context. Considerable effort has been devoted to gaining a mechanistic understanding of the roles of histone lysine demethylases in eukaryotic transcription, genome integrity and epigenetic inheritance, as well as in development, physiology and disease. However, because of the absence of any selective inhibitors, the relevance of the demethylase activity of JMJ enzymes in regulating cellular responses remains poorly understood. Here we present a structure-guided small-molecule and chemoproteomics approach to elucidating the functional role of the H3K27me3-specific demethylase subfamily (KDM6 subfamily members JMJD3 and UTX). The liganded structures of human and mouse JMJD3 provide novel insight into the specificity determinants for cofactor, substrate and inhibitor recognition by the KDM6 subfamily of demethylases. We exploited these structural features to generate the first small-molecule catalytic site inhibitor that is selective for the H3K27me3-specific JMJ subfamily. We demonstrate that this inhibitor binds in a novel manner and reduces lipopolysaccharide-induced proinflammatory cytokine production by human primary macrophages, a process that depends on both JMJD3 and UTX. Our results resolve the ambiguity associated with the catalytic function of H3K27-specific JMJs in regulating disease-relevant inflammatory responses and provide encouragement for designing small-molecule inhibitors to allow selective pharmacological intervention across the JMJ family.