Water-soluble Monomers Research Articles

Enzymatically Polymerized Organic Conductors on Native Lipid Membranes.

The dual capability of conductive polymers to conduct ions and electrons, in combination with their flexible mechanical properties, makes them ideal for bioelectronic applications. This study explores the in situ enzymatic polymerization of water-soluble π-conjugated monomers on native lipid bilayers derived from the F11 cell line, mimicking mammalian neural membranes. Enzymatic polymerization was catalyzed using horseradish peroxidase (HRP) in the presence of oxidant hydrogen peroxide (H2O2) and monitored via electrochemical quartz crystal microbalance with dissipation (EQCM-D) and electrochemical impedance spectroscopy (EIS). Results showed polymerization with HRP. The structural properties of the formed polymer films were characterized ex situ using atomic force microscopy (AFM), while the quality of the F11 native lipid vesicles and bilayer was respectively assessed through dynamic light scattering (DLS) and fluorescence recovery after photobleaching (FRAP) techniques. This work demonstrates, for the first time, the feasibility of the in situ formation of conductive polymers on native lipid membranes, offering a promising approach for the development of minimally invasive neural electrodes to diagnose and treat neurological disorders.

Interconnecting EDOT-Based Polymers with Native Lignin toward Enhanced Charge Storage in Conductive Wood.

The 3D micro- and nanostructure of wood has extensively been employed as a template for cost-effective and renewable electronic technologies. However, other electroactive components, in particular native lignin, have been overlooked due to the absence of an approach that allows access of the lignin through the cell wall. In this study, we introduce an approach that focuses on establishing conjugated-polymer-based electrical connections at various length scales within the wood structure, aiming to leverage the charge storage capacity of native lignin in wood-based energy storage electrodes. We demonstrate that poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) PEDOT/PSS, integrated within the cell wall lumen, can be interfaced with native lignin through the wood cell wall through in situ polymerization of a water-soluble S-EDOT monomer. This approach increases the capacitance of the conductive wood to 315 mF cm-2 at a scan rate of 5 mV s-1, which is seven and, respectively, two times higher compared to the capacitance of conductive wood made with the single components PEDOT/PSS or S-PEDOT. Moreover, we show that the capacitance is contributed by both the electroactive polymers and native lignin, with native lignin accounting for over 70% of the total charge storage capacity. We show that accessing native lignin through in situ creation of electrical interconnections within the wood structure offers a pathway toward sustainable, wood-based electrodes with improved charge-storage capacity for applications in electronics and energy storage.

Fabrication of POSS-centered polyester network as high anti-chlorine and anti-fouling separation layer of membrane via successive Photo-ATRP and interfacial polymerization for molecular separation

The incorporation of polyhedral oligomeric sesquisiloxane (POSS), a distinctive nanoparticle, into the membrane separation layer represents an effective strategy for enhancing the chlorine resistance of membranes. This modification contributes to both the durability of the membrane and its separation efficiency. However, POSS is easy to agglomerate, which affects the separation performance of the membrane. In this paper, POSS-centered polyhydroxy polymer (OMEPOSS-P(GMA-NMDG)) was synthesized via photo-induced atom transfer radical polymerization and used as water-soluble monomer to prepare polyester separation layer on porous substrates through interfacial polymerization with trimelanoyl chloride. The obtained POSS-centered polyester membrane exhibits a high dye removal rate exceeding 99 %, and it can realize the screening of dye molecules with different molecular weight and different charge. Notably, the membrane demonstrates excellent chlorine resistance, maintaining effective separation efficiency after exposure to sodium hypochlorite solutions at concentrations of 10 000 ppm for 96 h and 1000 ppm for 7 days. It is worth noting that the membrane showed high anti-fouling performance. This method provides a useful guideline for the development of chlorine-resistant and anti-fouling separation membranes.

Preparation of an environmentally friendly water-soluble sizing agent and its application in CF/PPESK composites

In this study, a series of high temperature resistant water-soluble thermoplastic sizing agents were designed and synthesized to improve the interfacial bonding of CF/PPESK composites. The effects of the ratio of water-soluble functional monomer (PPL) and high temperature resistant monomer (DHPZ) on the performance of the pastes were investigated. The results showed that the sizing agent with PPL: DHPZ = 6: 4 had the best performance, and its thermal decomposition temperature was up to 348 °C, which met the requirements of the composite molding process. The ILSS and flexural strength reached the peaks of 67.2 MPa and 1526.5 MPa. The retention rates were 89.7 % and 81.8 %, respectively, after hydrothermal aging treatment, compared with 77.7 % and 79.2 % for the epoxy sizing agent. The bottleneck of traditional epoxy sizing agent and CF/PPESK composites molding process mismatch has been broken.

Overcoming a Conceptual Limitation of Industrial ε-Caprolactone Production via Chemoenzymatic Synthesis in Organic Medium.

The multi-10.000 tons scale manufactured chemical ε-caprolactone attracts high industrial interest due to its favorable biodegradability properties. However, besides being of petrochemical origin yet, its production has a conceptual limitation that is the difficult extraction of this highly water-soluble monomer from the water phase resulting from the aqueous solution of H2O2 applied as reagent. In this contribution, we report a chemoenzymatic cascade starting from bio-based phenol, which makes use of O2 instead of H2O2 and runs in pure organic medium, thus requiring only simply decantation and distillation as work-up. In a first step, phenol is hydrogenated quantitatively to cyclohexanol under solvent-free conditions with a Ru-catalyst. After simple removal of the heterogenous catalyst, cyclohexanol is converted to ε-caprolactone in a biocatalytic double oxidation with very high yields just requiring O2 as reagent. This biocatalytic process proceeds in pure organic medium, thus avoiding tedious extraction to isolate the highly water-soluble ε-caprolactone and enabling a substantially simplified work-up by only centrifugal separation of lyophilized whole cells and solvent removal. This oxidation is accomplished using a tailor-made recombinant whole-cell catalyst containing an alcohol dehydrogenase and a cyclohexanone monooxygenase mutant.

Strategies for preparation of chitosan based water-soluble fluorescent probes to detect Cr3+ and Cu2+ ions

The low solubility of chitosan (CS) imposes adverse effects on its application. In this work, one of the aims is to improve the water solubility of CS. By introducing water-soluble side chains to CS, this aim was achieved. Besides, fluorescent moieties were incorporated into the side chains, the fluorescent copolymers were endowed with Cr3+ and Cu2+ ions recognition ability. Firstly, a reversible addition-fragmentation chain transfer polymerization (RAFT) reagent with naphthalimide units and CC groups was prepared. Water-soluble monomer methyl acrylic acid (MAA) was employed in the RAFT polymerization. Thus, water-soluble polymer with fluorescent unit and -C ≡ C on both ends of the polymer was obtained. They were introduced into CS, and the CS-based fluorescent copolymers were obtained eventually. The amount of MAA introduced could be tuned to obtain three side chains of different lengths. It was found that the more MAA was introduced, the better the solubility of CS-TP was. The detection limits (LOD) of Cr3+ and Cu2+ were 44.6 nM and 54.5 nM, respectively. The detection of Cr3+ and Cu2+ ions is further combined with a mobile APP to realize real-time, portable, and visual detection. And the application in the logic gate, a new detection platform, is prepared.

Low-toxic gelcasting of zircon ceramics

Zircon (ZrSiO4) ceramics are highly valued in various industries due to their exceptional physical and chemical properties. In the present work, zircon ceramics with high-density and desirable mechanical properties were successfully prepared using an aqueous gelcasting method, involving the use of a low-toxic and water-soluble monomer, N,N-dimethylacrylamide (DMAA), as the binder. A high solid loading and low viscosity zircon slurry was achieved by optimizing the pH and the dosage of the ammonium polyacrylate (PAA-NH3) dispersant. Zircon green bodies fabricated through the gelcasting method exhibited uniform microstructures and relatively high mechanical strength exceeding 11.0 MPa. The impact of solid loading on the density, decomposition, flexural strength, micro-hardness, and microstructure of the final ceramics were carefully studied. Notably, the ceramics, prepared by solidifying the slurry with a 45 vol% solid loading and sintering the green body at 1550 °C for 2 h, exhibited a relative density of 96.3 %, high phase purity, a uniform microstructure, and the highest flexural strength of 407.9 MPa. The results demonstrate that mechanically robust dense zircon ceramics can be effectively prepared using the low-toxic gelcasting method.

Organic-organic interfacial polymerization for the ultrathin polyamide organic solvent nanofiltration membranes

There is an increasing demand for advanced membranes that exhibit both high perm-selectivity and good stability in organic solvents, particularly for organic solvent nanofiltration (OSN). Traditional methods of synthesizing thin films using conventional interfacial polymerization (CIP) have been limited by the use of water-soluble monomers, which has hindered the development of high-performance membranes. To address this issue, a new method called organic-organic interfacial polymerization (OOIP) has been proposed. This method allows for the use of aromatic amines that are not water-soluble in the fabrication of ultrathin polyamide (PA) (<40 nm) thin film composite (TFC) membranes. By investigating five different organic solvents (tetrahydrofuran, acetone, N,N-dimethylformamide, N,N-dimethylacetamide, dimethyl sulfoxide) with varying water content as the organic phase for a water-insoluble benzidine monomer, two diffusion models of monomers were identified that resulted in different membrane structures and degrees of network crosslinking. The ultrathin PA membranes produced using tetrahydrofuran-H2O and N,N-dimethylformamide-H2O, along with solvent activation, demonstrated high methanol permeances of 11.4 L m−2 h−1 bar−1 and 6.0 L m−2 h−1 bar−1, respectively, while maintaining exceptional rejections of over 99.0 % for small molecules with molecular weights greater than 452 g mol−1. The OOIP method is scalable and reproducible, making it suitable for large-scale membrane production. This innovative approach shows great potential for advancing OSN technology and providing efficient and cost-effective separation solutions for various industries.

Development of a plugging material featuring external flexibility and internal rigidity

Recognizing the challenges of low strength, inadequate cementation, significant pore development, and excellent connectivity of reef limestone, as well as the persistent issues of ‘re-leakage’ and increasing leaks when using rigid bridge plugs, this paper posits the use of materials possessing both flexible and rigid properties for the prevention of leaks and plugging in reef limestone formations. Consequently, a plugging material exhibiting external flexibility and internal rigidity is developed (EFIR Material). This synergistic approach employs the deformability of flexible materials and the skeletal support of rigid materials to create a high-strength, dense plugging section. The new design enhances the formation’s pressure-bearing capacity while effectively addressing leakage issues. The material’s functional structure design, a core-shell structure of EFIR, is achieved by reverse-phase suspension polymerization of acrylamide (AM), 2-acrylamide-2-methylpropanesulfonic acid (AMPS), and alkyl ketone polymer (NVP), water-soluble monomers functioning as the shell and modified sand as the core. The results indicate that EFIR retains significant flexibility and strength upon water absorption and expansion. A sand bed made from 10 to 18 mesh calcareous sand exhibits excellent sealing properties. The optimal dosage of 3%-4% produces robust sealing effects, withstands pressures up to 7 MPa, and results in a tightly cemented, high-strength sand bed post-sealing with reef tuff, displaying high-quality sealing that is resistant to re-leakage.

Synergistic interfacial polymerization between hydramine/diamine and trimesoyl chloride: A novel reaction for NF membrane preparation

Polyester-amide (PEA) thin film composite (TFC) NF membranes have rapidly evolved towards a competitive performance, benefiting from their remarkable antifouling capability and superior chlorine resistance. In this report, a new concept of synergistic interfacial polymerization is explored, which promptly triggers the reaction between hydramines and trimesoyl chloride (TMC) in the presence of a trace amount of diamines. This rapid-start mode enables the formation of defect-free PEA films without the requirement of catalysis. A comprehensive characterization of physicochemical properties using high-resolution mass spectrometer (HRMS) reveals that the recombination and formation of a “hydramine-diamine” coupling unit plays a decisive role in activating the synergistic interfacial polymerization reaction with TMC molecules. Taking the pair of serinol and piperazine (PIP) as an example, the PEA-NF membrane fabricated with 0.1 w/v% serinol mixed with 0.04 w/v% PIP as water-soluble monomer and 0.1 w/v% TMC as oil phase monomer was found to have a pure water permeability (PWP) of 18.5 L·m−2·h−1·bar−1 and a MgSO4 rejection of 95.5 %, which surpasses almost all the reported PEA NF membranes. Findings of the current research provide more possibilities for the low-cost and rapid synthesis of high-performance PEA membranes aiming for water purification.

Development and field application of strongly resilient temporary plugging diversion agent for fracturing

Temporary plugging diversion fracturing in multistage horizontal well is normally used to improve stimulation efficiency and increase production in unconventional reservoirs. Temporary plugging agent plays an important role in diversion fracturing. A strongly resilient temporary plugging diversion agent can improve the effectiveness of fracturing diversion. Therefore, a novel organosilicon temporary plugging diversion agent (QBZU) was developed through micellar copolymerization method. Self-synthesized strongly resilient temporary plugging diversion agent (QBZU gel) was prepared by using acrylamide, N, N′-methylene bisacrylamide, surfactants, organosilicon, ammonium persulfate and sodium bisulfite as chemical raw materials. The micellar copolymerization is investigated to overcome the incompatibility of hydrophobic organosilicon and water-soluble monomer by adding some appropriate surfactants. The experimental results indicated that the combination of sodium dodecyl sulphonate and Tween 80 provided excellent copolymerization results. The characteristics of compressive resistance, salt resistance, shearing resistance, resilience and degradation are superior compared with traditional rigid granular temporary plugging agent widely used in oilfields (QG hydrogel). According to the experimental evaluation results of QBZU, its pressure-bearing capacity can reach 56.3MPa, shearing strength can reach 410N, elastic modulus can reach 80MPa, and Poisson ratio can reach 0.48. Meanwhile, the main synthetic factors affecting the resilient performance of QBZU were investigated, including polymer concentration, organosilicon concentration and the types of surfactant. Based on the fracturing pressure curve and microseismic monitoring results, the plugging and fracture diversion effectiveness was further confirmed.

The Effects of Organically Modified Lithium Magnesium Silicate on the Rheological Properties of Water-Based Drilling Fluids.

To address the problem of insufficient temperature and salt resistance of existing polymer viscosity enhancers, we designed an organic-inorganic hybrid composite as a viscosity enhancer for water-based drilling fluids, named LAZ, and it was prepared by combining a water-soluble monomer and lithium magnesium silicate (LMS) using an intercalation polymerization method. The composite LAZ was characterized using Fourier transform infrared spectroscopy, transformed target X-ray diffractometry, scanning electron microscopy, and thermogravimetric analysis. The rheological properties of the composite LAZ were evaluated. The composite LAZ was used as a water-based drilling fluid viscosity enhancer, and the temperature and salt resistance of the drilling fluid were evaluated. The results showed that the composite LAZ presented a complex reticulation structure in an aqueous solution. This reticulation structure intertwined with each other exhibited viscosity-enhancing properties, which can enhance the suspension properties of water-based drilling fluids. The aqueous solution of the composite LAZ has shear dilution properties. As shear rate increases, shear stress becomes larger. The yield stress value of the aqueous solution increases as the composite LAZ's concentration increases. The aqueous solution of the composite LAZ exhibits strong elastic characteristics with weak gel properties. The addition of the composite LAZ to 4% sodium bentonite-based slurry significantly increased the apparent viscosity and dynamic shear of the drilling fluid. The drilling fluids containing the composite LAZ had good temperature resistance at 150 °C and below. The rheological properties of brine drilling fluids containing the composite LAZ changed slightly before and after high-temperature aging at 150 °C.

Gelatin methacrylate based liquid dressing with antibacterial and hemostasis properties

For incompressible and irregularly shaped wounds, developing a novel dressing based on photo-crosslinked hydrogel that has both hemostasis and antibacterial functions is highly desirable. In this study, photoreactive substrate gelatin methacrylate (GelMA) and Poly (ethylene glycol) diacrylate (PEGDA) were combined with water-soluble quaternary ammonium antibacterial monomers (DMC). Interestingly, they can quickly change from liquid to hydrogel under visible light at 405 nm within 1 min, which is suitable for small incompressible wounds. Regarding the biosafety of the dressing, cell viability and blood viability test indicated that the GelMA/PEGDA/DMC3 dressing has no cytotoxicity toward L929 cells and red blood cells. The antibacterial performance test proved that the addition of DMC significantly improved the antibacterial performance of the dressing. Moreover, the GelMA/PEGDA/DMC3 dressing showed rapid hemostasis ability in tail clipping hemostasis test and liver hemostasis test. Taken together, this new type of convenient hydrogel dressing exhibits great potential as a quick hemostasis and antibacterial wound dressing candidate for small bleeding wounds.

Green Method for the Preparation of Durable Superhydrophobic Antimicrobial Polyester Fabrics with Micro-Pleated Structures.

To produce functional protective textiles with minimal environmental footprints, we developed durable superhydrophobic antimicrobial textiles. These textiles are characterized by a micro-pleated structure on polyester fiber surfaces, achieved through a novel plasma impregnation crosslinking process. This process involved the use of water as the dispersion medium, water-soluble nanosilver monomers for antimicrobial efficacy, fluorine-free polydimethylsiloxane (PDMS) for hydrophobicity, and polyester (PET) fabric as the base material. The altered surface properties of these fabrics were extensively analyzed using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectrometry (XPS), thermogravimetric analysis (TGA), and water contact angle (WCA) measurements. The antimicrobial performance of the strains was evaluated using Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus. After treatment, the fabrics exhibited enhanced hydrophobic and antimicrobial properties, which was attributed to the presence of a micro-pleated structure and nanosilver. The modified textiles demonstrated a static WCA of approximately 154° and an impressive 99.99% inhibition rate against both test microbes. Notably, the WCA remained above 140° even after 500 washing cycles or 3000 friction cycles.

Microfluidic fabrication of monodisperse microcapsules with gas cores.

A facile strategy for efficient and continuous fabrication of monodisperse gas-core microcapsules with controllable sizes and excellent ultrasound-induced burst performances is developed based on droplet microfluidics and interfacial polymerization. Monodisperse gas-in-oil-in-water (G/O/W) double emulsion droplets with a gas core and monomer-contained oil layer are fabricated in the upstream of a microfluidic device as templates, and then water-soluble monomers are added into the aqueous continuous phase in the downstream to initiate rapid interfacial polymerization at the O/W interfaces to prepare monodisperse gas-in-oil-in-solid (G/O/S) microcapsules with gas cores. The sizes of both microbubbles and G/O/W droplet templates can be precisely controlled by adjusting the gas supply pressure and the fluid flow rates. Due to the very thin shells of G/O/S microcapsules fabricated via interfacial polymerization, the sizes of the resultant G/O/S microcapsules are almost the same as those of the G/O/W droplet templates, and the microcapsules exhibit excellent deformable properties and ultrasound-induced burst performances. The proposed strategy provides a facile and efficient route for controllably and continuously fabricating monodisperse microcapsules with gas cores, which are highly desired for biomedical applications.

Adsorption of Congo Red by chitosan porous beads reinforced with epoxy resin

This study prepared epoxy resin reinforced porous beads (CERBs) by crosslinking a water-soluble epoxy monomer, 1,4-butanediol diglycidyl ether (BDE), with chitosan (CS) using isophorone diamine (IPD) as a crosslinking agent.

Omics-Based Investigation on Mechanisms Controlling Cellular Internalization of Keratin Monomers during Biodegradation by Stenotrophomonas maltophilia DHHJ

Introduction: The global poultry industry produces millions of tons of waste feathers every year, which can be bio-degraded to make feed, fertilizer, and daily chemicals. However, feather bio-degradation is a complex process that is not yet fully understood. This results in low degradation efficiency and difficulty in industrial applications. Omics-driven system biology research offers an effective solution to quickly and comprehensively understand the molecularmechanisms involved in a metabolic pathway. Methods: In the early stage of this process, feathers are hydrolyzed into water-soluble keratin monomers. In this study, we used high-throughput RNA-seq technology to analyze the genes involved in the internalization and degradation of keratin monomers in Stenotrophomonas maltophilia DHHJ strain cells. Moreover, we used Co-IP with LC-MS/MS technology to search for proteins that interact with recombinant keratin monomers. Results: We discovered TonB transports and molecular chaperones associating with the keratin monomer, which may play a crucial role in the transmembrane transport of keratin. Meanwhile, multiple proteases belonging to distinct families were identified as binding partners of keratin monomers, among which ATPases associated with diverse cellular activity (AAA+) family proteases are overrepresented. Four genes, including JJL50_15620, JJL50_17955 (TonB-dependent receptors), JJL50_03260 (ABC transporter ATP-binding protein), and JJL50_20035 (ABC transporter substrate-binding protein), were selected as representatives for determining their expressions under different culture conditions using qRT-PCR, and they were found to be upregulated in response to keratin degradation consistent with the data from RNA-seq and Co-IP. Conclusion: This study highlights the complexity of keratin biodegradation in S. maltophilia DHHJ, in which multiple pathways are involved such as protein folding, protein transport, and several protease systems. Our findings provide new insights into the mechanism of feather degradation.

Acrylate–methacrylate radical copolymerization kinetics of sparingly water-soluble monomers in polar and nonpolar solvents

The influence of solvent on radical copolymerization kinetics is studied to provide insight to emulsion polymerization systems.

Aqueous Sol-Gel Synthesis and Shaping of Covalent Organic Frameworks.

The intrinsic fragility and insoluble nature of covalent organic frameworks (COFs) have strongly impeded their processability for practical applications. Herein, an aqueous-based sol-gel synthetic strategy is reported for the synthesis and shaping of COFs with task-specific applications that satisfy the principles of green chemistry for gram-scale production of crystalline materials. Our successful approach involves three pivotal aspects: the "prodrug mimic" design of water-soluble monomers, the utilization of hydrolyzable bonds, and the manipulation of reaction kinetics. The generality of the method is demonstrated by the successful preparation of representative high-surface area two-dimensional (2D) COFs with several commonly used amines. By virtue of this strategy, a COF colloidal dispersion is achieved and can be formulated into processable fluids, structured films, and COF monoliths. Remarkably, the obtained lightweight (∼0.020 g cm-3) and robust aerogels displayed outstanding adsorption capacity (exceeding 57 times its own weight) toward a variety of organic solvents and exhibited superior thermal insulating properties compared to the widely used sponge and cotton. This work demonstrates a versatile strategy for the synthesis and shaping of processable COF materials in water that will contribute to the development of COF monoliths for advanced applications.

Efficient formation of poly(ethylene glycol) polymer brushes on gold electrodes via surface-initiated electrochemically mediated ATRP (SI-eATRP)

Electrochemically mediated surface-initiated atom transfer radical polymerization (SI-eATRP) is an interesting grafting from technique used to grow, in a controlled way, polymeric films from a wide range of surfaces, including metal substrates. Aqueous SI-eATRP offers an appealing strategy for the preparation of polymers by using water-soluble monomers, employing an oxidatively stable catalyst complex. The goal of this work is to tailor compact poly-(oligo(ethylene glycol)methacrylate) (p-OEGMA) brushes on gold electrodes by combining the formation of self-assembled monolayers (SAMs) containing a suitable ATRP initiator molecule, and the SI-eATRP polymerization approach. We have investigated the effects of the SAM-initiator nature, the applied potential, and the duration of the polymerization process on the properties of the grafted p-OEGMA-brushes. In addition, we employed electrochemical quartz crystal microbalance measurements to evidence the living character of the polymerization. The final properties of the tailored p-OEGMA-brush were studied by cyclic voltammetry and electrochemical impedance spectroscopy, obtaining information on the electronic and ionic blocking behaviour of these films, under different experimental conditions. Further information on structural conformation, composition, and organization was obtained from different characterization techniques: IRRAS and XPS spectroscopies, contact angle measurements, and SEM and AFM microscopies. These techniques confirmed that an efficient formation of p-OEGMA-brushes via SI-eATRP was achieved. Thus, the designed SI-eATRP system offers an interesting option to functionalize a wide variety of substrates with water-soluble and biocompatible monomers. Such coatings present potential applications in various fields, including biomedical applications.