Search Results (90)

Slurry-cast (SLC) electrode manufacturing faces problems such as thickness limitation and material stratification, which are caused by applying toxic organic solvents. Solvent-free electrode technology, as a sustainable alternative, could get rid of issues generated by solvents. In this study, dual-layer NCM811 solvent-free electrodes (DLEs) are fabricated via an electrostatic powder deposition method with an active material-rich upper layer to provide high energy output, while the more binder–conductor content base layer improves conductivity and contact with current collectors. The dual-layered structure overwhelms the single-layer electrode (SE) with stable cycling performance caused by more regulated pore structures. DLE maintains 74% capacity retention after 100 cycles at 0.3 C, while the SLC shows only 60% capacity retention. Additionally, DLE shows excellent rate performance at various rates, with 207.3 mAh g⁻¹, 193.9 mAh g⁻¹, 173.9 mAh g⁻¹, 157.3 mAh g⁻¹, and 120.4 mAh g⁻¹ at 0.1 C, 0.2 C, 0.5 C, 1.0 C, and 2.0 C, respectively. The well-designed DLE cathodes exhibit superior discharge-specific capacities, rate performance, and improved cycling stability than traditional SLC cathodes. It enlightens the path toward new structure innovations of solvent-free electrodes. Full article

Polybenzimidazole (PBI), a high-performance polymer known for its exceptional thermal stability and chemical resistance, was processed by solution electrospinning to manufacture fibrous non-woven membranes. The process was repeated under different conditions by adjusting four main settings: the polymer solution concentration, the flow rate, the voltage applied between the needle and the collector, and the separating distance. To clarify the interplay between process parameters and material properties, a Design of Experiment (DOE) approach was used to systematically analyze the effects of said parameters on microstructural properties, including fiber diameter, porosity, and air permeability, pointing out that the increase in viscosity improves fiber uniformity, while optimizing the applied voltage and the needle–collector distance enhances jet stability and solvent evaporation, crucial for defect-free fibrous microstructures. Post-processing via calendering further refined the membrane texture and properties, for example by reducing porosity and air permeability without significantly altering the fibrous morphology, particularly at low lamination ratios. Thermal and mechanical evaluations highlighted that the obtained electrospun PBI membranes exhibited enhanced flexibility, but lower tensile strength compared to cast films due to the underlying open pore microstructure. This integrated approach—combining experimental characterization, DOE-guided optimization, and post-processing via calendering—provides a systematic framework for tailoring PBI membranes for specific applications, such as filtration, fuel cells, and molecular sieving. The findings highlight the potential of PBI-based electrospun membranes as versatile materials, offering high thermal stability, chemical resistance, and tunable properties, thereby establishing a foundation for further innovation in advanced polymeric membrane design and applications for energy and sustainability. Full article

This study presents a green and solvent-free methodology based on thermal desorption coupled to gas chromatography-mass spectrometry (TD-GC-MS) to characterise cork’s volatile aromatic (VOC) profile. Samples from three geographical origins—Catalonia, Extremadura, and Sardinia—were analysed at different extraction temperatures. Cork stoppers from Sardinia were also analysed after two washing procedures (immersion and spray) and thermal treatment. The results showed that temperature and geographical origin significantly influenced the quantity and intensity of extracted VOCs, with higher extraction temperatures yielding a more comprehensive volatile profile. Vanillin was the most abundant compound in all samples. A multivariate analysis showed that cork from Extremadura was associated with carboxylic acids, Catalonia with furan derivatives and sugar-related compounds, and Sardinia with phenolic compounds linked to lignin degradation. Immersion-washed stoppers retained more lignin-derived and phenolic compounds, while spray-washed samples were characterised by a higher alkane content. Thermal treatment notably altered the VOC profile, increasing ketones such as acetophenone and 2-nonadecanone and reducing alkanes and fatty acids. These findings highlight the influence of the geographical origin and manufacturing process on the aromatic composition of cork, with potential applications in industries seeking natural active compounds. Full article

Polyphenylene sulfide (PPS)-based separators have garnered significant attention as high-performance components for next-generation lithium-ion batteries (LIBs), driven by their exceptional thermal stability (>260 °C), chemical inertness, and mechanical durability. This review comprehensively examines advances in PPS separator design, focusing on two structurally distinct categories: porous separators engineered via wet-chemical methods (e.g., melt-blown spinning, electrospinning, thermally induced phase separation) and nonporous solid-state separators fabricated through solvent-free dry-film processes. Porous variants, typified by submicron pore architectures (<1 μm), enable electrolyte-mediated ion transport with ionic conductivities up to >1 mS·cm⁻¹ at >55% porosity, while their nonporous counterparts leverage crystalline sulfur-atom alignment and trace electrolyte infiltration to establish solid–liquid biphasic conduction pathways, achieving ion transference numbers >0.8 and homogenized lithium flux. Dry-processed solid-state PPS separators demonstrate unparalleled thermal dimensional stability (<2% shrinkage at 280 °C) and mitigate dendrite propagation through uniform electric field distribution, as evidenced by COMSOL simulations showing stable Li deposition under Cu particle contamination. Despite these advancements, challenges persist in reconciling thickness constraints (<25 μm) with mechanical robustness, scaling solvent-free manufacturing, and reducing costs. Innovations in ultra-thin formats (<20 μm) with self-healing polymer networks, coupled with compatibility extensions to sodium/zinc-ion systems, are identified as critical pathways for advancing PPS separators. By addressing these challenges, PPS-based architectures hold transformative potential for enabling high-energy-density (>500 Wh·kg⁻¹), intrinsically safe energy storage systems, particularly in applications demanding extreme operational reliability such as electric vehicles and grid-scale storage. Full article

Objectives: Hot-melt extrusion (HME) offers a solvent-free, scalable approach for manufacturing pharmaceutical co-crystals (CCs), aligning with the industry’s shift to continuous manufacturing (CM). However, challenges like undefined yield optimization, insufficient risk management, and limited process analytical technology (PAT) integration hinder its industrial application. This study aimed to develop a proof-of-concept HME platform for CCs, assess process risks, and evaluate PAT-enabled monitoring to facilitate robust production. Methods: Using carbamazepine (CBZ) and nicotinamide (NIC) as model compounds, an HME platform compatible with PAT tools was established. A systematic risk assessment identified five key risk domains: materials, machinery, measurement, methods, and other factors. A Box–Behnken design of experiments (DoE) evaluated the impact of screw speed, temperature, and mixing sections on CC quality. Near-infrared (NIR) spectroscopy monitored CBZ-NIC co-crystal formation in real time during HME process. Results: DoE revealed temperature and number of mixing sections significantly influenced particle size (D₅₀: 2.0–4.0 μm), while screw speed affected efficiency. NIR spectroscopy detected a unique CC absorption peak at 5008.3 cm⁻¹, enabling real-time structural monitoring with high accuracy (R² = 0.9999). Risk assessment highlighted material attributes, process parameters, and equipment design as critical factors affecting CC formation. All experimental batches yielded ≥ 94% pure CCs with no residual starting materials, demonstrating process reproducibility and robustness. Conclusions: Overall, this work successfully established a continuous hot-melt extrusion (HME) process for manufacturing CBZ-NIC co-crystals, offering critical insights into material, equipment, and process parameters while implementing robust in-line NIR monitoring for real-time quality control. Additionally, this work provides interpretable insights and serves as a basis for future machine learning (ML)-driven studies. Full article

Wood, a vital material for both modern and heritage objects, is particularly susceptible to degradation caused by water due to its hydrophilic nature and porous structure. Therefore, developing sustainable strategies to protect wood is of significant importance. This study aims to produce a highly hydrophobic coating for the protection of wood following a straightforward procedure and using materials that are compatible with wood. First, nano/sub-microlignin (NL) is isolated and produced from beech wood through a one-step tailored organosolv process. Next, NL is incorporated into Sivo 121, a water-borne and solvent-free silane system recommended by the manufacturer for protecting wood surfaces. Composite coatings containing various concentrations of NL and Sivo 121 are applied to chestnut (Castanea spp.) and oak (Quercus spp.). The impact of NL concentration on the contact angles of water drops (CAs) and colour changes (ΔE) of the treated wood specimens is investigated. The coating with 4% w/w NL demonstrates enhanced hydrophobicity (CA = 145°) and has a negligible effect on the colour of pristine oak (ΔE < 3). The wetting properties of coated oak are not affected after 100 tape peeling cycles. However, the coating exhibits poorer performance on chestnut, i.e., CA = 135°, which declines after 80 peeling cycles, and ΔE > 5. The drop pH does not have any noticeable effect on CA. The latter remains stable even after prolonged exposure of coated oak and chestnut samples to artificial UV radiation and outdoor environmental conditions. Finally, the composite coating offers good and comparable protection for both wood species in the biological durability soil burial test Full article

Background/Objectives: The oral delivery of large-molecule drugs remains challenging due to poor solubility, perdemeability, and stability in the gastrointestinal tract, resulting in low bioavailability. In this study, hot melt extrusion (HME) was investigated as a solvent-free manufacturing technique for mucoadhesive bilayer films to improve drug absorption. Methods: Polyvinyl alcohol (PVA) and polyethylene oxide (PEO) were evaluated as mucoadhesive film-forming polymers, in conjunction with Eudragit^® RS as a water-insoluble backing layer. Paracetamol and lactase were utilized as small and large molecule APIs, respectively. The resulting films were assembled into bilayer film samples and examined for mechanical properties, mucoadhesion, and dissolution behavior. A novel dissolution model was developed to evaluate unidirectional drug transport. Results: The results showed that bilayer films could be successfully fabricated using HME, with different mechanical properties depending on the polymer and drug content. Tests with the newly developed dissolution model showed a unidirectional drug release. The model also confirmed the need for biorelevant dissolution test systems because of a better differentiation between polymers compared to standard test methods such as the paddle-over-disk method. Furthermore, the investigation revealed that the activity of enzymes was retained after extrusion, thus indicating the feasibility of processing biologics. Conclusions: This study highlights the potential of HME to produce bilayer films as an innovative drug delivery platform offering improved bioavailability for both small and large molecules. Full article

Natural deep eutectic solvents (NADESs) are a sustainable, green option for extraction and reaction media in biorefineries and various chemical and biotechnological applications. Particularly, enzymatic reactions profit from NADES applications, as these solvents help to maintain high substrate solubility while improving both enzyme stability and efficiency. Recent studies confirmed that NADESs can perform multiple functions simultaneously, as reaction media for biocatalytic conversions, but also as substrates and catalysts for reactions, fulfilling the role of a reactive solvent. This study reports the beneficial effect of designed reactive natural deep eutectic solvents (R-NADESs) on the esterification activity and thermal stability of free and immobilized lipases in the synthesis of polyol- and carbohydrate-based biosurfactants. We manufactured and characterized 16 binary and ternary R-NADES systems with choline chloride (ChCl) as the hydrogen bond acceptor (HBA) and carbohydrate polyols; mono-, di-, and oligosaccharides; urea (U); N-methyl urea (MU); and water as the hydrogen bond donors (HBDs), in different combinations and molar ratios, most of which are reported for the first time in this paper. We determined their physicochemical, thermal, and molecular properties, including among others viscosity, polarizability, and the number of hydrogen bonds, and we showed that these properties are controlled by composition, molar ratio, molecular properties, temperature, and water content. Many lipases, both native and immobilized, showed high stability and remarkable catalytic performance in R-NADESs during esterification reactions. Full article

Developing efficient anti-microbials for thoroughly addressing Salmonella contamination is essential for the improvement of food safety. Phage-built materials have shown great potential for biocontrol in environments. Due to challenges in delivery and stability, their widespread use has remained unattainable. Here, we have developed a honeycomb film template-based method for the high-throughput preparation of phage microgels. The honeycomb film template can be simply fabricated in a humid chamber based on a well-established breath figure method. The bacteriophage microgels can be further manufactured by dropping a pre-gelation solution containing bacteriophages into a honeycomb film template. This method can produce over 210,000 phage microgels in every square centimeter template with each microgel containing 1.04 × 10⁷ phages. They can kill 99.90% of the contaminated S. typhimurium 14,028 on chicken samples. This simple, heat-free, and solvent-free method can maintain the strong anti-bacterial efficiency of phages, which can expand the wide application of phage-built microgels for food decontamination. Full article

Solid-state electrolytes (SSEs), particularly garnet-type Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO), offer high stability and a wide electrochemical window. However, their grain boundaries limit ionic conductivity, necessitating high-temperature sintering for improved performance. Yet, this process results in brittle electrolytes prone to fracture during manufacturing. To address these difficulties, solvent-free solid-state electrolytes with a polyacrylonitrile (PAN) coating on LLZTO particles are reported in this work. Most notably, the PAN-coated LLZTO (PAN@LLZTO) electrolyte demonstrates self-supporting characteristics, eliminating the need for high-temperature sintering. Importantly, the homogeneous polymeric PAN coating, synthesized via the described method, facilitates efficient Li⁺ transport between LLZTO particles. This electrolyte not only achieves an ionic conductivity of up to 2.11 × 10⁻³ S cm⁻¹ but also exhibits excellent interfacial compatibility with lithium. Furthermore, a lithium metal battery incorporating 3% PAN@LLZTO-3%PTFE as the solid-state electrolyte and LiFePO₄ as the cathode demonstrates a remarkable specific discharge capacity of 169 mAh g⁻¹ at 0.1 °C. The strategy of organic polymer-coated LLZTO provides the possibility of a green manufacturing process for preparing room-temperature sinter-free solid-state electrolytes, which shows significant cost-effectiveness. Full article

The improvement of the mucosal sealing around the implant represents a challenge, one that prompted research into novel materials. To this purpose, a printable poly(ε-caprolactone) (PCL)-based composite loaded with alumina-toughened zirconia (ATZ) at increasing rates of 10, 20, and 40 wt.% was prepared, using a solvent casting method with chloroform. Disks were produced by 3D printing; surface roughness, free energy and optical contact angle were measured. Oral fibroblasts (PF) and epithelial cell (SG) tests were utilized to determine the biocompatibility of the materials through cell viability assay and adhesion and spreading evaluations. The highest level of ATZ resulted in an increase in the average roughness (S_a), while the maximum height (S_z) was higher for all composites than that of the unmixed PCL, regardless of their ATZ content. Surface free energy was significantly lower on PCL/ATZ 80/20 and PCL/ATZ 60/40, compared to PCL and PCL/ATZ 90/10. The contact angle was inversely related to the quantity of ATZ in the material. PF grew without variations among the different specimens at 1 and 3 days. After 7 days, PF grew significantly less on PCL/ATZ 60/40 and PCL/ATZ 80/20 compared to unmixed PCL and PCL 90/10. Conversely, ATZ affected and improved the growth of SG. By increasing the filler amount, PF cell adhesion and spreading augmented, while PCL/ATZ 80/20 was the best for SG adhesion. Overall, PCL/ATZ 80/20 emerged as the best composite for both cell types; hence, it is a promising candidate for the manufacture of custom made transmucosal dental implant components. Full article

Pig processing industries have produced large quantities of by-products, which have either been discarded or used to make low-value products. This study aimed to provide recommendations for manufacturing edible oil from pig brains, thereby increasing the value of pork by-products. The experiment compared non-solvent extraction methods, specifically wet rendering and aqueous saline, to a standard solvent extraction method, the Bligh and Dyer method, for extracting oil from pig brains. The yield, color, fatty acid profile, a number of lipid classes, and lipid stability against lipolysis and oxidation of the pig brain oil were comprehensively compared, and the results revealed that these parameters varied depending on the extraction method. The wet rendering process provided the highest extracted oil yield (~13%), followed by the Bligh and Dyer method (~7%) and the aqueous saline method (~2.5%). The Bligh and Dyer method and wet rendering techniques produced a translucent yellow oil; however, an opaque light-brown-red oil was found in the aqueous saline method. The Bligh and Dyer method yielded the oil with the highest phospholipid, cholesterol, carotenoid, tocopherol, and free fatty acid contents (p < 0.05). Although the Bligh and Dyer method recovered the most unsaturated fatty acids, it also recovered more trans-fatty acids. Aqueous saline and wet rendering procedures yielded oil with low FFA levels (<1 g/100 g). The PV of the oil extracted using all methods was <1 meq/kg; however, the Bligh and Dyer method had a significant TBARS content (7.85 mg MDA equivalent/kg) compared to aqueous saline (1.75 mg MDA equivalent/kg) and wet rendering (1.14 mg MDA equivalent/kg) (p < 0.05). FTIR spectra of the pig brain oil revealed the presence of multiple components in varying quantities, as determined by chemical analysis experiments. Given the higher yield and lipid stability and the lower cholesterol and trans-fatty acid content, wet rendering can be regarded as a simple and environmentally friendly method for safely extracting quality edible oil from pig brains, which may play an important role in obtaining financial benefits, nutrition, the zero-waste approach, and increasing the utilization of by-products in the meat industry. Full article

In recent years, solid dosage forms have gained interest in pediatric therapy because they can provide valuable benefits in terms of dose accuracy and stability. Particularly for orodispersible films (ODFs), the literature evidences increased acceptability and dose flexibility. Among the various available technologies for obtaining ODFs, such as solvent casting, hot-melt extrusion, and ink printing technologies, the solvent-free preparation methods exhibit significant advantages. This study investigated Vacuum Compression Molding (VCM) as a solvent-free manufacturing method for the preparation of flexible-dose pediatric orodispersible films. The experimental approach focused on selecting the appropriate plasticizer and ratios of the active pharmaceutical ingredient, diclofenac sodium, followed by the study of their impacts on the mechanical properties, disintegration time, and drug release profile of the ODFs. Additional investigations were performed to obtain insights regarding the solid-state properties. The ODFs obtained by VCM displayed adequate quality in terms of their critical characteristics. Therefore, this proof-of-concept study shows how VCM could be utilized as a standalone method for the production of small-scale ODFs, enabling the customization of doses to meet the individual needs of pediatric patients. Full article

The exposure of workers to propylene glycol monomethyl ether acetate (PGMEA) in manufacturing environments can result in potential health risks. Therefore, systems for PGMEA removal are required for indoor air quality control. In this study, core–shell zeolite socony mobil-5 (ZSM-5)/polyvinylpyrrolidone–polyvinylidene fluoride nanofibers were directly electrospun and partially wet-etched on a mesh substrate to develop a cover-free compact PGMEA air filter. The electrospinning behaviors of the core–shell nanofibers were investigated to optimize the electrospinning time and humidity and to enable the manufacture of thin and light air-filter layers. The partial wet etching of the nanofibers was undertaken using different etching solvents and times to ensure the exposure of the active sites of ZSM-5. The performances of the ZSM-5/PVDF nanofiber air filters were assessed by measuring five consecutive PGMEA adsorption–desorption cycles at different desorption temperatures. The synthesized material remained stable upon repeated adsorption–desorption cycles and could be regenerated at a low desorption temperature (80 °C), demonstrating a consistent adsorption performance upon prolonged adsorption–desorption cycling and low energy consumption during regeneration. The results of this study provide new insights into the design of industrial air filters using functional ceramic/polymer nanofibers and the application of these filters. Full article

The binder ratio in a commercial lithium-ion battery is very low, but it is one of the key materials affecting the battery’s performance. In this paper, polycarbonate-based polymers with liner or chain extension structures are proposed as binders. Then, dry LiFePO₄ (LFP) electrodes with these binders are prepared using the solvent-free method. Polycarbonate-based polymers have a high tensile strength and a satisfactory bonding strength, and the rich polar carbonate groups provide highly ionic conductivity as binders. The batteries with poly (propylene carbonate)-plus (PPC-P) as binders were shown to have a long cycle life (350 cycles under 1 C, 89% of capacity retention). The preparation of dry electrodes using polycarbonate-based polymers can avoid the use of solvents and shorten the process of preparing electrodes. It can also greatly reduce the manufacturing cost of batteries and effectively use industrial waste gas dioxide oxidation. Most importantly, a battery material with this kind of polycarbonate polymer as a binder is easily recycled by simply heating after the battery is discarded. This paper provides a new idea for the industrialization and development of a novel binder. Full article