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The advancement of non‐fullerene acceptors with crescent‐shaped geometry has led to the need for polymer donor improvements. Additionally, there is potential to enhance the photovoltaic parameters in high‐efficiency organic solar cells (OSCs). The random copolymerization method is a straightforward and effective strategy to further optimize photoactive morphology and enhance device performance. However, finding a suitable third component in terpolymers remains a crucial challenge. In this study, a series of terpolymer donors (PTF3, PTF5, PTF10, PTF20, and PTF50) is synthesized by introducing varying amounts of the trifluoromethyl‐substituted unit (CF3) into the PM6 polymer backbone. Even subtle changes in the CF3 content can significantly enhance all the photovoltaic parameters due to the optimized energy levels, molecular aggregation/miscibility, and bulk‐heterojunction morphology of the photoactive materials. Thus, the best binary OSC based on the PTF5:Y6‐BO achieves an outstanding power conversion efficiency (PCE) of 18.2% in the unit cell and a PCE of 11.6% in the sub‐module device (aperture size: 54.45 cm2), when using halogen‐free solvent o‐xylene. This work showcases the remarkable potential of the easily accessible CF3 unit as a key constituent in the construction of terpolymer donors in high‐performance OSCs. A series of random terpolymers is developed by incorporating readily accessible trifluoromethyl‐substituted benzene (TFB) units into the PM6 donor polymer. Incorporation of the TFB unit leads to optimal molecular packing and desirable aggregation/miscibility morphology in halogen‐free solvents, resulting in substantial efficiencies of 18.2% and 11.6% in the unit cell and sub‐module devices.

Advanced electrode materials that combine large surface area, adjustable porosity, and redox activity are essential to meet the growing need for greener and efficient energy storage devices. Since, conventional carbon-based materials frequently don’t provide the redox activity and adaptability that are required for high performance supercapacitor, researchers started to use various materials as replacement. One of the remarkable options is the use of porous organic polymers (POPs) as the electrode materials for supercapacitors. There have been many POPs reported till now; however, the majority of reported synthesis required suitable organic solvents as a synthesis medium, which is often a time-consuming and potentially hazardous process. Thus, the solvent-free synthesis of POPs for supercapacitor application is important but still in its infancy. By considering these points, this research deals with solvent-free synthesis of triazine-based porous organic polymer (T-POP) with a good yield and lower reaction time, in contrast to typical synthetic methods that utilize harsh conditions. The resultant T-POP has a specific surface area of 33.91 m−2 g−1, a micro-/mesoporous architecture that is hierarchical, and a large number of nitrogen functionalities that are redox active. These characteristics allow for effective charge storage by combining pseudocapacitive and electric double-layer processes. The T-POP exhibits a high specific capacitance of 3703 μF cm−2 at 0.01 mA cm−2, when used as a supercapacitor electrode. In addition to presenting a solvent-free method for creating high-performance porous polymers, this study emphasises POPs’ promise as next-generation materials for effective and sustainable energy storage applications.

Solvent-free microwave extraction (SFME) is a combination of microwave heating and dry distillation performed at atmospheric pressure without the addition of water or organic solvents that has been proposed as a green method for the extraction of essential oils from aromatic and medicinal herbs. In this work, SFME and the conventional techniques of steam distillation (SD) and hydrodistillation (HD) were compared with respect to the extraction and antioxidant and antimicrobial activities of Thymus mastichina essential oil. The main constituent of essential oils obtained using different methods was 1,8-cineole (eucalyptol). The results showed that the essential oils extracted by means of SFME in 30 min were quantitatively (yield) and qualitatively (aromatic profile) similar to those obtained using conventional HD over 120 min. In addition, SFME generates less waste and less solvent, consumes less energy, and provides a higher yield for a shorter extraction time, which is advantageous for the extraction of the T. mastichina essential oil compared to SD. The antioxidant and antimicrobial activities of the T. mastichina essential oil obtained from either SFME or conventional extraction methods (SD or HD) showed a similar pattern. Large-scale experiments using this SFME procedure showed a potential industrial application.

Chiral supramolecular polymers with stimuli‐responsive circularly polarized luminescence (CPL) are highly desirable for smart flexible optoelectronic devices, but remain rarely reported. Here, a simple solvent‐free supramolecular polymerization for preparing chiral polyurethanes is presented by in situ induced self‐assembly strategy, using cellulose nanocrystals (CNCs)‐based isocyanate prepolymers and macromolecular polyols as precursors, achieving precise control over polymer chain assembly with spot‐like arrangement. More importantly, by further incorporating a π‐conjugated luminescent dihydroxynaphthalene molecule, CPL‐active flexible polyurethane films with feather‐like nanostructures are constructed, which promote the ordered arrangement of CNCs‐based isocyanate segments due to the increased spatial resistance. The π─H bond network between CNCs and urethane‐linked benzene rings drives the self‐assembly, enabling higher‐level chiral amplification and enhanced fluorescence. Interestingly, the prepared chiral fluorescent polyurethanes display multimodal chiroptical stimuli responsiveness under various stimuli, such as temperature, solvent polarity, pH, and polarized light, due to the sensitivity of the π─H bond network. This work offers new insights into designing solvent‐free chiral supramolecular polymers with significant chiroptical potentials. Precise construction of the feather‐like nanostructured chiroptical polyurethanes using cellulose nanocrystals (CNCs)‐based isocyanate prepolymers with fluorescent naphthalene structures and macromolecular polyols as precursors is manifested by solvent‐free supramolecular polymerization. Furthermore, the sensitivity of the π─H bond network to various stimuli, including temperature, solvent polarity, pH, and polarized light, is applied to realize multimodal chiroptical stimuli responsiveness.

Solvent-free preparation types for cyclodextrin complexation, such as co-grinding, are technologies desired by the industry. However, in-depth analytical evaluation of the process and detailed characterization of intermediate states of the complexes are still lacking in areas. In our work, we aimed to apply the co-grinding technology and characterize the process. Fenofibrate was used as a model drug and dimethyl-β-cyclodextrin as a complexation excipient. The physical mixture of the two substances was ground for 60 min; meanwhile, samples were taken. A solvent product of the same composition was also prepared. The intermediate samples and the final products were characterized with instrumental analytical tools. The XRPD measurements showed a decrease in the crystallinity of the drug and the DSC results showed the appearance of a new crystal form. Correlation analysis of FTIR spectra suggests a three-step complexation process. In vitro dissolution studies were performed to compare the dissolution properties of the pure drug to the products. Using a solvent-free production method, we succeeded in producing a two-component system with superior solubility properties compared to both the active ingredient and the product prepared by the solvent method. The intermolecular description of complexation was achieved with a detailed analysis of FTIR spectra.

Copper(II)/polyimide‐linked covalent organic frameworks under solvent‐free and microwave‐assisted conditions have been used in an efficient one‐pot protocol for the preparation of 2,4,5‐trisubstituted imidazoles via benzil, aromatic aldehydes and ammonium acetate. By applying solvent‐free conditions and microwave irradiation, three‐component condensation provides safe operations, low pollution, quick access to products, and an easy set‐up. As a result of its reusability, the catalyst can also be reutilized for many runs without missing any activity.

Solvent‐free manufacturing is crucial for fabricating high‐performance sulfide‐electrolyte‐based all‐solid‐state lithium batteries (ASSLBs), with advantages including side reaction inhibition, less contamination, and practical scalability. However, the fabricated sulfide electrolytes commonly suffer from brittleness, limited ion transport, and unsatisfactory interfacial stability due to the uncontrolled dispersion of the sulfide particles within the polymer binder matrix. Herein, a “solid‐to‐liquid” phase transition strategy is reported to fabricate flexible Li6PS5Cl (LPSCl) electrolytes. The polycaprolactone (PCL)‐based binder (PLI) with phase‐transition characteristics fills the gap of LPSCl particles and tightly grafts on the particle surface via ion‐dipole interaction, bringing a thin and compact electrolyte membrane (80 µm). The simultaneously high Li‐ion conducting and electron insulating nature of PLI binder facilitates Li‐ion transport and ensures good interfacial stability between electrolyte and anode. Consequently, the sulfide electrolyte membrane exhibits high ionic conductivity (8.5 × 10−4 S cm−1), enabling symmetric and full cells with 10 and 2.5 times longer cycling life compared with that of the cells with pristine LPSCl electrolyte, respectively. The demonstrated strategy is versatile and can be extended to ethylene vinyl acetate copolymer (EVA) that also brings enhanced electrochemical performance. The thin sulfide electrolyte with high interfacial stability potentially facilitates dendrite‐free ASSLBs with high energy density. The versatile “solid‐to‐liquid” phase transition strategy is proposed to fabricate thickness‐confined and structurally robust sulfide electrolyte membranes via a dry‐film process. The “liquid” polycaprolactone‐based Li‐conducting binder (PLI) fills the gap of sulfide electrolyte particles and tightly grafts on the particle surface via ion‐dipole interaction, bringing a compact electrolyte membrane with excellent ion transport capability and favorable interfacial compatibility.

Molecular aggregation affects the electronic interactions between molecules and has emerged as a powerful tool in material science. Aggregate effect finds wide applications in the research of new physical phenomena; however, its value for chemical reaction development has been far less explored. Herein, we report the development of aggregation‐enabled alkene insertion into carbon–halogen bonds. The spontaneous cleavage of C–X (X = Cl, Br, or I) bonds generates an intimate ion pair, which can be quickly captured by alkenes in an aggregated state. Additional catalysts or promoters are not necessary under such circumstances, and solvent quenching experiments indicate that the aggregated state is critical for achieving such sequences. The ionic insertion mode is supported by mechanistic studies, density functional theory calculations, and symmetry‐adapted perturbation theory analysis. Results also show that the non‐aggregated state may quench the transition state and terminate the insertion process.

In recent years, almost all extraction processes in the perfume, cosmetic, pharmaceutical, food ingredients, nutraceuticals, biofuel and fine chemical industries rely massively on solvents, the majority of which have petroleum origins. The intricate processing steps involved in the industrial extraction cycle makes it increasingly difficult to predict the overall environmental impact; despite the tremendous energy consumption and the substantial usage of solvents, often the yields are indicated in decimals. The ideal alternative solvents suitable for green extraction should have high solvency, high flash points with low toxicity and low environmental impacts, be easily biodegradable, obtained from renewable (non-petrochemical) resources at a reasonable price and should be easy to recycle without any deleterious effect to the environment. Finding the perfect solvent that meets all the aforementioned requirements is a challenging task, thus the decision for the optimum solvent will always be a compromise depending on the process, the plant and the target molecules. The objective of this comprehensive review is to furnish a vivid picture of current knowledge on alternative, green solvents used in laboratories and industries alike for the extraction of natural products focusing on original methods, innovation, protocols, and development of safe products.

Goals of high efficiency, morphological analysis, and the ability to produce organic solar cell (OSC) sub‐modules using halogen‐free solvents are demanding. In this study, a robust conjugated polymer with thienothiophene π‐spacer with pendant alkyl side chain (NapBDT‐C12) was synthesized and used to fabricate sub‐modules. Excellent efficiencies were demonstrated by a NapBDT‐C12 integrated ternary blend, which was used to produce stable small‐area‐to‐sub‐module devices using O‐xylene. The efficiency of the NapBDT‐C12 added small‐area ternary devices (PM6:NapBDT‐C12:L8‐BO) was 18.71%. Owing to the controlled homogeneity of the blend with favorable nanoscale film morphology, enhanced carrier mobilities, and exciton dissociation/splitting properties, contributed to the efficiencies of small‐area‐to‐sub‐module OSCs. Moreover, a 55 cm2 sub‐module with an efficiency of 14.69% was accomplished by bar coating using O‐xylene under ambient conditions. This study displays the potential of a ternary blend based OSC device to produce high efficiency scalable sub‐modules at ambient conditions. A remarkable PCE of 14.69% was achieved by enhancing the morphology of air‐processed sub‐modules (55 cm2) fabricated using halogen‐free solvents (O‐xylene). This performance was achieved by regulating surface morphology, intra‐ and intermolecular interactions, and film optimal aggregation.