Chemistry - An Asian Journal最新文献

Recent advancements in supercapacitors (SCs) have sparked significant interest due to their exceptional electrochemical performance, high power density, fast charge–discharge rates, and long cycling life. As renewable energy sources emerge as eco-friendly alternatives to fossil fuels, improving energy storage technologies is crucial for meeting rising electricity demands. This review highlights the role of 2D inorganic nanostructure materials in enhancing SC performance, with a focus on materials like graphene, MXene, metal oxides, phosphides, and transition metal dichalcogenides (TMDs) based on molybdenum and tungsten. In particular, the unique structure of 2D materials offers increased ion accessibility and faster electron transport, which are crucial for improving charge-discharge efficiency and rate capability. The potential of 2D inorganic nanostructures in the design of next-generation supercapacitors, focusing on their ability to optimize energy storage mechanisms, including double-layer capacitance and pseudo-capacitance. It discusses the impact of active mass loading and compares the performance of different SC types, including electrochemical double-layer capacitors, hybrid supercapacitors, and pseudo-capacitors. Emphasis is placed on the synthesis techniques, including sol–gel, hydrothermal, CVD, and electro-polymerization, highlighting their influence on material properties and performance. Finally, comprehensive overview of SC electrode material applications is provided, emphasizing their potential in energy storage systems for sustainable development.

We develop an efficient palladium-catalyzed decarboxylative C─H alkenylation of cyclohexa-2,5-dienyl carboxylic acids with allylic alcohols and N-allyl sulfonamides, enabling regioselective access to diverse vinylarenes. The transformation proceeds under mild, operationally simple conditions and tolerates a broad range of alkyl, aryl, and heteroaryl substituents. Mechanistic studies reveal that the reaction is going via carboxylate-directed C─H activation and olefin insertion step. The method is scalable and offers a practical route to vinylarene scaffold-containing biologically relevant moieties.

To further improve the antibacterial performance of photocatalytic paper, a BiOBr/g-C₃N₄ photocatalyst was synthesized via a two-step method, involving calcination for g-C₃N₄ preparation followed by a solvothermal process for BiOBr/g-C₃N₄ composite formation. The BiOBr/g-C₃N₄ photocatalytic paper was fabricated by loading sunflower stalk pulp with a self-made hot-pressing device. In the composite, BiOBr and g-C₃N₄ form tight heterojunctions through close contact, facilitating efficient charge separation and enhancing visible-light utilization. The resulting photocatalytic paper exhibits excellent recyclability and strong antibacterial activity, achieving 99.99% antibacterial efficiency and extending the fruit preservation time by fourfold compared with the control group. This study provides a green and scalable approach for developing recyclable and biodegradable photocatalytic packaging materials with potential applications in sustainable food preservation.

The fast and selective oxidation protocol using cerium ammonium nitrate (CAN) in acetonitrile (MeCN) under ambient temperature and pressure was established. The primary features of this protocol include excellent substrate adaptability, gram-scale preparation with high productivity, and fast and selective oxidation of sulfides to sulfoxides. The mechanism of this reaction was demonstrated to involve a radical process. This protocol provides a fast and straightforward method for the oxidation of sulfides.

The delamination of LiCoO₂ (LCO) films on stainless steel (SS) substrates has remained a critical bottleneck for advancing all-solid-state thin-film lithium batteries (TFLBs). Here, we introduce a stress-engineering approach that fundamentally resolves this challenge through simultaneous monitoring, regulation, and utilization of film stress. In situ stress measurements revealed a universal transition of LCO films from tensile to compressive states during growth, with residual compressive stress in amorphous films originating from an “atomic pinning” mechanism. Among deposition parameters, working pressure was identified as the dominant factor for stress tuning, enabling precise control of stress evolution. Complementarily, substrate pre-annealing at 800°C in Ar released residual stresses and stabilized the SS surface, while moderate post-annealing of LCO films at 550°C preserved both mechanical integrity and electrochemical performance. This dual strategy effectively suppressed crack formation and delamination, yielding robust SS/LCO thin-film electrodes. By scaling this process to square-meter–scale SS/LCO/LiPON multilayers, all-solid-state TFLB cells were successfully fabricated, delivering an initial areal capacity of 38.4 µAh/(cm²·µm) and retaining 97.1% capacity after 1000 cycles. This work not only elucidates the intrinsic stress evolution and its atomic origins in LCO thin films but also pioneers a scalable route toward mechanically resilient, high-performance TFLBs.

We have disclosed the 9-fluorenol-catalyzed reductive dehalogenation of aryl halides. 9-Fluorenol, a readily available and structurally simple organic compound, serves as a catalytic single-electron reductant under light- and electricity-free conditions. Another key feature of this transformation is isopropyl alcohol, which simultaneously functions as the solvent, terminal reductant, and hydrogen source. Consequently, the reaction system requires only four components: substrate, catalyst, base, and solvent. This operationally simple method enabled efficient hydrodehalogenation of a wide range of aryl iodides as well as electron-deficient aryl bromides and chlorides.

Developing novel nonmetal nanozyme with high catalytic activity, environmental friendliness, and stability is challenging. In this work, a boron heteroatom-manipulated carbon-dots-based (B/Cdots) nanozyme was prepared via a simple one-step hydrothermal route. Doping of electron-hole boron could effectively downgrade their electronic energy barrier, therewith enhancing the electron transfer kinetics, and thereby promoting their peroxidase (POD)-like activity. Such POD-like activity of the B/Cdots can oxidize the colorless reduced 3,3’,5,5’-tetramethylbenzidine (TMB) to its blue oxidized state, oxTMB. Benefiting from the robust affinity of glutathione of antioxidant for silver(I) (Ag^I), the B/Cdots-based colorimetric platform was constructed for Ag^I monitoring, and displayed a good linearity from 0.5 to 140 µM with a limit of detection of 0.23 µM. Excitingly, the color alteration caused by Ag^I can also be easily observed by the naked eye and smartphone imaging, achieving convenient real-time onsite monitoring and eliminating the reliance on complex instruments or specialized expertise. Beyond developing a straightforward and robust multimodal method for Ag^I analysis, this work also enriches the extant inventory of nanozymes available for colorimetric assays and related fields.

Macrocyclic squaramide-containing receptors have previously been shown to bind sulfate with high selectivity and affinity in aqueous-organic mixtures. To increase binding affinity of this class of hydrogen-bonding receptors in pure water, macrocycles in which pyridinium groups have been inserted to provide additional charge-assisted hydrogen-bonding interactions were synthesized and their anion binding evaluated. The inclusion of charge-assisted interactions provides enhanced binding affinity for sulfate in water but concomitantly reduces ability of the receptors to discriminate sulfate from the closely related selenate and leads to unexpected changes in binding stoichiometry.

The generation of heteroatom-substituted C1 carbenoids is highly challenging due to their extreme instability and electronic perturbations. We report the reductive lithiation of organosulfur chloromethyl precursors using lithium naphthalenide (LiNp) under flow microreactor conditions. This method enables the flash generation of sulfur-containing lithium carbenoids, which were efficiently trapped with a wide range of electrophiles to afford functionalized organosulfur compounds. Spatially resolved optimization revealed that reaction efficiency critically depends on millisecond-scale residence times and temperature control, allowing selective generation while suppressing decomposition. The protocol tolerated diverse electrophiles, including carbonyls, isocyanates, and organometalloids, and subsequent selective deprotection of sulfur substituents further expanded synthetic utility. Comparative studies demonstrated the unique reactivity of sulfur versus oxygen or nitrogen analogues, highlighting the distinctive redox properties of organosulfur substituents.

We report a ruthenium(II)-catalyzed hydroarylation strategy for the stereoselective synthesis of trisubstituted alkenes via C─H bond activation of arylacetamides using weakly coordinating primary amides as directing groups in the presence of internal alkynes. This operationally simple and sustainable protocol demonstrates broad substrate scope and high diastereoselectivity, tolerating a wide range of electron-rich, electron-deficient, and sterically hindered arylacetamides. Both symmetrical and unsymmetrical internal alkynes are compatible with the transformation. The methodology is scalable and synthetically versatile as demonstrated through downstream functionalization. Mechanistic insights, supported by isotopic labeling and competition experiments, shed light on the reaction pathway.