Chemistry - An Asian Journal最新文献

Li-ion capacitors (LICs) integrate the desirable features of lithium-ion batteries (LIBs) and supercapacitors (SCs), but the kinetic imbalance between the both electrodes leads to inferior electrochemical performance. Thus, constructing an advanced anode with outstanding rate capability and terrific redox kinetics is crucial to LICs. Herein, heterostructured ZnS/SnS2 nanosheets encapsulated into N-doped carbon microcubes (ZnS/SnS2@NC) are successfully fabricated. The sufficient ZnS/SnS2 heterostructure possesses abundant active sites, and the built-in electric field formed at the heterojunction interface can facilitate electron/ion migration. The interconnected hollow carbon layers could reduce the electron transfer resistance effectively and accommodate the volume expansion of SnS2, thereby maintaining the structural stability. Due to the synergy between multi-components, the ZnS/SnS2@NC anode demonstrates impressive Li storage performance with an excellent cyclic durablity (690 mAh g-1 at 0.5 A g-1 after 600 cycles) and considerable rate capability. Moreover, when matched with active carbon, the ZnS/SnS2@NC based LIC device delivers an admirable energy density of 134.1 Wh kg-1 and a high power output of 11,250 W kg-1, as well as remarkable capacity retention of 73.2% after 6,000 cycles at 1.0 A g-1. The experimental results demonstrate the significance of optimized heterointerface engineering toward construction of electrode materials with high-performance for Li storage.

Herein, we describe a protocol for Brønsted acid-catalyzed regioselective coupling of azoles such as pyrazoles, 1,2,3-triazole, 1,3,4-triazole, benzotriazole, indazole and tetrazole, to cyclobutenes. These azoles could be directly coupled with various arylcyclobutenes with high site-selectivity, offering a distinct entry to more functionalized cyclobutanes. The usage of inexpensive TsOH•H2O catalyst, broad substrate scope, and open-air conditions make this protocol practically viable. This study not only contributes a feasible tool for selective functionalization of cyclobutenes, but also provides a strategy to introduce cyclobutane moieties into complex molecules.

The development of efficient electron-collecting monolayer materials is desired to lower manufacturing costs and improve the performance of regular (negative-intrinsic-positive, n-i-p) type perovskite solar cells (PSCs). Here, we designed and synthesized four electron-collecting monolayer materials based on thiazolidinone skeletons, with different lowest-unoccupied molecular orbital (LUMO) levels (rhodanine or thiazolidinedione) and different anchoring groups to the transparent electrode (phosphonic acid or carboxylic acid). These molecules, when adsorbed on indium tin oxide (ITO) substrates, lower the work function of ITO, decreasing the energy barrier for electron extraction at the ITO/perovskite interface and improving the device performance. The shift of work function, rather than the LUMO levels of the molecules themselves, was found to be correlated with the performance of the perovskite solar cells.

Traditional photocatalysts often have limited efficiency due to the high recombination rate of photogenerated electron-hole pairs. In this work, we synthesized 3D/2D ZnSe-MXene heterojunctions by an in situ electrostatic self-assembly method. Notably, the 3% MXene-ZnSe composite exhibited an optimized photocatalytic hydrogen production rate of 765.0 μmol g-1 h-1, about 1.6 times higher than that of pristine ZnSe. MXene's high conductivity and large surface area enhance catalytic performance by providing more active sites and efficient electron transfer pathways from ZnSe to MXene. This accelerates the separation and movement of photogenerated carriers, significantly reducing recombination. We have investigated the photocatalytic hydrogen production mechanism of the ZnSe-MXene composites using various characterization techniques. Our findings provide favourable insights into the synergistic effects within the heterojunction, offering valuable guidance for the design and development of advanced photocatalytic materials.

Smart luminescent materials have drawn a significant attention owing to their unique optical properties and versatility in sensor applications. These materials, encompassing a broad spectrum of organic, inorganic, and hybrid systems including quantum dots, organic dyes, and metal-organic frameworks (MOFs), offer tunable emission characteristics that can be engineered at the molecular or nanoscale level to respond to specific stimuli, such as temperature, pH, and chemical presence. Recent advancements have been driven by the integration of nanotechnology, which enhances the sensitivity and selectivity of luminescent materials in sensor platforms. The development of photoluminescent and electrochemiluminescent sensors, for instance, has enabled real-time detection and quantification of target analytes with high accuracy. Additionally, the incorporation of these materials into portable, user-friendly devices, such as smartphone-based sensors, broadens their applicability and accessibility. Despite their potential, challenges remain in optimizing the stability, efficiency, and biocompatibility of these materials under different conditions. This review provides a comprehensive overview of the fundamental principles of smart luminescent materials, discusses recent innovations in their use for sensor applications, and explores future directions aimed at overcoming current limitations and expanding their capabilities in meeting the growing demand for rapid and cost-effective sensing solutions.

(+)-Febrifugine, a natural antimalarial compound with a promising therapeutic profile, has become a hot target for synthetic chemists seeking to optimize its biological activity and expand its therapeutic applications. In this research, we present a stereocontrolled synthesis of (+)-febrifugine using both azide and azide-free approaches. Starting from the commercially available chiral pool precursor, d-glucose, the synthesis was completed in 20 steps for both approaches. Key reactions included the Zn-mediated Bernet-Vasella reaction, Horner-Wadsworth-Emmons reaction, and cyclization for constructing the chiral substituted piperidine ring. Additionally, α-bromoketone alkylation of quinazolinone was employed to assemble the (+)-febrifugine core structure.

Herein, we report the radical azidoamination of styrenes via the use of a combination of sodium azide and (diphenylmethylene)amino benziodoxolone under visible-light irradiation. This approach to unsymmetrical diamination provides a simple and practical method for constructing vicinal diamine scaffolds with two distinct and easily modifiable amino functionalities.

N-acyl/sulfonyl-α-phosphonated 1,2,3,4-tetrahydroiso-quinolines (THIQs) are highly important structural motifs in organic synthesis and drug discovery. However, the one-pot approach enabling direct difunctionalization of THIQs remains challenging. Herein we report a photomediated one-pot multicomponent cascade reaction to access N-acyl/sulfonyl-α-phosphonated THIQs via twice acyl/sulfonyl iminium. This method features air as an oxidant, high atom and step economy, and mild conditions.

A series of Dehydroabietylamine (DHAA) C-ring Schiff derivatives, L3-L20, were synthesized and their in vitro cytotoxic activity against the human tumor cell lines cervix HeLa, breast MCF-7, lung A549, liver HepG2, and the nonmalignant cell line umbilical vein HUVEC was investigated. Most of the compounds showed varying degrees of anticancer activity against HeLa cell lines while demonstrating lower toxicity to normal HUVEC cells compared to DHAA and doxorubicin (DOX), especially compound L19, which not only enhanced the anticancer activity of DHAA, but also significantly reduced the toxicity to normal cells, achieving a selectivity index (SI) 118 times higher than that of DHAA and 245 times higher than that of DOX. In addition, compound L19 induced apoptosis in HeLa cells in a dose-dependent manner and arrested the cell cycle in S phase. Spectroscopic experiments and molecular docking results showed that there was a strong interaction between the compounds and DNA. All these results indicate that the introduction of Schiff base structure on the C-ring of DHAA is an effective strategy for enhancing its selectivity, providing new insights for the design of DHAA-based anticancer compounds.

A simple method for constructing unsymmetrical 2-nitrobiaryls has been developed between substituted 1,4-dithiine-2-carbaldehyde and nitroolefins under metal-free conditions. To gain the advantage of the HOMO-raising effect of temporary substitutions on in situ generated dienamine intermediate, the present protocol established [4+2] benzannulation of 1,4-dithiane-tethered enals with nitroolefin. Further, easy unmasking of 1,4-dithiine units results in a benzannulation product like that of unsubstituted enals, which are difficult to access. Several 2-nitrobiaryls have been accessed with moderate to good yields and with promising synthetic applications.