New Journal of Chemistry最新文献

It is of great significance to develop high performance n-type polymer semiconductors (PSCs), which are essential for fabricating various p–n junction organic electronic devices. In this work, based on commonly used acceptor unit diketopyrrolopyrrole (DPP) and recently developed acceptors fluorenone imide (FOI)/cyanated fluorenone imide (FCNI), we prepared two new dual-acceptor (A1–A2) type PSCs, PFOI-DPP and PFCNI-DPP. Benefitting from improved components of the acceptor moieties in their backbones, the two polymers exhibited low-lying frontier molecular orbital energy levels. Theoretical simulation revealed that they also have a highly planar backbone. Ultimately, organic thin-film transistors based on the two polymers showed unipolar n-type characteristics with a maximum electron mobility of 0.55 cm² V⁻¹ s⁻¹.

Silent information regulator sirtuin 1 (SIRT1) is a niacinamide adenine dinucleotide (NAD)-dependent histone deacetylase and a promising target for the treatment of hepatocellular carcinoma (HCC). In this research, we designed SIRT1 inhibitors using various computational methods and validated their activity through experiments, while network pharmacology was used to explore the potential therapeutic effects of the designed compounds on HCC. Based on the 3D-QSAR contour map, pharmacophore, MOLCAD and ADMET analysis results, we attempted to construct seven compounds. Among them, compound 18a showed excellent predictive activity and pharmacokinetic properties. The molecular dynamics (MD) simulations indicated that compound 18a binds closely to the SIRT1 protein. PHE57, PHE33, ILE107 and ILE30 were considered to be key residues that facilitated the binding of the ligand to the receptor. Integrating experimental results and network pharmacology predictions indicated that compound 18a exerted its inhibitory effect on the proliferation of HCC possibly by regulating the FOXO signaling pathway and the PI3K-Akt signaling pathway. This study provides theoretical support for the design and discovery of novel SIRT1 inhibitors.

A simple one-step heterogeneous catalytic cyclization-based procedure was employed to prepare 2,4-disubstituted quinolines from ketones and 2-aminobenzophenones using Hβ zeolite as a catalyst in solvent-free conditions. Using a variety of substrates, the probabilities and constraints of catalytic activity were studied. Large scale studies validated the viability and effectiveness of scaling up this catalytic system. Furthermore, the catalyst has been employed repeatedly up to five times without any significant loss in its catalytic efficiency. This method provides a fascinating and green approach for synthesizing a broad range of 2,4-disubstituted quinoline derivatives utilizing simple starting materials and a heterogeneous catalyst in optimum reaction conditions. Furthermore, the anticancer potential of the synthesized compounds was evaluated in vitro against the PC-3, H460 and MDA-MB-231 cell lines. Cytotoxicity assays revealed that compounds 3c, 3q, and 3t exhibited significant anticancer activity against PC-3 cells, while compound 3m demonstrated potent activity against MDA-MB-231 cells. In addition, compounds 3d and 3f showed anti-cancer activity in H460 (lung cancer cells). Notably, compound 3aa exhibited broad-spectrum anticancer activity across all three tested cell lines. Further studies demonstrated that the selected compounds induced apoptosis and caused G1 or G2 phase cell cycle arrest, suggesting their potential anti-cancer activity through the regulation of cell cycle progression. Overall, these findings indicate that 2,4-disubstituted quinolines exhibit significant anti-cancer properties in breast, prostate and lung cancer cells.

Expression of concern for ‘Deep eutectic solvent mediated synthesis and fabrication of a WO₃–MgO nanocomposite as an electrode material for energy storage applications’ by C. Joel et al., New J. Chem., 2023, 47, 2797–2808, https://doi.org/10.1039/D2NJ05642A.

Herein, we describe a novel and rapid method for synthesizing vinyl ethers. This metal-free, straightforward technique efficiently introduces the vinyl ether moiety along with the sulfonyl fluoride functional group under mild conditions within 10 minutes. The strategy demonstrates high efficiency across various substrates, enabling the rapid synthesis of structurally diverse compounds. This approach highlights the potential to revolutionize industrial chemical processes by providing a practical and efficient route for organic synthesis.

The current study reports the electrocatalytic water oxidation by mononuclear bis-terpyridine Co(II) complexes of general formula [CoL^1–4₂]X₂ (where L¹ = 4′-phenyl-2,2′:6′,2′′-terpyridine, L² = 4′-(3,4-dimethoxyphenyl)-2,2′:6′,2′′-terpyridine, L³ = 4′-(3,4,5-trimethoxyphenyl)-2,2′:6′,2′′-terpyridine, L⁴ = 4′-(4-fluorophenyl)-2,2′:6′,2′′-terpyridine, and X = ClO₄⁻/Cl⁻). All the complexes have been fully characterized by single-crystal X-ray diffraction and mass spectroscopy, which show the CoN₆ core structure in all the complexes. The complexes exhibit moderate to good electrocatalytic activity at pH 13.5. During the water oxidation study, an electrocatalytic wave in cyclic voltammetry appears near the Co(IV/III) couple in all four complexes (1–4). The electrocatalytic water oxidation occurs at an onset potential of 0.80 V, 0.81 V, 0.72 V, and 0.85 V vs. NHE for 1, 2, 3, and 4, respectively. The efficiency of the catalysts has been found to depend on the electron-withdrawing and -donating capacity of the substituents in the ligand scaffold. An electron-donating –OMe group in the terpyridine results in the maximum rate, while the electron-withdrawing –F group displays the lowest rate of the water oxidation reaction. Determination of the TOF values by both the peak current method (TOF_1,2,3,4 = 10 s⁻¹, 16 s⁻¹, 40 s⁻¹, 1 s⁻¹, respectively) and FOWA (TOF_1,2,3,4 = 22 s⁻¹, 34 s⁻¹, 194 s⁻¹, 2 s⁻¹) method follows the same trend. The faradaic efficiency of the complexes has been found to be 61%, 64%, 68%, and 35% for complexes 1, 2, 3, and 4, respectively. The TON calculated for complexes 1, 2, 3, and 4 have been found to be 11, 13, 18, and 5, respectively. The mechanism of water oxidation has been proposed based on mass spectral data of the electrochemically oxidised species and DFT calculations. All the molecules act as active OEC (oxygen-evolving complexes) photochemically with visible light in the presence of [Ru(bpy)₃]Cl₂ as photosensitizer and Na₂S₂O₈ as electron acceptor.

Although LiFePO₄ (LFP) is considered a promising cathode active material (CAM) because of its excellent cost-effectiveness and thermal stability, its interfacial compatibility with sulfide-based solid electrolytes in all-solid-state batteries (ASSBs) remains a major technical hurdle. Herein, we investigated the effects of electrolyte interlayers to achieve high-efficiency LFP-based CAMs by applying interlayers of an argyrodite-based sulfide [Li_5.4PS_4.4Cl_0.8Br_0.8 (LPSCB)] or a halide with high Li-ion conductivity [Li₃InCl₆ (LIC) or Li_2.5Y_0.5Zr_0.5Cl₆ (LYZC)]. As a result, the ASSB cell with an LIC or LYZC interlayer exhibited better electrochemical performance than that with LPSCB, with initial discharge capacities of 113.5 and 110.3 mAh g⁻¹ at 0.1C, respectively. In particular, the sulfide interlayer suffered from serious Fe²⁺ oxidation because it interacted with other anions. Regarding the halides, LYZC was stable in contact with the sulfide SE but showed low reactivity with LFP, whereas LIC was stable with LFP but quite unstable with the sulfide SE. This strategy provides valuable insights for achieving superior interfacial structures in LFP-based ASSBs.

Copper zinc tin sulfide, Cu₂ZnSnS₄ (CZTS), has recently emerged as a promising candidate for photocatalytic applications due to its earth abundance, non-toxicity, and suitable bandgap for visible light absorption. CZTS has been prepared using different methods for a range of applications. This synthesis and development of CZTS and CZTS-based heterostructures have been compiled and discussed. This review provides an overview of the recent progress in utilizing CZTS for photocatalysis and highlights its advantages as well as its challenges. Moreover, this review also covers the surface modifications of CZTS that have been employed to enhance its photocatalytic activity. However, unexplored areas remain in research that could aid in advancing the development of CZTS and CZTS-based heterostructures. Therefore, this perspective review aims to offer insights into the fabrication and optimization of CZTS for photocatalytic applications under irradiation of visible light and future prospects have been suggested for further improvement in this field.

Cu₂₂Sn₁₀S₃₂, a type of Cu–Sn–S (CTS) compound, is known for its super-high carrier concentration, which is unfavorable for thermoelectric applications. In this work, nanostructured In₂O₃ was incorporated into a Cu₂₂Sn₁₀S₃₂ matrix (CTS-x wt% In₂O₃, x = 0, 1, 2, 3, 4, 5, 6, 7) through high-energy ball milling in conjunction with spark plasma sintering. Microstructure analysis reveals that the introduced nano-In₂O₃ reacts with Cu₂₂Sn₁₀S₃₂, with In being uniformly doped in the matrix. At higher In₂O₃ contents (x ≥ 5), a SnO₂ secondary phase appears. The incorporation of nano-In₂O₃ leads to a substantial decrease in carrier concentration by one order of magnitude. At the same time, the carrier mobility shows a clear increase due to the suppressed carrier–carrier scattering. This ultimately lowers the electrical conductivity, which also contributes to a significant decrease in electronic thermal conductivity. Additionally, the lattice distortion caused by the substitution of In for Cu also leads to a significant reduction in lattice thermal conductivity. Ultimately, a maximum zT of 0.6 at 723 K was achieved for the CTS-5 wt% In₂O₃ sample, which shows a 60% increase compared to the Cu₂₂Sn₁₀S₃₂ matrix. Our study illustrates that the introduction of nanoparticles into a CTS matrix can effectively lower its carrier concentration and lattice thermal conductivity, thereby optimizing its thermoelectric performance.

Dimethylamine (DMA) is a key precursor for the carcinogenic N-nitrosodimethylamine (NDMA), yet the role of radical intermediates in DMA oxidation and N–N bond formation remains unclear. Using electron paramagnetic resonance (EPR), this study explored free radical generation in the DMA/NaClO and DMA/KMnO₄ systems, previously linked to NDMA formation. Without spin traps, three long-lived nitrogen-containing radicals were detected: dimethyl nitroxide radicals (DMNO˙), tetramethylhydrazine cation radicals (TMH˙⁺), and N,N-dimethylaminomethyl radicals (UDMHr). Their formation depends on pH, reaction time, and oxidant type and concentration. DMNO˙, formed via DMA oxygenation or hydrogen abstraction, is unstable at acidic pH and converts to N,N-dimethylhydroxylamine (DIMHA). TMH˙⁺ likely arises from tetramethylhydrazine (TMH) through single-electron transfer, followed by further reactions to produce UDMHr, a key NDMA precursor. This study proposes pathways for these radicals in DMA oxidation, offering direct EPR evidence of N-containing radicals and their potential role in NDMA formation.