Latest ArticlesRealizing both a high emission efficiency and luminescence dissymmetry factor (glum) in circularly polarized solution processable organic light-emitting diodes (CP-OLEDs) remains a significant challenge. In this contribution, two chiral phosphorescent liquid crystals based on cyclometalated platinum complexes are prepared, in which the chiral s-2-methyl-1-butyl group is introduced into the cyclometalating ligand and the mesogenic fragment is attached to the periphery of the ancillary ligand. The platinum complexes exhibit both smectic and chiral nematic phases as evidenced by polarized optical microscopy, differential scanning calorimetry and small-angle X-ray diffraction. Remarkably, a high photoluminescent quantum efficiency of over 78% and clear circularly polarized luminescent signal with gPL of about 10–2 are observed for the complexes. Further, solution-processed CP-OLEDs show maximum external quantum efficiencies (EQE) of over 15% and strong circularly polarized electroluminescent signals with a gEL ≈ 10–2. This research demonstrates that both liquid crystallinity and the number of chiral centers play key roles in improving the chiroptical property, paving the way for a new approach for the design of high-efficiency CPL emitters.
Developing an efficient Zn-based catalyst modified with Trifluoromethanesulfonic acid (TfOH) ligand is extremely desirable for the acetylene hydration reaction. In this paper, with the use of a simple impregnation method, a series of Zn-TfOH/AC catalysts were synthesized, and the Zn-1.5TfOH/AC catalyst demonstrated the optimal catalytic performance with 96% acetylene conversion in the hydration of acetylene. The X-ray absorption fine structure (XAFS) spectra of the fresh Zn-1.5TfOH/AC catalysts demonstrated the establishment of the Zn-O4 coordination structure. According to the characterization results, TfOH ligands effectively inhibited carbon accumulation and Zinc loss, improved acidic sites and the dispersion of active metal, and produced more catalytic active site. Furthermore, the hydration reaction mechanism of Zn-TfOH/AC catalyst with Zn(OTf)2, TfO-ZnCl, and TfO-ZnOH complex configurations was explored by the Density Functional Theory (DFT) method, which showed that the activation barrier increased sequentially TfO-ZnOH < Zn(OTf)2 < TfO-ZnCl. Importantly, the OH− in TfO-ZnOH is involved in the reaction and regenerated by the dissociation of H2O, which lowers the energy barrier. This will provide a reference to design more efficient nonmercury catalysts for acetylene hydration.
Heterogeneous Fenton has been widely used in the disposal of organic pollutants, however, slow regeneration of Fe(Ⅱ) remains limitation for its practical application of long-term treatment. Herein, we come up with a novel Fe-based heterogeneous Fenton catalyst named as FeSxOy-X (X is the ratio of ethylene glycol to N, N-dimethylformamide). With the help of the abundant defect electrons in Sulfur vacancies, Fe(Ⅱ) regeneration on the surface of FeSxOy-1:1 was accelerated, resulting in a stable proportion of Fe(Ⅱ) on the surface, which maintained continuously stable generation of hydroxyl radical (•OH) and singlet oxygen (1O2). Thus, without any organic reagents or cocatalysts, FeSxOy-1:1 based Fenton system achieved effective long-term degradation of 560 mg/L quinoline within only 7 days, which was evidently better than reported FeS and SV-FeS2 (SV: Sulfur vacancy). The system had excellent adaptability to water quality and the COD removal rate of biochemical wastewater was as high as 79.8%.
Ibrutinib is a first-line treatment drug for B-cell malignancies. However, resistance to ibrutinib has been reported due to BTKC481S mutation. Although PROTAC strategy is expected to overcome this clinical resistance, it has limitations such as large molecular weight and moderate bioactivity, which restrict its potential clinical application. Herein, we report a new type of potent BTKC481S-targeting PROTAC degrader. Through design, computer-assisted optimization and SAR studies, we have developed a representative BTKC481S degrader L6 with a much smaller molecular weight and improved solubility. Notably, L6 demonstrates better BTK degrading activity and lower IC50 value in ibrutinib-resistant cell line than the first-generation BTK degrader P13I. Optimization strategy of L6 provides a general approach in the development of PROTACs targeting BTK and other proteins for future study.
Atmospheric pollutants can deteriorate air quality and put human health at risk. There is a growing need for green, economical, and efficient technologies, among which catalytic elimination technology is the most promising, to remove atmospheric pollutants. Two-dimensional transition metal oxides (2D TMOs) have recently become attractive catalysts due to their highly exposed active sites, excellent reactant transport properties, and extraordinary catalytic performance. This review systematically summarizes the top-down and bottom-up preparation methods of 2D TMOs and focuses on the specific applications of 2D TMOs in the catalytic elimination of atmospheric inorganic pollutants and volatile organic pollutants. The development of 2D TMOs in the catalytic elimination of atmospheric pollutants is prospected. This review is expected to provide design insights into efficient 2D TMOs to remove atmospheric pollutants.
A new Rh(Ⅲ)-catalyzed aldehydic C-H activation/[4 + 3] annulation cascade of N-sulfonyl-2-aminobenzaldehydes with gem-difluorocyclopropenes is reported for the first time, and used to produce a range of hitherto unreported precedented β-monofluorinated benzo[b]azepin-5-ones with good yields and complete regioselectivity. This approach features a broad substrate scope, good functional group tolerance, and high regioselectivity, which may include Rh(Ⅲ)-catalyzed aldehydic C−H activation, tandem site-/regioselective insertion, defluorinated ring-scission, and 1, 2-elimination.
The NO gas is easily oxidized to form toxic by-products (NO2) during the oxidation process, which are adsorbed on the catalyst surface and inhibit the subsequent reaction. For photocatalytic NO removal, a significant challenge is to achieve catalytic stability while maintaining high conversion efficiency. Here, we fabricated a (BiO)2CO3/β-Bi2O3 heterostructure that enables efficient charge transfer and promotes the NO removal. We propose that the catalytic stability depends on the heterojunction structure, which is able to generate interfacial charge transfer channels. In addition, we further introduce graphene quantum dots on the heterojunction structure, which further strengthens the interfacial charge transfer dynamics and finally realizes that the NO2 byproduct could gain electrons and convert to the final product (nitrite or nitrate). This composite structure not only exhibits high activity for NO removal but also maintains long-term stability under visible light.
The co-crystallization of quercetin (Qur) with a flexible molecule 4-(4-pyridinyldisulfanyl) pyridine (DPDS) in different solvents and conditions was investigated, yielded five multi-component crystalline phases and characterized with X-ray diffractions and thermal analysis. Although the crystal system of Qur-DPDS-MeOH and Qur-DPDS-Dioxane is the same, the desolvation results revealed that Qur-DPDS-MeOH transformed to Qur-DPDS when MeOH solvent molecules escape from the lattice, while Qur-DPDS-Dioxane transformed to Qur-DPDS-Ⅱ through a similar process, which is same with Qur-DPDS-THF. These two cocrystal polymorphs Qur-DPDS and Qur-DPDS-Ⅱ obey an enantiotropic relationship. Moreover, the formation of cocrystal solvates improves the packing efficiency of crystals. Crystal structure analysis showed that hydrogen bonds and conformations of the corresponding parent molecules play a major role in molecular assembly and crystal packing patterns, thus bring different physicochemical properties. Finally, the fluorescence spectra and quantum-chemical calculations were carried out to explore the difference in the optical-physical properties.
Bicyclic peptides, a class of polypeptides with two loops within their structure, have emerged as powerful tools in the development of new peptide drugs. They have the potential to bind to challenged drug targets, with antibody-like affinity and selectivity. Meanwhile, bicyclic peptides possess small molecule-like access to chemical synthesis, which is conducive to large-scale synthesis and screening. In the last five years, bicyclic peptide technology has been increasingly developed, and researchers have carried out a variety of studies to elucidate the potential functions of bicyclic peptides. With the continuous development of synthetic methods and the advances of new technology to build bicyclic peptide libraries, bicyclic peptides are now becoming widely used in the development of new drugs for various diseases. This perspective provides an overview of the structure types, synthesis and applications of bicyclic peptides in current drug development, and our own views on future challenges of bicyclic peptides.
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