Latest ArticlesCopper-catalyzed divergent annulations between α-diketones and alkynyl α-diketones have been achieved, delivering a series of highly functionalized and biologically important cis-hexahydro-2H-cyclopenta[b]furan (HCPF) and 2-hydroxydihydrofuran-3(2H)-one (HDFO) products with high levels of stereoselectivity under identical conditions. The protocol features the use of earth-abundant copper catalyst, mild conditions, shortening synthetic routes in constructing different molecular frameworks, and reducing the corresponding possible waste production. The substituents of the nucleophilic α-diketones play crucial roles in switching the reaction pathways.
Neuromuscular blocking agents (NMBAs) are extensively used during anesthesia to improve surgical conditions by relaxing skeletal muscle movements. Rapid neuromuscular recovery after surgery is desirable to facilitate the recovery of muscle function and prevent residual blockade. Decamethonium (C10) is a classic NMBA, which has been restricted over the past decades ascribed to lack of a suitable antidote in clinic. Herein we used carboxylatopillar[6]arene (CP6A) to reverse neuromuscular blocker effect of C10 through direct host-guest encapsulation. NMR and isothermal titration calorimetry served to confirm the complexation between CP6A and C10 with robust affinity [(1.07 ± 0.14) × 107 L/mol]. The CP6A was further used as a reversal agent of C10, which facilitated to decrease C10 concentration in mice blood and excrete via urinary clearance, resulting in rapid recovery from muscle relaxation. These favorable outcomes might lead us to suggest that this supramolecular strategy could allow patients to regain lucidity much faster than spontaneous recovery from anesthesia.
A hexafluoroisopropanol (HFIP)-catalyzed highly diastereoselective formal [4 + 2] cyclization between ortho-hydroxyphenyl para-quinone methides and difluoroenoxysilanes is developed. This tandem protocol provides a simple and straightforward approach to assemble diverse multiply functionalized difluorinated chromans with high to excellent diastereoselectivity by employing difluoroenoxysilane as a new C2 synthon.
The first example of stereoconvergent 1, 3-dipolar cycloaddition of nitrile oxides and nitrile imines with E/Z isomeric mixture of electron-deficient olefins is reported, delivering isoxazolines and pyrazolines bearing two vicinal stereogenic tertiary and trifluoromethylated quaternary carbon centers with perfect regio- and diastereoselectivities. The possibility of concerted cycloaddition/epimerization sequence under basic condition to form the thermodynamically stable diastereomers is excluded through some control experiments and DFT calculations, and a stepwise mechanism is proposed.
A new type of covalent organic framework (COF) was achieved using combination of structrally rigid and conformationally othorganal building blocks. The N-2-aryl-substituted triazole derivative (NAT-CHO) was prepared with co-planar conformation among the three aromatic rings as the "flat" building block. The 4, 4′, 4′′, 4′′′-(ethene-1, 1, 2, 2-tetrayl)tetraaniline) (ETTA) was applied as the "twist" building block. A 2D sheet of network was obtained through imine formation. The resulting NAT-COF gave excellent thermal and chemical stability, survived aqueous solutions from pH 5 to 13. With large-size building blocks, the porous framework NAT-COF gave efficient gas adsorption with excellent selectivity of C3 propane over C1 me-thane, suggesting its potential application for selective gas capture and separation.
MeOTf-catalyzed formal [4 + 2] annulation of styrene oxides with alkynes to afford polysubstituted naphthalenes has been realized, which undergoes sequential electrophilic cyclization/ring expansion. A range of substrates were tolerated in the formation of naphthalene derivatives with high regioselectivity in satisfactory yields. The reaction could also be carried out on gram scale.
DNA-functionalized gold nanoparticles are one of the most versatile bionanomaterials for biomedical and clinical diagnosis. Herein, we discovered that the performance of DNAzyme cleaving the substrate is highly related to its length. This intriguing phenomenon only appears at the interfaces of DNA-functionalized gold nanoparticles. We systematically investigated the causes of this phenomenon. We conjectured that the DNAzyme with extended nucleotides that do not match its substrate strand is vulnerable to non-specific adsorption, electrostatic repulsion, and steric hindrance. Based on our improved understanding of this phenomenon, we have successfully developed a highly sensitive and specific amplifiable biosensor to detect human apurinic/apyrimidinic endonuclease 1.
Aromatic carboxylic acids (ACAs) may be as transformed key metabolites via gut microbiome for playing better pharmacological effects. However, it's rare to achieve high-specificity, high-sensitivity, and high-throughput detection simultaneously, especially, for tracing trace ACAs in gut microbiome. In this work, firstly, a novel dual-template and double-shelled molecularly imprinted 96-well microplates (DDMIPs) was designed and amplified signal for p-hydroxybenzoic acid (PBA) and 3, 4, 5-trimethoxycinnamic acid (TMA). Additionally, the DDMIPs and a stable isotope labeling derivatization (SILD) method combined with the ultra-high performance liquid chromatography triple quadrupole tandem mass spectrometry (UHPLC-TQ MS) was firstly stepwise integrated, achieving high-effective, high-sensitive, and high-throughput study of gut microbiome metabolism. The whole strategy showed lower limits of detections (LODs) up to 1000 folds than the traditional method, and revealed a more real metabolism-time profile of PBA and TMA by 3-step signal amplification. The platform also laid the foundation for fast, simple, high-selective, high-effective, and high-throughput metabolism and pharmacological research.
In this paper, Ni3S2 nanosheet (NS) was generated by chemical etching with sodium sulfide directly on the nickel foam (NF), which was induced by dielectric barrier discharge plasma in liquid. Compared with other chemical etching methods of nickel-based nanomaterials, this method was not only rapid (40 min) and mild (at room temperature and atmospheric pressure), but also showed consistent stability and good reproducibility. The Ni3S2 NS/NF electrode showed excellent performance in the electrochemical detection of formaldehyde under alkaline conditions. It had a good linear relationship with the concentration of formaldehyde in the range of 0.002-5.45 mmol/L (R2 = 0.9957) and the limit of detection (LOD) was 1.23 µmol/L (S/N = 3). The sensitivity was 1286.9 µA L mmol‒1 cm‒2, and the response time was about 5 s. The plasma-induced chemical etching strategy provides a simple and stable electrode preparation method, which has great application prospects in nonenzymatic electrochemical sensors.
Excellent optical properties involving strong visible light response and superior carrier transport endow metal halide perovskites (MHP) with a fascinating prospect in the field of photocatalysis. Nevertheless, the poor stability of MHP nanocrystals (NCs) in water-contained system, especially without the protection of long alkyl chain ligands, severely restricts their photocatalytic performance. In this context, we report an effortless strategy for the generation of ligand-free MHP NCs based photocatalyst with high water tolerance, by coating PbI2 on the surface of ligand-free formamidinium lead bromide (FAPbBr3) NCs via the facile procedure of in-situ conversion with the aid of ZnI2. Under the protection of PbI2 layer, the resultant FAPbBr3/PbI2 composite exhibits significantly ameliorated stability in an artificial photosynthesis system with CO2 and H2O vapor as feedstocks. Moreover, the formation of compact PbI2 layer can accelerate the separation of photogenerated carriers in FAPbBr3 NCs, bringing forth a remarkable improvement of CO2 photoreduction efficiency with an impressive electron consumption yield of 2053 µmol/g in the absence of organic sacrificial agents, which is 7-fold over that of pristine FAPbBr3 NCs.
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