Latest ArticlesA phosphorescent supramolecular foldamer is conveniently constructed by the 1:1 host–guest complexation with cucurbit[8]uril and 1, 2-diaminocyclohexane-bridged 4-(4-bromophenyl)-pyridinium salt. The tightly compact host–guest complexation in molecular foldamer can greatly suppress the fluorescence emissive channel and promote the intersystem crossing from singlet to triplet states, thus leading to the green phosphorescence at ambient temperature in aqueous solution. More intriguingly, the phosphorescence emission shows very rapid and sensitive responsiveness to different antibiotics in both inanimate milieu and living cells. Remarkably, the limit of detection of such binary inclusion complex toward sulfamethazine can reach as low as 1.86 × 10−7 mol/L. Thus, it is envisaged that this supramolecular nanoplatform featuring unique complexation-enhanced phosphorescence emission may hold great promise in sensing and detecting many other biological targets under physiological environment.
The selective synthesis of N2-sulfonyl and N2-H 1, 2, 3-triazoles via organocatalytic annulation of enaminone/enaminoester with sulfonyl azide has been realized. The unconventional selectivity providing N2-sulfoyl 1, 2, 3-triazoles takes place in pure water, wherein the hydrogen bond effect between water and the intermediate resulting from enamine-azide corporation accounts for the novel reaction selectivity. On the other hand, the reactions conducted in DMSO specifically afford N2-H 1, 2, 3-triazoles in the absence of such hydrogen bond effect.
The biological activities of a series of 3, 3′-spirocyclic indole derivatives containing CF2, phosphine oxide, indole, and cyano functional groups were evaluated, and these derivatives were found to exhibit anti-TMV, fungicidal, and insecticidal activities.
Three bench-stable difluoromethylene phosphonate hydrazones were prepared from simple diethyl(difluoromethyl)phosphonate within two steps in good yields. The [3 + 2] cycloaddition reaction of these diazo precursors with aryl diazonium salts has been accomplished under metal-free conditions with exclusive regioselectivity. This transformation provides practical access to a broad panel of 2-aryl-2H-tetrazol-5-yl difluoromethylene phosphonates, including the corresponding derivatives of amino acid (phenylalanine) and drug cores (Pomalidomide and Lapatinib fragment).
Anthrones are key structural motifs in many natural products, bioactive compounds and pharmaceutical chemicals. Earth-abundant-metal-catalyzed asymmetric functionalization of anthrones has not proved to be viable. Herein, we disclosed a highly enantioselective propargylic substitution of anthrones with propargylic esters using copper salts with chiral N, N, P-ligand. This strategy is amenable to a broad range of substrates, uses readily available starting materials, provides excellent yields with remarkable enantioselectivity under mild conditions, and enables attractive products diversification routes.
Nature consists of various soft tissues with well-ordered hierarchical anisotropic structures, which play essential roles in biological systems to exhibit particular functions. Mimicking bio-tissues, synthetic hydrogels with anisotropic structures have received considerable attention in recent years. However, existing approaches to fabricate anisotropic hydrogels often require complicated procedures, which are time-consuming and labor-demanding. Inspired by the dry-induced crystallization phenomenon, we report a simple yet effective prestretching-drying-swelling method to afford anisotropic crystalline polyvinyl alcohol hydrogels. Owing to the distinct anisotropic microstructure, the hydrogels demonstrate excellent mechanical properties with noticeable directional distinction. It is revealed that both the enhancing of pre-orientation strain and the extending of heating time make the hydrogels with better mechanical properties and more remarkable anisotropicity. Owing to the anisotropically aligned structure, the hydrogels exhibit remarkably differential ionic conductivity: the difference between the parallel and vertical conductivity of the same sample can reach as high as 6.6 times, making the materials possible candidates as nano-conductive materials. We anticipate that this simple yet effective approach may become highly useful for fabricating oriented hydrogels and endow the materials with more promising application prospects in the future.
The preparation of amorphous pure organic room-temperature phosphorescence materials with high efficiency is still a challenging task. Herein, we introduce a CB[6] derivative-based supramolecular self-assembling strategy. A water soluble and ellipsoidal deformed CB[6] derivative is used to self-assemble with 4-(4-bromophenyl)-1-methylpyridin-1-ium chloride, bromide and hexafluorophosphate in water. After freeze-drying, the obtained amorphous complexes exhibit brilliant green phosphorescence emission under ambient conditions, with phosphorescence efficiency up to 59%, 60% and 72%, respectively. This is the first report of amorphous non-polymeric pure organic room-temperature phosphorescence with such a high efficiency. In view of the dynamic self-assembling property, the complexes are responsive to water, which could enable information encryption.
We report supramolecular AND logic gates based on host-guest complexation between acid-labile acyclic cucurbit[n]uril (CB[n]) molecular container and NaClO-responsive dye. Supramolecular AND logic gate is turned on due to acid-triggered degradation of molecular container and the release of the dye, followed by NaClO-induced fluorescence "switch on" effect of the dye. The reason for AND molecular logic gate is discovered to be the combination of oxidation inhibition and fluorescence "switch off" effect. Supramolecular AND logic gate is confirmed to be operational in live MCF-7 and HeLa cancer cells.
A bioinspired acid-triggered hemiacetalization/dehydration/[3 + 3]-type cycloaddition cascade process was disclosed, diastereoselectively furnishing furo[2,3-b]chromene skeleton under mild conditions. The viability of this approach was demonstrated by syntheses of a series of furo[2,3-b]chromene and pyrano[2,3-b]chromene derivatives. The successful total syntheses of two lignan-phloroglucinol hybrids, hyperaspidinols A and B, exemplified the synthetic utility of our biomimetic methodology.
Developing non-noble-metal oxygen evolution reaction (OER) electrocatalysts with high performance is critical to electrocatalytic water splitting. In this work, we fabricated CoFe-layered double hydroxide (LDH) nanowire arrays on graphite felt (CoFe-LDH/GF) via a hydrothermal method. The CoFe-LDH/GF, as a robust integrated 3D OER anode, exhibits excellent catalytic activity with the need of low overpotential of 252 and 285 mV to drive current densities of 10 and 100 mA/cm2 in 1.0 mol/L KOH, respectively. In addition, it also maintains electrochemical durability for at least 24 h. This work would open up avenues for the development of GF like attractive catalyst supports for oxygen evolution applications.
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