Latest ArticlesThe 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.
Chiral covalent organic frameworks (CCOFs) featuring chirality, stability, and good porosity have attracted a considerable amount of attention due to their important applications, such as asymmetric catalysis, chiral separation, and chiral recognition. In this study, a β-cyclodextrin (β-CD) covalent organic framework (β-CD-COF) diluted with polysiloxane OV-1701 was explored as a novel chiral stationary phase (CSP) for gas chromatography (GC) separation of racemates. The β-CD-COF coated capillary column had excellent selectivity, not only for the separation of linear alkanes, linear alcohols, fatty acid methyl esters mixture, the Grob mixture and positional isomers, but also for the resolution of chiral compounds, including chiral alcohols, aldehydes, ethers, and amino acid derivatives. In addition, the β-CD-COF-coated capillary column presented good repeatability and reproducibility. This work indicated the great potential of the CCOFs coated capillary column for the chromatographic separation of enantiomers.
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.
Excellent radiation resistance is a prerequisite for pressure-sensitive hydrogels to be used in high-energy radiation environments. In this work, tannic acid-modified boron nitride nanosheet (BNNS-TA) is first prepared as the radiation-resistant additive by a facile one-step ball milling of hexagonal boron nitride and tannic acid. Then, polyacrylamide (PAAm)-based pressure-sensitive hydrogel doped with BNNS-TA and Fe3+ ions is fabricated. The ternary BNNS-TA/Fe3+/PAAm hydrogel exhibits excellent compressive strength (at least four times the compressive strength of unfilled pure PAAm hydrogel), pressure-sensitive performance (gauge factor is up to 1.4), and performance recovery due to the combination of multiple intermolecular interactions, such as covalent crosslinking, hydrogen bonds, and ion coordination interactions. The BNNS-TA/Fe3+/PAAm hydrogel can be made as a pressure sensor installed in the control circuit or attached on the human body to detect human activities accurately. More importantly, the compressive strength and the pressure-sensitive performance of the BNNS-TA/Fe3+/PAAm hydrogel can be maintained after the hydrogel is irradiated by 60Co gamma-ray at an absorbed dose of 15 kGy. As a comparison, the compressive strength of the unfilled PAAm hydrogel is only a quarter of that before irradiation. This work not only reveals a facile method to achieve the preparation of chemically modified BNNS as a promising radiation-resistant additive but also provides a novel strategy for the development of pressure-sensitive hydrogel devices in radiation environments.
By the replacement of halogen anion, three new multifunctional organic-inorganic hybrid perovskites (thiomorpholinium)PbX3 (X = Cl, Br, I) were successfully synthesized and underwent reversible structural transformation above room temperature, accompanied by the anomalous change of dielectric constant. With the adjustment of the halogen anion from Cl to I in the inorganic skeleton, the space group is transformed from centrosymmetric space group P21/c ((thiomorpholinium)PbCl3) to chiral one P212121 ((thiomorpholinium)PbBr3, (thiomorpholinium)PbI3) at room temperature. The ordered-disordered transition of organic cations and the change of hydrogen bonds with the increase of temperature lead to above-room-temperature phase transitions. Ultraviolet absorption and second-harmonic generation (SHG) measurements confirmed that both the band gap and SHG activity of (thiomorpholinium)PbX3 (X = Cl, Br, I) crystals were tunable. The band gaps reveal a broadening trend with 3.532 eV, 3.410 eV and 3.175 eV along the Cl → Br → I series. This work provides an effective molecular design for multifunctional organic-inorganic perovskites.
The undesirable enzymatic activity of nanozymes under near neutral pH condition and the traditional single signal output always restrict the analytical application of nanozyme-based biosensors. Herein, graphitic carbon nitride nanosheets supported palladium nanosheets composite (Pd/g-C3N4) with both oxidase-like activity and fluorescent property is synthesized. Notably, Pd/g-C3N4 exhibits enhanced oxidase-like activity compared to Pd NSs under pH 7.4. By combining Pd/g-C3N4 with o-phenylenediamine (OPD), a ratiometric fluorescence assay for acetylcholinesterase (AChE) activity detection is developed. Pd/g-C3N4 can catalyze oxidation of nonfluorescent OPD to fluorescent oxidized OPD (oxOPD, Em = 565 nm), which can quench fluorescence of g-C3N4 supporter (Em = 441 nm) through fluorescence resonance energy transfer (FRET). However, in presence of AChE, acetylthiocholine can be hydrolyzed into thiocholine, which will block the oxidase-like activity of Pd/g-C3N4 and then hamper the FRET process. This ratiometric fluorescence assay is also viable to screen AChE inhibitor. This work will guide design of ratiometric fluorescence assay based on nanozymes with improved enzymatic activity.
Carbon dots (CDs), because of their unique properties, are being rapidly developed as important luminescent materials for imaging, sensing, and use in photonic devices. However, most of the reported fundamental properties of the CDs are results of investigations conducted in the solution state, which may be completely different from those conducted in the solid state. In this work, we study the luminescence properties, photostability, and the dynamics of CDs in different matrix environments, from ensemble to the single-particle level. We observed that the properties associated with the emission centers and photostability of CDs were extremely sensitive to the local chemical environment. A better understanding of the dependence of the spectroscopic properties of CDs on the complex local chemical environment is an important step toward finding new ways of controlling the optical properties of CDs and optimizing their use in various applications.
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.
In this work, hierarchical NiS@ZnIn2S4 heterostructure was developed by constructing ultra-thin ZnIn2S4 (ZIS) nanosheets on hollow NiS nanospheres for hydrogen production from photocatalytic water splitting. The NiS@ZIS displayed a strong optical absorption ability in the visible region and a high specific surface area of 33.14 m2/g. The Type-I band alignment in NiS@ZIS heterostructure was determined by the combination of UV–vis absorption spectroscopy and Mott-Schottky curves. The photocatalytic hydrogen production of NiS@ZIS (1.24 mmol g-1 h-1) was nearly 5.6 times higher than that of ZIS under visible light, in the absence of any co-catalyst and sacrificial agent. The separation and migration of charge in NiS@ZIS were characterized by a series of spectroscopy and photo/electrochemical tests, which verified the efficient charge transfer from ZIS to NiS.
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