Latest ArticlesA multifunctional nanocomposite of AgNPs@GQDs is prepared by synergistic in-situ growth of silver nanoparticles (AgNPs) on the complex of tannic acid (TA) and graphene quantum dots (GQDs) for the construction of dual-mode biosensing platform and cancer theranostics. The nanocomposite exhibits a hydrogen peroxide (H2O2)-responsive degradation, in which Ag0 is oxidized to Ag+ along with the release of oxidized TA and GQDs. The degradation induces the decreased absorbance and enhanced fluorescence (FL) intensity due to the suppression of Förster resonance energy transfer (FRET) in AgNPs@GQDs, which is employed for colorimetric/fluorescence dual-mode sensing of H2O2. The intrinsic peroxidase-like activity of GQDs nanozyme can effectively catalyze the oxidation reaction, enhancing the detection sensitivity significantly. Based on the generation of H2O2 from the oxidation of glucose with the catalysis of glucose oxidase (GOx), this nanoprobe is versatilely used for the determination of glucose in human serum. Further, through combining the H2O2-responsive degradation of AgNPs@GQDs with high H2O2 level in cancer cells, the nanocomposites exhibit good performance in cancer cell recognition and therapy, in which the synergistic anticancer effect of Ag+ and oxidized TA contribute to effective cell death, and the liberated GQDs are used to monitor the therapeutic effect by cell imaging.
In this study, we prepared mitochondrion targeting peptide-grafted magnetic graphene oxide (GO) nanocarriers for efficient impairment of the tumor mitochondria. The two-dimensional GOMNP-MitP nanosheets were synthesized by grafting magnetic γ-Fe2O3 to the surface of GO, followed by covalent modification of mitochondrion targeting peptide (MitP). GOMNP-MitP exhibited the high capacity of loading the anticancer drug mitoxantrone (MTX), and preferentially targeted the tumor mitochondria. With the aid of alternating magnetic field (AMF), the MTX-loading GOMNP-MitP released MTX to the mitochondria, severely impairing mitochondrial functions, including attenuation of ATP production, decrease in mitochondrial membrane potential (MMP), and further leading to activation of apoptosis. This study realized high-efficient mitochondrion-targeting drug delivery for anticancer therapy by two-dimensional nanoplatforms.
In this work, various Co3O4-ZSM-5 catalysts were prepared by the microwave hydrothermal method (MH-Co3O4@ZSM-5), dynamic hydrothermal method (DH-Co3O4@ZSM-5), and conventional hydrothermal method (CH-Co3O4/ZSM-5). Their catalytic oxidation of dichloromethane (DCM) was analyzed. Detailed characterizations such as X-ray diffractometer (XRD), scanning microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), H2 temperature-programmed reduction (H2-TPR), temperature-programmed desorption of O2 (O2-TPD), temperature-programmed desorption of NH3 (NH3-TPD), diffuse reflectance infrared Fourier-transform spectra with NH3 molecules (NH3-DRIFT), and temperature-programmed surface reaction (TPSR) were performed. Results showed that with the assistance of microwave, MH-Co3O4@ZSM-5 formed a uniform core-shell structure, while the other two samples did not. MH-Co3O4@ZSM-5 possessed rich surface adsorbed oxygen species, higher ratio of Co3+/Co2+, strong acidity, high reducibility, and oxygen mobility among the three Co3O4-ZSM-5 catalysts, which was beneficial for the improvement of DCM oxidation. In the oxidation of dichloromethane, MH-Co3O4@ZSM-5 presented the best activity and mineralization, which was consistent with the characterizations results. Meanwhile, according to the TPSR test, HCl or Cl2 removal from the catalyst surface was also promoted in MH-Co3O4@ZSM-5 by their abundant Brønsted acid sites and the promotion of Deacon reaction by Co3O4 or the synergistic effect of Co3O4 and ZSM-5. According to the results of in situ DRIFT studies, a possible reaction pathway of DCM oxidation was proposed over the MH-Co3O4@ZSM-5 catalysts.
A simple and efficient visible-light-induced photoredox-catalyzed diarylation of N-methacryloyl-2-arylbenzoimidazoles with aryl diazonium salts was developed. The reaction provides a convenient access to a variety of benzimidazoisoquinolinones through the construction of two CC bonds in one step under mild reaction conditions.
High-mobility and strong luminescent materials are essential as an important component of organic photodiodes, having received extensive attention in the field of organic optoelectronics. Beyond the conventional chemical synthesis of new molecules, pressure technology, as a flexible and efficient method, can tune the electronic and optical properties reversibly. However, the mechanism in organic materials has not been systematically revealed. Here, we theoretically predicted the pressure-depended luminescence and charge transport properties of high-performance organic optoelectronic semiconductors, 2, 6-diphenylanthracene (DPA), by first-principle and multi-scale theoretical calculation methods. The dispersion-corrected density functional theory (DFT-D) and hybrid quantum mechanics/molecular mechanics (QM/MM) method were used to get the electronic structures and vibration properties under pressure. Furthermore, the charge transport and luminescence properties were calculated with the quantum tunneling method and thermal vibration correlation function. We found that the pressure could significantly improve the charge transport performance of the DPA single crystal. When the applied pressure increased to 1.86GPa, the hole mobility could be doubled. At the same time, due to the weak exciton coupling effect and the rigid flat structure, there is neither fluorescence quenching nor obvious emission enhancement phenomenon. The DPA single crystal possesses a slightly higher fluorescence quantum yield ~ 0.47 under pressure. Our work systematically explored the pressure-dependence photoelectric properties and explained the inside mechanism. Also, we proposed that the external pressure would be an effective way to improve the photoelectric performance of organic semiconductors.
A nickel(Ⅱ)-catalyzed asymmetric alkylation of acyclic oxocarbenium ions generated in situ from corresponding acetals with carboxylic acid derivatives to prepare β-alkoxyl carbonyl moieties with diverse α-substituents has been disclosed. The method exhibited broad scope of acetals and carboxylic acid derivatives with excellent enantioselectivity and good functional group compatibility, and can be conducted in a gram-scale without obvious loss of efficiency.
A chiral cobalt pincer complex, when combined with an achiral electron-rich mono-phosphine ligand, catalyzes efficient asymmetric hydrogenation of a wide range of aryl ketones, affording chiral alcohols with high yields and moderate to excellent enantioselectivities (29 examples, up to 93% ee). Notably, the achiral mono-phosphine ligand shows a remarkable effect on the enantioselectivity of the reaction.
Charge transfer via electron hopping from an electron donor (D) to an acceptor (A) in nanoscale, plays a crucial role in optoelectronic materials, such as organic light-emitting diodes (OLEDs) and organic photovoltaic cells (OPVs). Here, we propose a strategy for binding D/A units in space, where intramolecular charge-transfer can take place. The resulted material DM-Me-B is able to give bright emission in this molecular architecture because of the good control of D/A interaction and conformational rigidity. Moreover, DM-Me-B presents small singlet-triplet splitting energy, enabling thermally activated delayed fluorescence. Therefore, the DM-Me-B exhibits ~20% maximum external quantum efficiency and low efficiency roll-off at 1000cd/m2, certifying an effective strategy in controlling D/A blocks through space.
The 1D microwires based on π-extended azaBODIPY were successfully prepared and characterized for the first time. The bisphenanthrene-fused azaBPP-12C with four hydrophobic chains was prepared through de novo synthesis method involving the Suzuki reaction and subsequent oxidative ring-fused coupling. The microwires and aggregation behavior were studied using SEM, XRD and absorption spectroscopy. Finally, an H-type aggregation was confirmed in the solution process.
p-TsOH catalyzed Diels-Alder reaction of 3-(indol-3-yl)maleimides with 3-phenacylideneoxindoles in toluene at 80 ℃ for two hours afforded cis/trans isomers of 3a', 4′, 6′, 10c'-tetrahydrospiro[indoline-3, 5′-pyrrolo[3, 4-c]carbazoles] in nearly comparable yields, which could be easily converted to the corresponding 4′, 6′-dihydrospiro[indoline-3, 5′-pyrrolo[3, 4-c]carbazole] in high yields and with high diastereoselectivity by further DDQ oxidation., the similar reaction of 3-(indol-3-yl)maAdditionallyleimides with 2-arylidene-1, 3-indanediones in toluene 80 ℃ and sequential DDQ oxidation afforded functionalized dihydrospiro[indene-2, 5′-pyrrolo[3, 4-c]carbazoles] as major products.