Latest ArticlesWe developed one-pot aqueous copolymerization of two dopamine prodrugs to prepare dual drugs-conjugated polydopamine nanoparticles (PDOXCBs), which integrated near infrared (NIR)-mediated photothermal effect with cocktail chemotherapy into one copolymer nanoparticle. Upon a mild NIR irradiation (808 nm, 1 W/cm2, 10 min), PDOXCBs gradually heated aqueous solution over 12.8–13.9 ℃, which accordingly enhanced in vitro dual doxorubicin (DOX) and chlorambucil (CB) drug-release with assistance of the other stimuli of pH 5.0 and 10 mmol/L D,L-dithiothreitol (DTT). The combination photothermal-cocktail chemotherapy (PTT－CCT) treatment based on PDOXCB27 plus NIR irradiation gave a highly lowered half maximal inhibitory concentration (IC50) of 2.23 μg/mL and a combination index of 0.36, displaying a superior synergistic effect between PTT and CCT in vitro.
Inorganic lead halide perovskites are attractive optoelectronic materials owing to their relative stability compared to organic cation alternatives. The chemical vapor deposition (CVD) method offers potential for high quality perovskite film growth. The deposition temperature is a critical parameter determining the film quality owing to the melting difference between the precursors. Here, perovskite films were deposited by the CVD method at various temperatures between 500-800 ℃. The perovskite phase converts from CsPb2Br5 to CsPbBr3 gradually as the deposition temperature is increased. The grain size of the perovskite films also increases with temperature. The phase transition mechanism was clarified. The photoexcited state dynamics were investigated by spatially and temporally resolved fluorescence measurements. The perovskite film deposited under 750 ℃ condition is of the CsPbBr3 phase, showing low trap-state density and large crystalline grain size. A photodetector based on perovskite films shows high photocurrent and an on/off ratio of ~2.5×104.
A practical synthesis of α-bromo/iodo/chloroketones from olefins under visible-light irradiation conditions has been developed. In the presence of PhI(OAc)2 as promoter and under ambient conditions, the reactions of styrenes and triiodomethane undergo the transformation smoothly to deliver the corresponding α-iodoketones without additional photocatalyst in good yields under sunlight irradiation. Meanwhile, the reactions of styrenes with tribromomethane and trichloromethane generate the desired α-bromoketones and α-chloroketones in high yields by using Ru(bpy)3Cl2 as a photocatalyst under blue LED (450–455 nm) irradiation.
The 2D nanomaterials have achieved the superlubrication property whatever in solid or liquid lubrication in recent years. However, whether or not the nanosheets can stably disperse in oils and smoothly enter into the asperity of friction pairs is crucial for exerting the function of antifriction. The structure of 2D QDs is desirable for addressing these issues due to its smaller 3D size. In this study, we developed a facile preparation process for WS2 QDs with uniform 2 nm size from nanosheets via hydrothermal-assisted grinding approach. The structure of the as-obtained WS2 QDs was determined by a series of characterizations. The results showed that the as-obtained WS2 QDs exhibited the typical spectrum features of nanosized quantum dot. The results of the tribological performance in grease verified that the average friction coefficient (ACOFs) and wear volume (AWVs) were decreased by 7.89% and 63.90% relative to grease, respectively, exhibiting a preferable friction reducing and wear resistance.
A Pd-catalyzed enantioselective synthesis of 2-methyl-3-methyleneindoline in up to 89% yield and 84% ee from racemic vinyl benzoxazinanones has been developed with the help of (R,R)-BenzP* ligand. Mechanism studies support the formation of palladacyclobutane as the key intermediate via C2 attack to π-allyl Pd complex. The β-hydride elimination provides a new reaction pathway for the palladacyclobutane.
Based on the crystal structures of two cucurbit[6]uril/calix[n]arene-based supramolecular frameworks reported by Long and co-workers, we further investigated the interactions of cucurbit[6]uril with 4-sulfocalix[4]arene and 4-sulfocalix[6]arene using 1H NMR spectroscopy and isothermal titration calorimetry (ITC), respectively. Moreover, solid fluorescent materials were prepared via the adsorption of fluorescent dyes by these porous supramolecular frameworks, which exhibit a selective response to certain volatile organic compounds.
Metal organic frameworks (MOFs) are a kind of promising materials in many applications, while the fast and controllable synthesis of MOFs is still challenging. Here, taking HKUST-1 as illustration, a micro-plasma electrochemistry (MIPEC) strategy was developed to accelerate the synthesis process of MOFs with micro-plasma acting as cathode. Treating the HKUST-1 precursor solution with micro-plasma cathode could not only transfer the electrons into the solution leading to the deprotonation effect, but also generate radical species to trigger and accelerate the nucleation and growth of MOFs at the plasma-liquid interface. Thus, uniform and nanosize MOFs could be prepared within minutes. The obtained MOFs show similar excellent uranium adsorption properties compared with those obtained by other method, with a highly adsorption capability of uranium with 550 mg/g in minutes. The novel MIPEC strategy developed in this work provides an alternative for controllable synthesis of MOFs, and especially has potential application in accelerating traditional organic synthesis.
A cascade carbonylative ring expansion and [2 + 2]/[4 + 2] cycloaddition of strained 1-iminylphosphirane complexes with aryl allenes were reported. The carbonylative ring expansion of 1-iminylphosphirane complexes provides an azaphosphacyclohexone complex intermediate with a C＝P double bond. The following [2 + 2] or dearomatic [4 + 2] cycloaddition of this intermediate with allenes is modulated by the aryl substituents on the imino carbon. The regioselective [2 + 2] cycloaddition with 1, 1-diarylallene provides an entry to bicyclo[4.2.0]octan-4-one skeletons featuring a four-membered phosphacyclobu-tane moiety. While dearomatic [4 + 2] cycloaddition was preferred with less aromatic naphthalene and yielded octahydrochrysene skeleton containing heteroatoms.
AA005 (1), a potent anticancer mimicking molecule of natural Annonaceous acetogenin, features a central C2-symmetric triglycol moiety and three stereogenic centers. To support ongoing animal studies, a scalable 10-step synthesis of AA005 (1) has been studied, optimized and accomplished in this work, starting from commercially available economic materials ethylene glycol and (R)-epichlorohydrin. A regio- and stereo-controlled BF3·Et2O-promoted epoxide opening of (R)-epichlorohydrin with ethylene glycol was investigated, optimized and successfully applied to the scalable preparation of the crucial fragment 6a with C2-symmetry. Further successive epoxide openings elaborated both two side chains and the whole skeleton with proper nucleophiles and electrophiles. Comparison and optimization of the reaction sequences finally led to completion of a new multi-gram synthesis of AA005 (1) with satisfactory enantiomeric and diastereomeric purity.
A novel BF3-promoted [3 + 2] annulation of azonaphthalenes and ynamides is described. This protocol provides a modular and efficient entry to functionalized amino benzo[e]indole derivatives smoothly.
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